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Abstract

Dipole and quadrupole modes are the two lowest orders of localized surface plasmon resonance (LSPR) eigenmodes in metallic nanoparticles. Of these two modes, the quadrupole mode is forbidden for symmetric metallic nanoparticles excited by linearly polarized light at normal incidence. Here, we demonstrate excitation of the quadrupole mode in symmetrical gold (Au) nanoblocks shined with s-polarized light at oblique incidence. In particular, we probe the near-field LSPR in Au nanoblocks using photoemission electron microscopy (PEEM) and find that at oblique incidence, the dipole and quadrupole modes can be selectively excited, in terms of near-field enhancement, by manipulating the light polarization state. More importantly, by time-resolved PEEM measurements, we experimentally demonstrate that the quadrupole mode in symmetrical Au nanoblocks has longer dephasing time than that of the dipole mode.

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Localized surface plasmon resonances (LSPRs) are collective charge oscillations that are confined to the surfaces of metallic nanoparticles (NPs)(1, 2) and have been attracting considerable research interest for a broad range of applications such as sensing,(2-4) imaging,(4, 5) lasing,(6) energy harvesting,(7-10) photochemical reactions,(11, 12) and artificial photosynthesis.(13, 14) The optical properties of LSPRs are influenced by their size and shape as well as the type of metal used and the surrounding dielectric environment.(1, 2) For a given metal (typically gold or silver), when the size of the metallic NP is much smaller than the wavelength of incident light, the fundamental dipole resonance mode dominates the in-phase oscillation of the free electrons in the NP. In contrast, when the size is comparable to or even larger than the wavelength of the light, free electrons at different locations in the NP oscillate in different phases, resulting in the excitation of quadrupole or multipolar modes.(15) Multipolar LSPR modes in metal nanorods have been imaged using scanning near-field optical microscopy (SNOM)(16-18) and, very recently, using electron energy-loss spectroscopy.(19, 20)

Because of symmetry selection rules, in the dipole approximation the quadrupole mode and other even-order multipolar modes are forbidden for thin symmetric nanoparticles irradiated with linearly polarized light at normal incidence. However, the quadrupole mode becomes accessible through phase retardation or symmetry breaking.(21-24) Esteban et al. have reported the simultaneous mapping of dipole and quadrupole LSPRs for Au nanodisks of different diameters under oblique-incidence irradiation using SNOM.(22) The excitation of dipole and quadrupole modes on planar nanoparticles of the same size and their near-field properties should be very interesting and may improve the understanding of different-order LSPRs. However, no such studies have been performed to date. Furthermore, the nature of the quadrupole mode should produce a narrower line width, i.e., a higher Q-factor than that of the dipole mode, which suggests that the quadrupole mode should be more suitable for sensing applications.(2-4) When compared with the dipole mode, the damping of the quadrupole mode should be reduced, leading to a longer dephasing process. Nonetheless, there is no experimental evidence that shows quadrupole mode has longer dephasing time than dipole mode.

In addition to the SNOM technique(16-18, 25, 26) and other near-field mapping techniques,(27-30) recent development of nonlinear photoemission electron microscopy (PEEM) using femtosecond laser pulses as the excitation light source is found promising for pinpointing the near-field properties of surface plasmon resonances for both localized modes and propagation modes.(31-36) Very recently, by using PEEM, we demonstrated direct near-field imaging of Au nanoparticles with a high spatial resolution down to ≃10 nm.(37) We also succeeded in probing the ultrafast dephasing of the LSPRs on Au nanoparticles using time-resolved PEEM. In this study, by applying PEEM as a tool, we verify that the quadrupole mode could be excited by s-polarized light at oblique incidence and further explored the selective excitation of dipole and quadrupole modes through the manipulation of the polarization and wavelength of the incident light. Furthermore, our time-resolved PEEM measurements experimentally demonstrate that the quadrupole mode has a longer dephasing time than the dipole mode.

Results and Discussion

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Characterization of Topography and Far-Field Spectra

The nanoparticles that were investigated in this study were square nanoblocks, which are symmetric structures, meaning that the quadrupole mode is forbidden at normal incidence. The Au nanoblocks were fabricated on ITO-coated glass via standard electron-beam lithography, followed by metal sputtering and lift-off. Figure 1a presents typical scanning electron microscopy (SEM) images of the fabricated structures. The Au nanoblocks were arranged in a two-dimensional square array with an area of 150 × 150 μm² and a pitch size of 500 nm. Each nanoblock had dimensions of 200 × 200 × 30 nm³. The far-field extinction spectrum was measured using a Fourier-transform infrared (FTIR) spectrometer equipped with an infrared microscope. As seen in Figure 1b, a strong, wide extinction band centered at approximately 875 nm was observed in the spectrum. This band was attributed to the dipole LSPR of the Au nanoblocks. A weak shoulder-like peak also appeared at approximately 765 nm. This peak was attributed to the quadrupole LSPR mode, as will be proven later. This quadrupole mode was observed primarily because the light incidence was not exactly normal during the acquisition of the spectrum; instead, the Cassegrainian objective lens that was used in the FTIR spectrometer provided a range of incidence angles between 16° and 32°.

Figure 1. Characterization of the Au nanoblocks and PEEM measurements. (a) SEM images of the Au nanoblocks; the scale bar in the inset is 100 nm. (b) The far-field extinction spectrum of Au nanoblocks. (c) A schematic diagram of PEEM setup, in which the laser is directed onto the sample at either normal incidence or oblique incidence with an incidence angle of 74°. (d–f) PEEM images (FOV of 0.75 μm) of one nanoblock in an array under different excitation conditions: (d) femtosecond laser pulses with a central wavelength of 860 nm at normal incidence, (e) femtosecond pulses and UV light from a mercury lamp, and (f) UV light only. The laser polarization was horizontally aligned. The scale bars in (d–f) represent 100 nm.

Near-Field Mapping and Spectra

First, we performed PEEM measurements on the sample using a wavelength-tunable (720–920 nm) femtosecond laser source with a pulse duration of 100 fs. The laser light could be directed onto the sample at either normal incidence or oblique incidence at a fixed incidence angle of 74°, as shown in Figure 1c. Figure 1d presents a typical PEEM image in the field of view (FOV = 0.75 μm) of a nanoblock in an array that was irradiated by femtosecond laser pulses under normal incidence with a central wavelength of 860 nm, which was nearly at the dipole LSPR peak wavelength. As expected, four hot spots from the nanoblock are apparent in the image. This result was essentially similar to our previous observations on Au nanorods(37) and reflects on the electric field (near-field) intensity distribution of Au nanoblocks upon excitation of the LSPR. We used an additional UV light source, a mercury lamp, to further confirm that the hot spots originated from the four corners of the nanoblocks, as shown in the PEEM images presented in Figure 1e, in which the sample was simultaneously irradiated with the laser and the UV light. However, no hot spots were observed under only UV light excitation (Figure 1f). The wavelength of the UV light was far from the LSPR wavelength; thus, the one-photon PEEM image that was obtained under UV light excitation was a direct observation of the morphologies of the nanoblocks and served as a reference to determine the plasmonic hot spots that were induced by the femtosecond laser pulses. Notably, this is the first report of the acquisition of a PEEM image of a single plasmonic nanostructure for such a low FOV and demonstrates that PEEM can be used to investigate the near fields of more complex plasmonic systems at a high spatial resolution.

We systematically investigated the wavelength-dependent near-field properties of the Au nanoblocks by performing PEEM measurements. The laser wavelength was tuned from 720 to 920 nm in increments of 10 nm under three incidence conditions: normal incidence, oblique incidence with p-polarization, and oblique incidence with s-polarization. The same pulse duration and laser power were maintained for each excitation condition. We found that for normal incidence and oblique incidence with p-polarization, the strongest photoemission was obtained at a wavelength of 860 nm, which was near the far-field dipole peak wavelength. In contrast, for oblique incidence with s-polarization, the photoemission at this wavelength was very weak, and the strongest photoemission was obtained at a wavelength of 760 nm. Thus, a new mode other than the dipole mode was excited. The PEEM images (FOV = 10 μm) for five different wavelengths (720, 760, 800, 860, and 920 nm) under these three different incidence conditions are presented in Figure S1 of the Supporting Information.

By integrating the photoemission signal and plotting this integral against the incidence wavelength, we can obtain the wavelength-dependent photoemission intensity curves. Because the photoemission (PE) intensity is correlated with the near-field electric field intensity on the sample surface in a nonlinear manner, the wavelength-dependent PE curve can be treated as the nonlinear near-field spectrum of the Au nanoblocks. Usually, the peaks in the wavelength-dependent PE curve correspond to LSPR modes detected from the near field. This technique has been recently employed to investigate the near-field dark plasmon modes in a system of individual Au nanoparticles that were placed at a subnanometer distance from an Au film(34) and the dipole LSPRs in aluminum nanorods.(38) As seen in Figure 2, irradiation with light in different polarization states at oblique incidence produced clearly different near-field spectra. Under p-polarized irradiation, only the dipole mode was excited. However, under s-polarized irradiation, the dipole-mode peak did not appear, and the quadrupole mode was efficiently excited instead. The two curves were normalized to the curve that was obtained under p-polarized light excitation, revealing that the near-field enhancement at the quadrupole resonance was even higher than that at the dipole resonance. This result demonstrated that the dipole and quadrupole LSPRs could be selectively excited by manipulating the polarization of the incident light, at least within a near-field perspective, which increased the near-field enhancement of the quadrupole mode. Figure 2 (top) presents two PEEM images that were recorded at the peak wavelengths of the quadrupole and dipole modes, with the light obliquely incident from the left side. In contrast with the results that were obtained at normal incidence, the near-field intensity distribution was not symmetric under either p- or s-polarized light excitation. This result was attributed to the retardation effect and the near-field interference between the incident light field and the LSPR field. In addition, for normal incidence, only one plasmon mode centered at 850 nm appeared in the near-field spectra presented in Figure S2 in the Supporting Information, which was identified as the dipole mode.

Figure 2. Wavelength dependent PEEM measurements. Wavelength-dependent photoemission (PE) intensity integrated from PEEM images acquired at oblique incidence (74° from the normal) using a wavelength-tunable femtosecond laser source with different polarization states. The two curves were normalized to the maximum PE intensity observed under p-polarized laser excitation. The insets present two PEEM images corresponding to the two peak wavelengths, and the dash lines outline the Au nanoblocks.

To explain the experimental observations, we performed a numerical simulation using a finite-difference time-domain (FDTD) method. Figure 3a shows the different characteristics of the near-field intensity spectra (the enhancement factor against the excitation wavelength) that were obtained under p- and s-polarized irradiation. For p-polarization, only a dipole band centered at approximately 900 nm was observed. However, for s-polarization, the quadrupole mode at 750 nm was excited. Since the wavelength dependent PE intensity curves shown in Figure 2 also represent the wavelength dependent near-field intensity enhancement in a nonlinear manner, it is reasonable to believe that the two plasmon modes observed in Figure 3a correspond to those which appeared in Figure 2. It is also noted that the calculated near-field enhancement of the quadrupole mode is larger than that of the dipole mode qualitatively agreeing with the experimental results shown in Figure 2. The electric field intensity distribution at the interface between the Au nanoblocks and the substrate, which is presented in the left column of Figure 3b, reproduced the measured PEEM patterns (insets of Figure 2), considering the nonlinearity of the photoemission. To further examine the origin of the plasmon resonance modes under different light polarizations, we also calculated the charge distributions on the nanoblocks under both incident light polarizations at the corresponding wavelengths. For p-polarized light excitation, the charge distribution at the resonance peak of 900 nm yielded an in-phase distribution along the in-plane direction of the light polarization, clearly indicating the fundamental nature of the dipole resonances. However, for s-polarized light excitation, the charge distribution at the corresponding wavelength of 750 nm exhibited an out-of-phase charge distribution, indicating the presence of a quadrupole mode.

Figure 3. FDTD numerical calculation results. (a) Calculated wavelength-dependent electric field enhancement at the interface of the nanoblocks and the substrate. (b) Calculated electric field intensity distributions (left panels) and charge distributions (right panels) for both p-polarization (top panels) and s-polarization (bottom panels) at the corresponding peak wavelengths.

Notably, under s-polarized light irradiation, no clear dipole peak was observed in the near-field spectra in either the experimental (Figure 2) or simulated results (Figure 3a), primarily because of the significant damping caused by the large phase retardation effect at grazing incidence. In terms of the near-field enhancement, we conclude that the dipole and quadrupole LSPR modes can be selectively excited at oblique incidence by switching between the p- and s-polarization states. It is also worth noting that our near-field spectra (wavelength dependent PE intensity spectra) were obtained by scanning the laser wavelength at the step of 10 nm and during tuning the wavelength, the focal spot, the pulse duration, and the nonlinear order can be slightly changed. This makes it difficult to obtain the real linear near-field intensity spectra, so that it is also difficult to estimate the spectral line width and to infer the dephasing time of the plasmon modes precisely. However, qualitatively it can be found that the bandwidth of the quadrupole mode is narrower than that of the dipole mode, which implies that the quadrupole mode has a longer dephasing time. Next, we will confirm this hypothesis using time-resolved PEEM measurements.

Dynamics of Dipole and Quadrupole LSPRs

Time-resolved PEEM measurements were performed by an interferometric pump–probe technique, which was developed to probe the dynamics of plasmon resonances first by Petek group.(32, 33) A second femtosecond laser source was used in the experiment, which delivered a 7 fs laser pulse with a bandwidth above 200 nm at a repetition rate of 77 MHz. The laser spectrum ranged from 650 to 1000 nm (central wavelength: 850 nm) as can be found in the Supporting Information (Figure S3). This laser beam was thus capable of exciting both the dipole and quadrupole modes of the Au nanoblocks that were used in this study. The femtosecond laser beam was passed through a Mach–Zehnder interferometer to form phase-correlated pump and probe optical pulses and was then focused onto the sample, as shown in the schematic presented in Figure 4a. A series of PEEM images was recorded by adjusting the delay between the pump and probe pulses, at a frame interval of 0.7 fs (π/2 rad with respect to the 850 nm carrier wave of the laser pulse). From the time evolution of PEEM images, the oscillation of the hot spots could be observed.(37)

Figure 4. Time-resolved PEEM measurements. (a) A schematic diagram of the setup for the time-resolved PEEM measurements. (b) Evolution of the PE intensity for both p- and s-polarized light excitation (corresponding to the dipole and quadrupole LSPR modes, respectively) within the phase delay of (0–20) × 2π rad (corresponding to the delay time of 0–56 fs). The inset in (b) shows the time-resolved PE signals expended in the phase delay within (2–6) × 2π rad. PEEM measured and numerical simulated PE intensity for the dipole mode (c) and the quadrupole mode (d) as a function of the delay time between pump and probe pulses. Careful analysis and comparison of the PEEM experimental data with calculations yield a dephasing time of 5 and 9 fs for the dipole and the quadrupole mode, respectively.

The sample used for this time-resolved study is almost identical as that used above. The near-field photoemission spectra could be found in the Supporting Information (Figure S4), which is very similar as Figure 2. The dipole and quadrupole modes are selectively excited by p-pol and s-pol light and the two modes are centered at 770 and 860 nm, respectively. Figure 4b presents the time evolution of photoemission (PE) intensity curves, in which each data represents the integrated PE intensity from one PEEM image (FOV = 10 μm) at the corresponding delay time. The measurements were performed at both the positive and the negative delays and the signals are almost symmetric. For clarity, only half of the curves is shown in Figure 4b. As discussed in our previous study,(36) over a short delay time during which the pump and probe beams overlap, the oscillation of the LSPR hot spots is nearly dominated by the interference of the pump and probe pulses such that the hot spots resonate at the laser carrier frequency. When the delay is longer, the pump and probe pulses are separated. The coherent LSPR fields that are excited by the pump pulses can preserve the memory of the optical phase of the excitation pulses; thus, the two LSPR fields that are induced by the pump and probe pulses can interfere with each other and dominate the oscillation of the hot spots. As can be seen in the inset of Figure 4b, the oscillation phase of the quadrupole LSPR mode is definitely moving inward, while that of the dipole LSPR mode is not. The observed phase difference means the eigen frequency of the quadrupole mode is higher than the carrier frequency of the 7 fs laser pulse. This is consistent with the spectral measurements shown in the Supporting Information (Figure S4). Furthermore, the total photoemission yield decays because of the dephasing of the LSPR field. If we assume two plasmon modes have the same resonance frequencies but different dephasing time, for the one that has longer dephasing time, the pump induced LSPR field should be able to interfere with the probe induced LSPR field at relatively longer time. However, in the case we have discussed here, the dipole mode and quadrupole from the nanoblocks have different resonance frequencies, so that we cannot compare the dephasing time of the two modes by simply comparing the width of the time-resolved PE curves. Instead, numerical simulations are necessary to obtain the dephasing time of the LSPR modes. Kubo et al. have obtained the dephasing times of LSPRs on silver nanostructures by fitting the time-resolved two-photon photoemission signals.(32)

In this study, we performed numerical calculation of the time-resolved nonlinear photoemission signal by employing a plasmon oscillator model with an exponential damping term and including the nonlinearity of the photoemission.(39, 40) To perform the simulations, we also have to know the driving electric field E(t) + E(t + t_d), where t_d is the time delay between the pump and probe pulses. In our experiments, E(t) was determined as a sech²-shaped pulse with the pulse duration of 7 fs (the stimulated measurement of the autocorrelation trace of the pulses at the sample position can be found in Figure S5 in the Supporting Information). Another important parameter in the simulations is the nonlinear photoemission order, which should be dependent on the laser wavelength and the work function of the material. The nonlinear order of gold irradiated by near-infrared femtosecond laser pulses from Ti:sapphire laser is typically reported to be 3 or 4.(37, 41) In the current work, the ultrashort 7 fs laser pulse has very wide spectral range (650–1000 nm), and within the whole spectral range, the nonlinear order is variable. The average nonlinear orders for the dipole and quadrupole modes are 3.7 and 3.6, respectively, which were obtained from the peak to background ratio in the time-resolved PE curves. The values are in accordance with the recently reported value of 3.5, which was measured under experimental conditions similar as that in the current work.(42) The detailed description of the simulation model can be found in the Supporting Information. In the simulations, the dephasing time was used as a fitting parameter and we compared the simulation results with the experimental data and obtained the best fitted dephasing time.

We stimulated the time-resolved photoemission intensity curves for both the p-polarization (Figure 4c) and s-polarization cases (Figure 4d). The resulting stimulated curves yielded the best fitted dephasing time of 5 and 9 fs, respectively. As demonstrated above, the dipole and quadrupole modes could be selectively excited by switching the light polarization between the p- and s-polarization states. A reasonable hypothesis is that for p-polarized and s-polarized light incidence, the photoemission was dominated by the dipole and quadrupole LSPR fields, respectively. Thus, we conclude that the quadrupole mode has a longer dephasing time than the dipole mode. Noting again that from intuition the time-resolved photoemission signal of the quadrupole mode seems to decay faster than that of the dipole mode, it does not necessarily mean that the quadrupole mode has faster dephasing time. We can argue this phenomenon from the point of view of the phase information in the time-resolved measurements. Compared to the dipole mode, the quadrupole mode is more detuned from the carrier frequency of the laser. As a consequence of “detuned” excitation, a coherent oscillation of LSPR at its natural frequency, which is sustained for a few femtoseconds after the pump–pulse leave, will cause destructive interference with probe pulses at the delay phases of n × 2π rad, where n is an integer. Suppressions of photoemission peaks and the phase leading seen for the quadrupole mode at the phase delay of (3–6) × 2π rad (Figure 4b) are induced in this manner. Eventually, the width of time-resolved photoemission signal (interferometric autocorrelation curve) of the quadrupole mode can be narrower than that of the dipole, even though the quadrupole has a longer dephasing time. As discussed above and described in the model (Supporting Information), the time-resolved photoemission signal is dependent on the driving field, LSPR wavelength, and the dephasing time. We have performed some supplementary calculations shown in Figure S6 in the Supporting Information. As we can see from Figure S6a–d, for the same LSPR wavelength, the calculated time-resolved photoemission signal decays slowly with the increase of the dephasing time, while if we fix the dephasing time, we can clearly find the signal decays slowest when the LSPR wavelength is closest to the central wavelength of the driving laser field.

To our knowledge, this study provides the first experimental measurement of the dephasing time of the quadrupole plasmon mode. More importantly, it is the first experimental proof that the dephasing of the quadrupole mode is longer than that of the dipole mode. It is noted that the nonlinear photoemission properties have been compared for the dipole and quadrupole modes of Ag nanoparticles, but the dynamical measurements have not been performed.(43) It is known that the dephasing of LSPR mainly results from the radiative damping that is the scattering loss and the nonradiative decay, which occurs via excitation of electron–hole pairs either by intraband excitation or interband excitation.(44) In this study, both the dipole and quadrupole modes are far from the interband transition region leading to negligible contribution to damping, and the damping from intraband excitation can be thought to be similar. However, for the quadrupole mode, the radiative damping is suppressed due to the less net dipole moment resulting in a longer dephasing time than the dipole mode. It is also worth mentioning that here the dephasing time of both the dipole and quadrupole modes are for the same ensemble of nanoparticles. The effect of the sample inhomogeneity on the dephasing time for both modes should be the same, although the inhomogeneity effect is considered low due to high fabrication quality of electron beam lithography. Consequently, it is more convincing to state that the quadrupole mode has longer dephasing time.

Conclusions

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In conclusion, we experimentally investigated the near-field properties of dipole and quadrupole LSPRs using PEEM. For Au nanoblocks, we found that the dipole and quadrupole modes could be selectively excited at oblique incidence. For p-polarized light excitation, solely the dipole mode was excited and dominated the plasmonic field enhancement; in contrast, for s-polarized light excitation, the quadrupole mode was dominant and provided even higher electric field enhancement. Furthermore, we used time-resolved PEEM to experimentally demonstrate that the dephasing of the quadrupole mode was slower than that of the dipole mode. These results may deepen our understanding of the quadrupole LSPR mode, and this study paves the way toward further investigations of the near field and dynamics of complex plasmonic systems in which different LSPR modes are hybridized or coupled.

Methods

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Sample Fabrication and Characterization

Ordered arrays of Au nanoblocks were fabricated on ITO substrates using electron-beam lithography (EBL) and metal evaporation techniques. A high-resolution EBL system (ELS-7000HM, Elionix) operating at 100 kV was used in this study. A conventional copolymer resist (ZEP520, Zeon Chemicals) was diluted with a ZEP thinner (1:1) and spin coated onto the substrate at 1000 rpm for 10 s and at 4000 rpm for 90 s. The substrate was then prebaked on a hot plate for 2 min at 150 °C. The EBL was operated at an electrical current of 50 pA. After development, a 2 nm-thick titanium layer was then deposited via sputtering (MPS-4000, ULVAC) onto the substrate to serve as an adhesive layer, followed by the deposition of a 30 nm-thick Au film. Lift-off was performed by successively immersing the sample in anisole, acetone, methanol, and ultrapure water in an ultrasonic bath. Field-emission scanning electron microscopy (JSM-6700FT, JEOL) and Fourier transform infrared (FTIR) spectroscopy (FT/IR-6000TM-M, JASCO) were used to characterize the morphologies and far-field spectral properties of the Au nanostructures, respectively.

PEEM Measurements

PEEM measurements were performed using a PEEM with an energy analyzer (Elmitec GmbH) that has a spatial resolution down to 4 nm. The femtosecond laser excitation source consisted of two mode-locked Ti:sapphire femtosecond laser systems with a repetition rate of 77 MHz. One source was a wavelength-tunable (720–920 nm) system that delivered 100 fs laser pulses at a bandwidth of approximate 15 nm. We used this source to perform the wavelength-dependent PEEM measurements. The second source could deliver 7 fs laser pulses at a central wavelength around 850 nm at bandwidths above 200 nm, and at the sample position, the pulse duration was measured to be 7 fs by a simulated measurement outside of the PEEM chamber (Figure S3 and Figure S5). This extreme ultrashort laser source was used for the time-resolved PEEM measurements. The sample was irradiated with femtosecond laser pulses at either a fixed incidence angle of 74° or normal incidence. In this work, the oblique incidence is mainly used. In this case, the laser beam was focused by a focal lens with the focal length of 150 mm, and the size of focused beam spot on the sample was estimated to be 50 × 200 μm². The polarization of the laser beam was controlled by a λ/2 waveplate, and both p- or s-polarized light could be easily obtained at oblique incidence. In the time-resolved PEEM measurements, chirp mirror pairs and a wedge pair were used to compensate for the dispersion to obtain the shortest possible pulse duration inside the PEEM chamber. The interferometric time-resolved apparatus consisted of a Mach–Zehnder interferometer. Typically, time-resolved PEEM images were recorded by adjusting the delay time in increments corresponding to a π/2 phase delay (0.7 fs at a carrier wavelength of 850 nm).

Numerical Simulations

The FDTD Solutions software package (Lumerical, Inc.) was used to numerically calculate the field distributions of the Au nanostructures. The optical properties of Au were obtained using data from Johnson and Christy.(45) The ITO-covered glass substrate was assumed to behave as a dielectric with an average refractive index of n = 1.55. The FDTD simulations were performed on a discrete, nonuniformly spaced mesh with a maximum resolution of 3 nm.

Supporting Information

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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b00715.

PEEM images of the Au nanoblocks excited with five different wavelengths under three different incidence conditions, near-field photoemission spectra under normal incidence, near-field photoemission spectra of the sample for time-resolved PEEM measurements, characterization of the incident laser field on the PEEM sample position, modeling the time-resolved photoemission signal, and some supplementary calculations of time-resolved photoemission signal (PDF)

nn6b00715_si_001.pdf (861.76 kb)

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Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

Author Information

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Corresponding Author
- Hiroaki Misawa - Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0021, Japan; Department of Applied Chemistry & Institute of Molecular Science, National Chiao Tung University, Hsinchu 30010, Taiwan; Email: [email protected]
Authors
- Quan Sun - Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0021, Japan; Creative Research Institution, Hokkaido University, Sapporo 001-0021, Japan
- Han Yu - Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0021, Japan
- Kosei Ueno - Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0021, Japan
- Atsushi Kubo - Institute of Physics, University of Tsukuba, Tsukuba 305-8571, Japan
- Yasutaka Matsuo - Research Institute for Electronic Science, Hokkaido University, Sapporo 001-0021, Japan
Notes
The authors declare no competing financial interest.

Acknowledgment

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Q.S. would like to thank Dr. O. Lecarme for helpful discussion on FDTD simulations. We acknowledge Prof. V. Biju for his careful and critical reading of the manuscript. This study was supported by KAKENHI Grant-in-Aid for Scientific Research (S) (No. 23225006), Young Scientist (B) (No. 26870014), and the Innovative Areas “Artificial Photosysnthesis (AnApple)” (No. 25107501) from the Japan Society for the Promotion of Science (JSPS), the Nanotechnology Platform (Hokkaido University), and the Low-Carbon Research Network of Japan.

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4
Noble Metals on the Nanoscale: Optical and Photothermal Properties and Some Applications in Imaging, Sensing, Biology, and Medicine
Jain, Prashant K.; Huang, Xiaohua; El-Sayed, Ivan H.; El-Sayed, Mostafa A.
Accounts of Chemical Research (2008), 41 (12), 1578-1586CODEN: ACHRE4; ISSN:0001-4842. (American Chemical Society)
A review. Noble metal nanostructures attract much interest because of their unique properties, including large optical field enhancements resulting in the strong scattering and absorption of light. The enhancement in the optical and photothermal properties of noble metal nanoparticles arises from resonant oscillation of their free electrons in the presence of light, also known as localized surface plasmon resonance (LSPR). The plasmon resonance can either radiate light (Mie scattering), a process that finds great utility in optical and imaging fields, or be rapidly converted to heat (absorption); the latter mechanism of dissipation has opened up applications in several new areas. The ability to integrate metal nanoparticles into biol. systems has had greatest impact in biol. and biomedicine. In this Account, the authors discuss the plasmonic properties of gold and silver nanostructures and present examples of how they are being utilized for biodiagnostics, biophys. studies, and medical therapy. For instance, taking advantage of the strong LSPR scattering of gold nanoparticles conjugated with specific targeting mols. allows the mol.-specific imaging and diagnosis of diseases such as cancer. The authors emphasize in particular how the unique tunability of the plasmon resonance properties of metal nanoparticles through variation of their size, shape, compn., and medium allows chemists to design nanostructures geared for specific bio-applications. The authors discuss some interesting nanostructure geometries, including nanorods, nanoshells, and nanoparticle pairs, that exhibit dramatically enhanced and tunable plasmon resonances, making them highly suitable for bio-applications. Tuning the nanostructure shape (e.g., nanoprisms, nanorods, or nanoshells) is another means of enhancing the sensitivity of the LSPR to the nanoparticle environment and, thereby, designing effective biosensing agents. Metal nanoparticle pairs or assemblies display distance-dependent plasmon resonances as a result of field coupling. A universal scaling model, relating the plasmon resonance frequency to the interparticle distance in terms of the particle size, becomes potentially useful for measuring nanoscale distances (and their changes) in biol. systems. The strong plasmon absorption and photothermal conversion of gold nanoparticles has been exploited in cancer therapy through the selective localized photothermal heating of cancer cells. For nanorods or nanoshells, the LSPR can be tuned to the near-IR region, making it possible to perform in vivo imaging and therapy. The examples of the applications of noble metal nanostructures provided herein can be readily generalized to other areas of biol. and medicine because plasmonic nanomaterials exhibit great range, versatility, and systematic tunability of their optical attributes.
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Kawata, S.; Inouye, Y.; Verma, P. Plasmonics for Near-field Nano-Imaging and Superlensing Nat. Photonics 2009, 3, 388– 394 DOI: 10.1038/nphoton.2009.111
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5
Plasmonics for near-field nano-imaging and superlensing
Kawata, Satoshi; Inouye, Yasushi; Verma, Prabhat
Nature Photonics (2009), 3 (7), 388-394CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
A review. Diffraction of light prevents optical microscopes from having spatial resoln. beyond a value comparable to the wavelength of the probing light. This essentially means that visible light cannot image nanomaterials. Here the authors review the mechanism for going beyond this diffraction limit and discuss how manipulation of light by surface plasmons propagating along the metal surface can help to achieve this. The interesting behavior of light under the influence of plasmons not only allows superlensing, in which perfect imaging is possible through a flat thin metal film, but can also provide nano-imaging of practical samples by using a localized surface plasmon mode at the tip of a metallic nanoprobe. The authors also discuss the current research status and some intriguing future possibilities.
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Yang, A. K.; Hoang, T. B.; Dridi, M.; Deeb, C.; Mikkelsen, M. H.; Schatz, G. C.; Odom, T. W. Real-Time Tunable Lasing from Plasmonic Nanocavity Arrays Nat. Commun. 2015, 6, 6939 DOI: 10.1038/ncomms7939
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6
Real-time tunable lasing from plasmonic nanocavity arrays
Yang, Ankun; Hoang, Thang B.; Dridi, Montacer; Deeb, Claire; Mikkelsen, Maiken H.; Schatz, George C.; Odom, Teri W.
Nature Communications (2015), 6 (), 6939CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
Plasmon lasers can support ultrasmall mode confinement and ultrafast dynamics with device feature sizes below the diffraction limit. However, most plasmon-based nanolasers rely on solid gain materials (inorg. semiconducting nanowire or org. dye in a solid matrix) that preclude the possibility of dynamic tuning. Here, we report an approach to achieve real-time, tunable lattice plasmon lasing based on arrays of gold nanoparticles and liq. gain materials. Optically pumped arrays of gold nanoparticles surrounded by liq. dye mols. exhibit lasing emission that can be tuned as a function of the dielec. environment. Wavelength-dependent time-resolved expts. show distinct lifetime characteristics below and above the lasing threshold. By integrating gold nanoparticle arrays within microfluidic channels and flowing in liq. gain materials with different refractive indexes, we achieve dynamic tuning of the plasmon lasing wavelength. Tunable lattice plasmon lasers offer prospects to enhance and detect weak phys. and chem. processes on the nanoscale in real time.
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Atwater, H. A.; Polman, A. Plasmonics for Improved Photovoltaic Devices Nat. Mater. 2010, 9, 205– 213 DOI: 10.1038/nmat2629
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7
Plasmonics for improved photovoltaic devices
Atwater, Harry A.; Polman, Albert
Nature Materials (2010), 9 (3), 205-213CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)
In this review, we survey recent advances at the intersection of plasmonics and photovoltaics and offer an outlook on the future of solar cells based on these principles. The emerging field of plasmonics has yielded methods for guiding and localizing light at the nanoscale, well below the scale of the wavelength of light in free space. Now plasmonics researchers are turning their attention to photovoltaics, where design approaches based on plasmonics can be used to improve absorption in photovoltaic devices, permitting a considerable redn. in the phys. thickness of solar photovoltaic absorber layers, and yielding new options for solar-cell design.
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Nishijima, Y.; Ueno, K.; Yokota, Y.; Murakoshi, K.; Misawa, H. Plasmon-Assisted Photocurrent Generation from Visible to Near-Infrared Wavelength Using a Au-Nanorods/TiO₂ Electrode J. Phys. Chem. Lett. 2010, 1, 2031– 2036 DOI: 10.1021/jz1006675
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8
Plasmon-Assisted Photocurrent Generation from Visible to Near-Infrared Wavelength Using a Au-Nanorods/TiO2 Electrode
Nishijima, Yoshiaki; Ueno, Kosei; Yokota, Yukie; Murakoshi, Kei; Misawa, Hiroaki
Journal of Physical Chemistry Letters (2010), 1 (13), 2031-2036CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
Nanoparticles of noble metals exhibit localized surface plasmons (LSPs) assocd. with the enhancement of an electromagnetic field due to its localization in nanometric domains at the surface of nanoparticles. The authors demonstrate the plasmonic photoelec. conversion from visible to near-IR wavelength without deteriorating photoelec. conversion by using electrodes in which Au nanorods are elaborately arrayed on the surface of a TiO2 single crystal.
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Ueno, K.; Misawa, H. Plasmon-Enhanced Photocurrent Generation and Water Oxidation from Visible to Near-Infrared Wavelengths NPG Asia Mater. 2013, 5, e61 DOI: 10.1038/am.2013.42
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Plasmon-enhanced photocurrent generation and water oxidation from visible to near-infrared wavelengths
Ueno, Kosei; Misawa, Hiroaki
NPG Asia Materials (2013), 5 (Sept.), e61CODEN: NAMPCE; ISSN:1884-4057. (Nature Publishing Group)
A review. This paper presents recent studies of plasmon-enhanced photoelec. conversion and H2O oxidn. by visible and near-IR light irradn. Since the discovery of the Honda-Fujishima effect in 1972, significant efforts were devoted to lengthening the light-energy conversion wavelength. In this context, plasmonic photoelec. conversion was recently demonstrated at visible-to-near-IR wavelengths without deteriorating photoelec. conversion by employing TiO2 (TiO2) single-crystal photoelectrodes, in which Au nanorods are elaborately arrayed on the surface. A KClO4 aq. soln. was employed as an electrolyte soln. without addnl. electron donors; thus, H2O mols. provided the electrons. The stoichiometric evolution of O and H2O2 as a result of the 4- or 2-electron oxidn. of H2O mols., resp., was accomplished with near-IR light irradn. using the plasmonic optical antenna effect. As there is very little overpotential for H2O oxidn., these results constitute a significant advancement in this field. This photoelec. conversion system could potentially be employed in artificial photosynthesis systems that exceed the photosynthetic capabilities of plants by allowing for photoconversion over a wide range of wavelengths.
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Clavero, C. Plasmon-Induced Hot-Electron Generation at Nanoparticle/Metal-Oxide Interfaces for Photovoltaic and Photocatalytic Devices Nat. Photonics 2014, 8, 95– 103 DOI: 10.1038/nphoton.2013.238
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10
Plasmon-induced hot-electron generation at nanoparticle/metal-oxide interfaces for photovoltaic and photocatalytic devices
Clavero, Cesar
Nature Photonics (2014), 8 (2), 95-103CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
A review. Finding higher efficiency schemes for electron-hole sepn. is of paramount importance for realizing more efficient conversion of solar energy in photovoltaic and photocatalytic devices. Plasmonic energy conversion has been proposed as a promising alternative to conventional electron-hole sepn. in semiconductor devices. This emerging method is based on the generation of hot electrons in plasmonic nanostructures through electromagnetic decay of surface plasmons. Here, the fundamentals of hot-electron generation, injection and regeneration are reviewed, with special attention paid to recent progress towards photovoltaic devices. This new energy-conversion method potentially offers high conversion efficiencies, while keeping fabrication costs low. However, several considerations regarding the materials, architectures and fabrication methods used need to be carefully evaluated to advance this field.
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Tsuboi, Y.; Shimizu, R.; Shoji, T.; Kitamura, N. Near-Infrared Continuous-Wave Light Driving a Two-Photon Photochromic Reaction with the Assistance of Localized Surface Plasmon J. Am. Chem. Soc. 2009, 131, 12623– 12627 DOI: 10.1021/ja9016655
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Wu, B. T.; Ueno, K.; Yokota, Y.; Sun, K.; Zeng, H. P.; Misawa, H. Enhancement of a Two-Photon-Induced Reaction in Solution Using Light-Harvesting Gold Nanodimer Structures J. Phys. Chem. Lett. 2012, 3, 1443– 1447 DOI: 10.1021/jz300370b
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12
Enhancement of a Two-Photon-Induced Reaction in Solution Using Light-Harvesting Gold Nanodimer Structures
Wu, Botao; Ueno, Kosei; Yokota, Yukie; Sun, Kai; Zeng, Heping; Misawa, Hiroaki
Journal of Physical Chemistry Letters (2012), 3 (11), 1443-1447CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
We performed a quant. anal. of plasmon-assisted two-photon photochromic reactions on light-harvesting gold nanodimer structures. Our strategy for the quant. anal. of two-photon-induced photochem. reactions on gold nanostructures is using not only a confined photochem. reaction chamber but also a soln. system. The strong intensification of near-field light at the nanogap positions on gold nanodimer pairs promoted two-photon absorption by a closed-form diarylethene deriv., resulting in highly efficient photochromic conversion to the open-form structure.
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Zhong, Y.; Ueno, K.; Mori, Y.; Shi, X.; Oshikiri, T.; Murakoshi, K.; Inoue, H.; Misawa, H. Plasmon-Assisted Water Splitting Using Two Sides of the Same SrTiO₃ Single-Crystal Substrate: Conversion of Visible Light to Chemical Energy Angew. Chem., Int. Ed. 2014, 53, 10350– 10354 DOI: 10.1002/anie.201404926
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13
Plasmon-Assisted Water Splitting Using Two Sides of the Same SrTiO3 Single-Crystal Substrate: Conversion of Visible Light to Chemical Energy
Zhong, Yuqing; Ueno, Kosei; Mori, Yuko; Shi, Xu; Oshikiri, Tomoya; Murakoshi, Kei; Inoue, Haruo; Misawa, Hiroaki
Angewandte Chemie, International Edition (2014), 53 (39), 10350-10354CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)
A plasmon-induced water splitting system that operates under irradn. by visible light was successfully developed; the system is based on the use of both sides of the same strontium titanate (SrTiO3) single-crystal substrate. The water splitting system contains two soln. chambers to sep. hydrogen (H2) and oxygen (O2). To promote water splitting, a chem. bias was applied by regulating the pH values of the chambers. The quantity of H2 evolved from the surface of platinum, which was used as a redn. co-catalyst, was twice the quantity of O2 evolved from an Au-nanostructured surface. Thus, the stoichiometric evolution of H2 and O2 was clearly demonstrated. The hydrogen-evolution action spectrum closely corresponds to the plasmon resonance spectrum, indicating that the plasmon-induced charge sepn. at the Au/SrTiO3 interface promotes water oxidn. and the subsequent redn. of a proton on the backside of the SrTiO3 substrate. The chem. bias is significantly reduced by plasmonic effects, which indicates the possibility of constructing an artificial photosynthesis system with low energy consumption.
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Oshikiri, T.; Ueno, K.; Misawa, H. Plasmon-Induced Ammonia Synthesis through Nitrogen Photofixation with Visible Light Irradiation Angew. Chem., Int. Ed. 2014, 53, 9802– 9805 DOI: 10.1002/anie.201404748
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14
Plasmon-Induced Ammonia Synthesis through Nitrogen Photofixation with Visible Light Irradiation
Oshikiri, Tomoya; Ueno, Kosei; Misawa, Hiroaki
Angewandte Chemie, International Edition (2014), 53 (37), 9802-9805CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)
We have successfully developed a plasmon-induced technique for ammonia synthesis that responds to visible light through a strontium titanate (SrTiO3) photoelectrode loaded with gold (Au) nanoparticles. The photoelectrochem. reaction cell was divided into two chambers to sep. the oxidized (anodic side) and reduced (cathodic side) products. To promote NH3 formation, a chem. bias was applied by regulating the pH value of these compartments, and ethanol was added to the anodic chamber as a sacrificial donor. The quantity of NH3 formed at the ruthenium surface, which was used as a co-catalyst for SrTiO3, increases linearly as a function of time under irradn. with visible light at wavelengths longer than 550 nm. The NH3 formation action spectrum approx. corresponds to the plasmon resonance spectrum. We deduced that plasmon-induced charge sepn. at the Au/SrTiO3 interface promotes oxidn. at the anodic chamber and subsequent nitrogen redn. on the cathodic side.
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You, E. A.; Zhou, W.; Suh, J. Y.; Huntington, M. D.; Odom, T. W. Polarization-Dependent Multipolar Plasmon Resonances in Anisotropic Multiscale Au Particles ACS Nano 2012, 6, 1786– 1794 DOI: 10.1021/nn204845z
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Imura, K.; Nagahara, T.; Okamoto, H. Plasmon Mode Imaging of Single Gold Nanorods J. Am. Chem. Soc. 2004, 126, 12730– 12731 DOI: 10.1021/ja047836c
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16
Plasmon Mode Imaging of Single Gold Nanorods
Imura, Kohei; Nagahara, Tetsuhiko; Okamoto, Hiromi
Journal of the American Chemical Society (2004), 126 (40), 12730-12731CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)
We have investigated two-photon-induced photoluminescence images and spectra of single gold nanorods by using an apertured scanning near-field optical microscope. The obsd. PL spectrum of single gold nanorod can be explained by the radiative recombination of the electron-hole pair near the X and L symmetry points. PL images reveal characteristic features reflecting an eigenfunction of a specific plasmon mode as well as elec. field distributions around the nanorod.
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Imura, K.; Nagahara, T.; Okamoto, H. Near-field Optical Imaging of Plasmon Modes in Gold Nanorods J. Chem. Phys. 2005, 122, 154701 DOI: 10.1063/1.1873692
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17
Near-field optical imaging of plasmon modes in gold nanorods
Imura, Kohei; Nagahara, Tetsuhiko; Okamoto, Hiromi
Journal of Chemical Physics (2005), 122 (15), 154701/1-154701/5CODEN: JCPSA6; ISSN:0021-9606. (American Institute of Physics)
We have investigated optical properties of single gold nanorods by using an apertured-type scanning near-field optical microscope. Near-field transmission spectrum of single gold nanorod shows several longitudinal surface plasmon resonances. Transmission images obsd. at these resonance wavelengths show oscillating pattern along the long axis of the nanorod. The no. of oscillation increases with decrement of observing wavelength. These spatial characteristics were well reproduced by calcd. local d.-of-states maps and were attributed to spatial characteristics of plasmon modes inside the nanorods. Dispersion relation for plasmons in gold nanorods was obtained by plotting the resonance frequencies of the plasmon modes vs. the wave vectors obtained from the transmission images.
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Denkova, D.; Verellen, N.; Silhanek, A. V.; Valev, V. K.; Van Dorpe, P.; Moshchalkov, V. V. Mapping Magnetic Near-Field Distributions of Plasmonic Nanoantennas ACS Nano 2013, 7, 3168– 3176 DOI: 10.1021/nn305589t
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19
Rossouw, D.; Couillard, M.; Vickery, J.; Kumacheva, E.; Botton, G. A. Multipolar Plasmonic Resonances in Silver Nanowire Antennas Imaged with a Subnanometer Electron Probe Nano Lett. 2011, 11, 1499– 1504 DOI: 10.1021/nl200634w
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Multipolar Plasmonic Resonances in Silver Nanowire Antennas Imaged with a Subnanometer Electron Probe
Rossouw, D.; Couillard, M.; Vickery, J.; Kumacheva, E.; Botton, G. A.
Nano Letters (2011), 11 (4), 1499-1504CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
We detect short-range surface plasmon-polariton (SR-SPP) resonances setup in individual silver nanoantenna structures at high-spatial resoln. with a scanning, subnanometer electron probe. Both even and odd multipolar resonant modes are resolved up to sixth order, and we measure their spatial distribution in relation to nanoantenna structures at energies down to 0.55 eV. Fabry-Perot type SR-SPP reflection phase shifts are calcd. from direct measurements of antinode spacings in high-resoln. plasmonic field maps. We observe resonant SR-SPP antinode bunching at nanoantenna terminals in high-order resonant modes, and antinode shifts in nonhomogeneous local environments. Finally, we achieve good agreement of our exptl. SR-SPP maps with numerical calcns. of photon excited near fields, using a novel integrated photon excitation geometry.
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Martin, J.; Kociak, M.; Mahfoud, Z.; Proust, J.; Gérard, D.; Plain, J. High-Resolution Imaging and Spectroscopy of Multipolar Plasmonic Resonances in Aluminum Nanoantennas Nano Lett. 2014, 14, 5517– 5523 DOI: 10.1021/nl501850m
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High-Resolution Imaging and Spectroscopy of Multipolar Plasmonic Resonances in Aluminum Nanoantennas
Martin, Jerome; Kociak, Mathieu; Mahfoud, Zackaria; Proust, Julien; Gerard, Davy; Plain, Jerome
Nano Letters (2014), 14 (10), 5517-5523CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
The authors report on the high resoln. imaging of multipolar plasmonic resonances in Al nanoantennas using EELS. Plasmonic resonances ranging from near-IR to UV are measured. The spatial distributions of the multipolar resonant modes are mapped and their energy dispersion is retrieved. The losses in the Al antennas are studied through the full width at half-max. of the resonances, unveiling the wt. of both interband and radiative damping mechanisms of the different multipolar resonances. In the blue-UV spectral range, high order resonant modes present a quality factor up to 8, 2 times higher than low order resonant modes at the same energy. Near-IR to UV tunable multipolar plasmonic resonances in Al nanoantennas with relatively high quality factors can be engineered. Al nanoantennas are thus an appealing alternative to Au or Ag ones in the visible and can be efficiently used for UV plasmonics.
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Hao, F.; Larsson, E. M.; Ali, T. A.; Sutherland, D. S.; Nordlander, P. Shedding Light on Dark Plasmons in Gold Nanorings Chem. Phys. Lett. 2008, 458, 262– 266 DOI: 10.1016/j.cplett.2008.04.126
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21
Shedding light on dark plasmons in gold nanorings
Hao, Feng; Larsson, Elin M.; Ali, Tamer A.; Sutherland, Duncan S.; Nordlander, Peter
Chemical Physics Letters (2008), 458 (4-6), 262-266CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
The authors present an exptl. and theor. anal. of the optical properties of Au nanorings of different sizes and cross sections. For light polarized parallel to the ring, the optical spectrum can depend sensitively on the angle of incidence. For normal incidence, the spectrum was characterized by two dipolar ring resonances. As the angle of incidence becomes more oblique, several previously dark multipolar ring resonances appear in the spectra. The appearance of the multipolar resonances is a consequence of retardation and can be understood in simple general terms.
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Esteban, R.; Vogelgesang, R.; Dorfmüller, J.; Dmitriev, A.; Rockstuhl, C.; Etrich, C.; Kern, K. Direct Near-Field Optical Imaging of Higher Order Plasmonic Resonances Nano Lett. 2008, 8, 3155– 3159 DOI: 10.1021/nl801396r
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22
Direct Near-Field Optical Imaging of Higher Order Plasmonic Resonances
Esteban, R.; Vogelgesang, R.; Dorfmueller, J.; Dmitriev, A.; Rockstuhl, C.; Etrich, C.; Kern, K.
Nano Letters (2008), 8 (10), 3155-3159CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
The authors map in real space and by purely optical means near-field optical information of localized surface plasmon polariton (LSPP) resonances excited in nanoscopic particles. Careful polarization control enables apertureless scanning near-field optical microscopy (aSNOM) to image dipolar and quadrupolar LSPPs of the bare sample with high fidelity in both amplitude and phase. This establishes a routine method for in situ optical microscopy of plasmonic and other resonant structures under ambient conditions.
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Zhang, Y.; Jia, T. Q.; Zhang, S. A.; Feng, D. H.; Xu, Z. Z. Dipole, Quadrupole and Octupole Plasmon Resonance Modes in Non-Concentric Nanocrescent/Nanodisk Structure: Local Field Enhancement in the Visible and Near Infrared Regions Opt. Express 2012, 20, 2924– 2931 DOI: 10.1364/OE.20.002924
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24
Fang, Z. Y.; Cai, J. Y.; Yan, Z. B.; Nordlander, P.; Halas, N. J.; Zhu, X. Removing a Wedge from a Metallic Nanodisk Reveals a Fano Resonance Nano Lett. 2011, 11, 4475– 4479 DOI: 10.1021/nl202804y
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Removing a Wedge from a Metallic Nanodisk Reveals a Fano Resonance
Fang, Zheyu; Cai, Junyi; Yan, Zhongbo; Nordlander, Peter; Halas, Naomi J.; Zhu, Xing
Nano Letters (2011), 11 (10), 4475-4479CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
A wide variety of complex, multicomponent plasmonic nanostructures possess Fano resonances. Here the authors introduce a remarkably simple planar nanostructure, a single metallic nanodisk with a missing wedge-shaped slice, that supports a Fano resonance. In this geometry, the Fano line shape arises from the coupling between a hybridized plasmon resonance of the disk and a narrower quadrupolar mode supported by the edge of the missing wedge slice. As a consequence, both disk size and wedge angle control the properties of the resonance. A semianal. description of plasmon hybridization proves useful for analyzing the resulting line shape.
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Schnell, M.; García-Etxarri, A.; Huber, A. J.; Crozier, K.; Aizpurua, J.; Hillenbrand, R. Controlling the Near-Field Oscillations of Loaded Plasmonic Nanoantennas Nat. Photonics 2009, 3, 287– 291 DOI: 10.1038/nphoton.2009.46
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25
Controlling the near-field oscillations of loaded plasmonic nanoantennas
Schnell, M.; Garcia-Etxarri, A.; Huber, A. J.; Crozier, K.; Aizpurua, J.; Hillenbrand, R.
Nature Photonics (2009), 3 (5), 287-291CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
Optical and IR antennas enable a variety of cutting-edge applications ranging from nanoscale photodetectors to highly sensitive biosensors. All these applications critically rely on the optical near-field interaction between the antenna and its load' (biomols. or semiconductors). However, it is largely unexplored how antenna loading affects the near-field response. Here, the authors use scattering-type near-field microscopy to monitor the evolution of the near-field oscillations of IR gap antennas progressively loaded with metallic bridges of varying size. The authors' results provide direct exptl. evidence that the local near-field amplitude and phase can be controlled by antenna loading, in excellent agreement with numerical calcns. By modeling the antenna loads as nanocapacitors and nanoinductors, the change of near-field patterns induced by the load can be understood within the framework of circuit theory. Targeted antenna loading provides an excellent means of engineering complex antenna configurations in coherent control applications, adaptive nano-optics and metamaterials.
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Tanaka, Y.; Ishiguro, H.; Fujiwara, H.; Yokota, Y.; Ueno, K.; Misawa, H.; Sasaki, K. Direct Imaging of Nanogap-Mode Plasmon-Resonant Fields Opt. Express 2011, 19, 7726– 7733 DOI: 10.1364/OE.19.007726
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Barnard, E. S.; Pala, R. A.; Brongersma, M. L. Photocurrent Mapping of Near-field Optical Antenna Resonances Nat. Nanotechnol. 2011, 6, 588– 593 DOI: 10.1038/nnano.2011.131
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Photocurrent mapping of near-field optical antenna resonances
Barnard, Edward S.; Pala, Ragip A.; Brongersma, Mark L.
Nature Nanotechnology (2011), 6 (9), 588-593CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)
An increasing no. of photonics applications make use of nanoscale optical antennas that exhibit a strong, resonant interaction with photons of a specific frequency. The resonant properties of such antennas are conventionally characterized by far-field light scattering techniques. Many applications require quant. knowledge of the near-field behavior, and existing local field measurement techniques provide only relative, rather than abs., data. A photodetector platform that uses a Si-on-insulator substrate to spectrally and spatially map the abs. values of enhanced fields near any type of optical antenna by transducing local elec. fields into photocurrent is demonstrated. The resonant optical and materials properties are quantifiable of nanoscale (∼50 nm) and wavelength-scale (∼1 μm) metallic antennas as well as high refractive index semiconductor antennas. The data agree with light scattering measurements, full-field simulations, and intuitive resonator models.
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Nicoletti, O.; de la Peña, F.; Leary, R. K.; Holland, D. J.; Ducati, C.; Midgley, P. A. Three-Dimensional Imaging of Localized Surface Plasmon Resonances of Metal Nanoparticles Nature 2013, 502, 80– 84 DOI: 10.1038/nature12469
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Three-dimensional imaging of localized surface plasmon resonances of metal nanoparticles
Nicoletti, Olivia; de la Pena, Francisco; Leary, Rowan K.; Holland, Daniel J.; Ducati, Caterina; Midgley, Paul A.
Nature (London, United Kingdom) (2013), 502 (7469), 80-84CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
The remarkable optical properties of metal nanoparticles are governed by the excitation of localized surface plasmon resonances (LSPRs). The sensitivity of each LSPR mode, whose spatial distribution and resonant energy depend on the nanoparticle structure, compn. and environment, has given rise to many potential photonic, optoelectronic, catalytic, photovoltaic, and gas- and bio-sensing applications. However, the precise interplay between the three-dimensional (3D) nanoparticle structure and the LSPRs is not always fully understood and a spectrally sensitive 3D imaging technique is needed to visualize the excitation on the nanometer scale. Here we show that 3D images related to LSPRs of an individual silver nanocube can be reconstructed through the application of electron energy-loss spectrum imaging, mapping the excitation across a range of orientations, with a novel combination of non-neg. matrix factorization, compressed sensing and electron tomog. Our results extend the idea of substrate-mediated hybridization of dipolar and quadrupolar modes predicted by theory, simulations, and electron and optical spectroscopy, and provide exptl. evidence of higher-energy mode hybridization. This work represents an advance both in the understanding of the optical response of noble-metal nanoparticles and in the probing, anal. and visualization of LSPRs.
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Leiderer, P.; Bartels, C.; König-Birk, J.; Mosbacher, M.; Boneberg, J. Imaging Optical Near-Fields of Nanostructures Appl. Phys. Lett. 2004, 85, 5370– 5372 DOI: 10.1063/1.1819990
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There is no corresponding record for this reference.
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Ghenuche, P.; Cherukulappurath, S.; Taminiau, T. H.; van Hulst, N. F.; Quidant, R. Spectroscopic Mode Mapping of Resonant Plasmon Nanoantennas Phys. Rev. Lett. 2008, 101, 116805 DOI: 10.1103/PhysRevLett.101.116805
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Spectroscopic Mode Mapping of Resonant Plasmon Nanoantennas
Ghenuche, Petru; Cherukulappurath, Sudhir; Taminiau, Tim H.; van Hulst, Niek F.; Quidant, Romain
Physical Review Letters (2008), 101 (11), 116805/1-116805/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
The authors present spatially resolved spectral mode mapping of resonant plasmon gap antennas using two-photon luminescence microspectroscopy. The obtained maps are in good agreement with 3-dimensional calcns. of the antenna modes. The evolution of the modal field with wavelength, both in the gap and along the two coupled Au nanowires forming the antenna, is directly visualized. At resonance, the luminescence for the gap area is enhanced at least 80 times and a comparison with the antenna extremities shows a dynamical charge redistribution due to the near-field coupling between the two arms.
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Aeschlimann, M.; Brixner, T.; Fischer, A.; Kramer, C.; Melchior, P.; Pfeiffer, W.; Schneider, C.; Strüber, C.; Tuchscherer, P.; Voronine, D. V. Coherent Two-Dimensional Nanoscopy Science 2011, 333, 1723– 1726 DOI: 10.1126/science.1209206
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31
Coherent Two-Dimensional Nanoscopy
Aeschlimann, Martin; Brixner, Tobias; Fischer, Alexander; Kramer, Christian; Melchior, Pascal; Pfeiffer, Walter; Schneider, Christian; Strueber, Christian; Tuchscherer, Philip; Voronine, Dmitri V.
Science (Washington, DC, United States) (2011), 333 (6050), 1723-1726CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)
A spectroscopic method that dets. nonlinear quantum mech. response functions beyond the optical diffraction limit and allows direct imaging of nanoscale coherence is introduced. In established coherent 2-dimensional (2D) spectroscopy, 4-wave-mixing responses are measured using 3 ingoing waves and 1 outgoing wave; thus, the method is diffraction-limited in spatial resoln. In coherent 2D nanoscopy, 4 ingoing waves are used and the final state detected via photoemission electron microscopy, which has 50-nm spatial resoln. Local nanospectra from a corrugated Ag surface were recorded, and subwavelength 2D line shape variations were obsd. Plasmonic phase coherence of localized excitations persisted for ∼100 fs and exhibited coherent beats. The observations are best explained by a model in which coupled oscillators lead to Fano-like resonances in the hybridized dark- and bright-mode response.
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Kubo, A.; Onda, K.; Petek, H.; Sun, Z. J.; Jung, Y. S.; Kim, H. K. Femtosecond Imaging of Surface Plasmon Dynamics in a Nanostructured Silver Film Nano Lett. 2005, 5, 1123– 1127 DOI: 10.1021/nl0506655
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Femtosecond Imaging of Surface Plasmon Dynamics in a Nanostructured Silver Film
Kubo, Atsushi; Onda, Ken; Petek, Hrvoje; Sun, Zhijun; Jung, Yun S.; Kim, Hong Koo
Nano Letters (2005), 5 (6), 1123-1127CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
Light interacting with nanostructured metals excites the collective charge d. fluctuations known as surface plasmons (SP). Through excitation of the localized SP eigenmodes incident light is trapped on the nanometer spatial and femtosecond temporal scales and its field is enhanced. Here we demonstrate the imaging and quantum control of SP dynamics in a nanostructured silver film. By inducing and imaging the nonlinear two-photon photoemission from the sample with a pair of identical 10-fs laser pulses while scanning the pulse delay, we record a movie of SP fields at a rate of 330-as/frame.
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Kubo, A.; Pontius, N.; Petek, H. Femtosecond Microscopy of Surface Plasmon Polariton Wave Packet Evolution at the Silver/Vacuum Interface Nano Lett. 2007, 7, 470– 475 DOI: 10.1021/nl0627846
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Femtosecond Microscopy of Surface Plasmon Polariton Wave Packet Evolution at the Silver/Vacuum Interface
Kubo, Atsushi; Pontius, Niko; Petek, Hrvoje
Nano Letters (2007), 7 (2), 470-475CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
A movie of the dispersive and dissipative propagation of surface plasmon polariton (SPP) wave packets at a Ag/vacuum interface is recorded by the interferometric time-resolved photoemission electron microscopy with 60 nm spatial resoln. and 330 as frame interval. The evolution of SPP wave packets is imaged through a two-path interference created by a pair of 10 fs phase correlated pump-probe light pulses at 400 nm. The wave packet evolution is simulated using the complex dielec. function of Ag.
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Schertz, F.; Schmelzeisen, M.; Mohammadi, R.; Kreiter, M.; Elmers, H. J.; Schönhense, G. Near Field of Strongly Coupled Plasmons: Uncovering Dark Modes Nano Lett. 2012, 12, 1885– 1890 DOI: 10.1021/nl204277y
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Near Field of Strongly Coupled Plasmons: Uncovering Dark Modes
Schertz, Florian; Schmelzeisen, Marcus; Mohammadi, Reza; Kreiter, Maximilian; Elmers, Hans-Joachim; Schoenhense, Gerd
Nano Letters (2012), 12 (4), 1885-1890CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
Strongly coupled plasmons in a system of individual Au nanoparticles placed at sub-nm distance to a Au film (nanoparticle-on-plane, NPOP) are studied using 2 complementary single particle spectroscopy techniques. Optical scattering spectroscopy exclusively detects plasmon modes that couple to the far field via their dipole moment (bright modes). By using photoemission electron microscopy (PEEM), the authors detect in the identical NPOPs near-field modes that do not couple to the scattered far field (dark modes) and are characterized by a strongly enhanced nonlinear electron emission process. Both far- and near-field spectroscopy were carried out for identical individual nanostructures interacting via a sub-nm gap. Strongly resonant electron emission occurs at excitation wavelengths far off-resonant in the scattering spectra.
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Lemke, C.; Schneider, C.; Leißner, T.; Bayer, D.; Radke, J. W.; Fischer, A.; Melchior, P.; Evlyukhin, A. B.; Chichkov, B. N.; Reinhardt, C.; Bauer, M.; Aeschlimann, M. Spatiotemporal Characterization of SPP Pulse Propagation in Two-Dimensional Plasmonic Focusing Devices Nano Lett. 2013, 13, 1053– 1058 DOI: 10.1021/nl3042849
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Spatiotemporal Characterization of SPP Pulse Propagation in Two-Dimensional Plasmonic Focusing Devices
Lemke, Christoph; Schneider, Christian; Leissner, Till; Bayer, Daniela; Radke, Joern W.; Fischer, Alexander; Melchior, Pascal; Evlyukhin, Andrey B.; Chichkov, Boris N.; Reinhardt, Carsten; Bauer, Michael; Aeschlimann, Martin
Nano Letters (2013), 13 (3), 1053-1058CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
The spatiotemporal evolution of a SPP wave packet with femtosecond duration is exptl. studied in 2 different plasmonic focusing structures. A 2-dimensional reconstruction of the plasmonic field in space and time is possible by the numerical anal. of interferometric time-resolved photoemission electron microscopy data. The time-integrated and time-resolved view onto the wave packet dynamics allow 1 to characterize and compare the capabilities of 2-dimensional components for use in plasmonic devices operating with ultrafast pulses.
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Cinchetti, M.; Gloskovskii, A.; Nepjiko, S. A.; Schönhense, G.; Rochholz, H.; Kreiter, M. Photoemission Electron Microscopy as a Tool for the Investigation of Optical Near Fields Phys. Rev. Lett. 2005, 95, 047601 DOI: 10.1103/PhysRevLett.95.047601
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36
Photoemission electron microscopy as a tool for the investigation of optical near fields
Cinchetti, M.; Gloskovskii, A.; Nepjiko, S. A.; Schonhense, G.; Rochholz, H.; Kreiter, M.
Physical Review Letters (2005), 95 (4), 047601/1-047601/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiOx). Photoemission was induced by illumination with a Hg UV lamp (photon energy cutoff ℏ ωUV = 5.0 eV, wavelength λUV = 250 nm) and with a Ti:sapphire femtosecond laser (ℏ ωl = 3.1 eV, λl = 400 nm, pulse width <200 fs), resp. While homogeneous photoelectron emission from the metal is obsd. upon illumination at energies above the Ag plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signature of the local elec. field therefore providing a tool to map the optical near field with the resoln. of emission electron microscopy.
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Sun, Q.; Ueno, K.; Yu, H.; Kubo, A.; Matsuo, Y.; Misawa, H. Direct Imaging of the Near Field and Dynamics of Surface Plasmon Resonance on Gold Nanostructures Using Photoemission Electron Microscopy Light: Sci. Appl. 2013, 2, e118 DOI: 10.1038/lsa.2013.74
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37
Direct imaging of the near field and dynamics of surface plasmon resonance on gold nanostructures using photoemission electron microscopy
Sun, Quan; Ueno, Kosei; Yu, Han; Kubo, Atsushi; Matsuo, Yasutaka; Misawa, Hiroaki
Light: Science & Applications (2013), 2 (Dec.), e118CODEN: LSAIAZ; ISSN:2047-7538. (Nature Publishing Group)
Localized surface plasmon resonance (LSPR) can be supported by metallic nanoparticles and engineered nanostructures. An understanding of the spatially resolved near-field properties and dynamics of LSPR is important, but remains exptl. challenging. We report exptl. studies toward this aim using photoemission electron microscopy (PEEM) with high spatial resoln. of sub-10 nm. Various engineered gold nanostructure arrays (such as rods, nanodisk-like particles and dimers) are investigated via PEEM using near-IR (NIR) femtosecond laser pulses as the excitation source. When the LSPR wavelengths overlap the spectrum of the femtosecond pulses, the LSPR is efficiently excited and promotes multiphoton photoemission, which is correlated with the local intensity of the metallic nanoparticles in the near field. Thus, the local field distribution of the LSPR on different Au nanostructures can be directly explored and discussed using the PEEM images. In addn., the dynamics of the LSPR is studied by combining interferometric time-resolved pump-probe technique and PEEM. Detailed information on the oscillation and dephasing of the LSPR field can be obtained. The results identify PEEM as a powerful tool for accessing the near-field mapping and dynamic properties of plasmonic nanostructures.
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Lecarme, O.; Sun, Q.; Ueno, K.; Misawa, H. Robust and Versatile Light Absorption at Near-Infrared Wavelengths by Plasmonic Aluminum Nanorods ACS Photonics 2014, 1, 538– 546 DOI: 10.1021/ph500096q
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Robust and Versatile Light Absorption at Near-Infrared Wavelengths by Plasmonic Aluminum Nanorods
Lecarme, Olivier; Sun, Quan; Ueno, Kosei; Misawa, Hiroaki
ACS Photonics (2014), 1 (6), 538-546CODEN: APCHD5; ISSN:2330-4022. (American Chemical Society)
The authors study the far-field and near-field properties of Al nanorods fabricated by electron beam lithog. and exhibiting plasmonic resonance in the near-IR region. First, plasmonic modes within nanorod arrays can be tuned by geometrical parameters, allowing 1 to control the system transparency. Next, the light absorption in this structure is closely examd., and Al has great potential due to its unique interband transition at 800 nm. The roles of the dielec. confinement and the coupling between plasmonic resonance and the interband transition are particularly emphasized, as their adjustment can be used to switch from highly scattering particles to absorbing particles without a significant modification of the plasmonic resonance position. Finally, the authors image the plasmon-generated local field distribution in the Al nanostructures and observe, for the 1st time, the effect of the interband transition on the near-field behavior. The effect of the dielec. confinement is also numerically studied, as it is shown to play a significant role in near-field enhancement.
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Lamprecht, B.; Krenn, J. R.; Leitner, A.; Aussenegg, F. R. Resonant and Off-Resonant Light-Driven Plasmons in Metal Nanoparticles Studied by Femtosecond-resolution Third-harmonic Generation Phys. Rev. Lett. 1999, 83, 4421– 4424 DOI: 10.1103/PhysRevLett.83.4421
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Resonant and Off-Resonant Light-Driven Plasmons in Metal Nanoparticles Studied by Femtosecond-Resolution Third-Harmonic Generation
Lamprecht, B.; Krenn, J. R.; Leitner, A.; Aussenegg, F. R.
Physical Review Letters (1999), 83 (21), 4421-4424CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
The authors report on a femtosecond-resoln. study of the plasmon fields in Au nanoparticles using 3rd-harmonic generation. Controlled resonant and off-resonant plasmon excitation is achieved by tailoring the nanoparticle sample by an electron-beam-lithog. method. Comparing the measured 3rd order interferometric autocorrelation function of the plasmon field with simulations based on a simple harmonic oscillator model the authors ext. the temporal characteristic of the plasmon oscillation. For off-resonant excitation of particle plasmons the authors find a beating between the driving laser field and the plasmon field which demonstrates clearly the nature of the plasmon as a collective electron oscillation.
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Hanke, T.; Krauss, G.; Träutlein, D.; Wild, B.; Bratschitsch, R.; Leitenstorfer, A. Efficient Nonlinear Light Emission of Single Gold Optical Antennas Driven by Few-Cycle Near-Infrared Pulses Phys. Rev. Lett. 2009, 103, 257404 DOI: 10.1103/PhysRevLett.103.257404
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Efficient Nonlinear Light Emission of Single Gold Optical Antennas Driven by Few-Cycle Near-Infrared Pulses
Hanke, T.; Krauss, G.; Trautlein, D.; Wild, B.; Bratschitsch, R.; Leitenstorfer, A.
Physical Review Letters (2009), 103 (25), 257404/1-257404/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
Individual nanometer-sized plasmonic antennas are excited resonantly with few-cycle laser pulses in the near IR. Intense 3rd-harmonic emission of visible light prevails for fundamental photon energies <1.1 eV. Interband luminescence and 2nd harmonic generation occur solely at higher driving frequencies. The authors attribute these findings to multiphoton resonances with the d-band transitions of Au. The strong 3rd-order signal allows direct measurement of a subcycle plasmon dephasing time of 2 fs, highlighting the efficient radiation coupling and broadband response of the devices.
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Grubisic, A.; Schweikhard, V.; Baker, T. A.; Nesbitt, D. J. Coherent Multiphoton Photoelectron Emission from Single Au Nanorods: The Critical Role of Plasmonic Electric Near-Field Enhancement ACS Nano 2013, 7, 87– 99 DOI: 10.1021/nn305194n
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Coherent Multiphoton Photoelectron Emission from Single Au Nanorods: The Critical Role of Plasmonic Electric Near-Field Enhancement
Grubisic, Andrej; Schweikhard, Volker; Baker, Thomas A.; Nesbitt, David J.
ACS Nano (2013), 7 (1), 87-99CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)
Electron emission from individual Au nanorods deposited on In-Sn-oxide (ITO) following excitation with femtosecond laser pulses near the rod longitudinal plasmon resonance is studied via scanning photoionization microscopy. The measured electron signal strongly depends on the excitation laser polarization and wavelength. Correlated secondary electron microscopy (SEM) and dark-field microscopy (DFM) studies of the same nanorods unambiguously confirm that max. electron emission results from (i) laser polarization aligned with the rod long axis and (ii) laser wavelength resonant with the localized surface plasmon resonance. The exptl. results are in good agreement with quant. predictions for a coherent multiphoton photoelec. effect, which is identified as the predominant electron emission mechanism for metal nanoparticles under employed excitation conditions. According to this mechanism, the multiphoton photoemission rate is increased by over 10 orders of magnitude in the vicinity of a localized surface plasmon resonance, due to enhancement of the incident electromagnetic field in the particle near-field. These findings identify multiphoton photoemission as an extremely sensitive metric of local elec. fields (i.e., hot spots) in plasmonic nanoparticles/structures that can potentially be exploited for direct quantitation of local elec. field enhancement factors.
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Mårsell, E.; Losquin, A.; Svärd, R.; Miranda, M.; Guo, C.; Harth, A.; Lorek, E.; Mauritsson, J.; Arnold, C. L.; Xu, H. X.; L’Huillier, A.; Mikkelsen, A. Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna Nano Lett. 2015, 15, 6601– 6608 DOI: 10.1021/acs.nanolett.5b02363
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Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna
Marsell Erik; Losquin Arthur; Svard Robin; Miranda Miguel; Guo Chen; Harth Anne; Lorek Eleonora; Mauritsson Johan; Arnold Cord L; Xu Hongxing; L'Huillier Anne; Mikkelsen Anders; Xu Hongxing
Nano letters (2015), 15 (10), 6601-8 ISSN:.
The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.
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Grubisic, A.; Ringe, E.; Cobley, C. M.; Xia, Y. N.; Marks, L. D.; Van Duyne, R. P.; Nesbitt, D. J. Plasmonic Near-Electric Field Enhancement Effects in Ultrafast Photoelectron Emission: Correlated Spatial and Laser Polarization Microscopy Studies of Individual Ag Nanocubes Nano Lett. 2012, 12, 4823– 4829 DOI: 10.1021/nl302271u
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Plasmonic Near-Electric Field Enhancement Effects in Ultrafast Photoelectron Emission: Correlated Spatial and Laser Polarization Microscopy Studies of Individual Ag Nanocubes
Grubisic, Andrej; Ringe, Emilie; Cobley, Claire M.; Xia, Younan; Marks, Laurence D.; Van Duyne, Richard P.; Nesbitt, David J.
Nano Letters (2012), 12 (9), 4823-4829CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
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Abstract
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Figure 1
Figure 1. Characterization of the Au nanoblocks and PEEM measurements. (a) SEM images of the Au nanoblocks; the scale bar in the inset is 100 nm. (b) The far-field extinction spectrum of Au nanoblocks. (c) A schematic diagram of PEEM setup, in which the laser is directed onto the sample at either normal incidence or oblique incidence with an incidence angle of 74°. (d–f) PEEM images (FOV of 0.75 μm) of one nanoblock in an array under different excitation conditions: (d) femtosecond laser pulses with a central wavelength of 860 nm at normal incidence, (e) femtosecond pulses and UV light from a mercury lamp, and (f) UV light only. The laser polarization was horizontally aligned. The scale bars in (d–f) represent 100 nm.
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Figure 2
Figure 2. Wavelength dependent PEEM measurements. Wavelength-dependent photoemission (PE) intensity integrated from PEEM images acquired at oblique incidence (74° from the normal) using a wavelength-tunable femtosecond laser source with different polarization states. The two curves were normalized to the maximum PE intensity observed under p-polarized laser excitation. The insets present two PEEM images corresponding to the two peak wavelengths, and the dash lines outline the Au nanoblocks.
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Figure 3
Figure 3. FDTD numerical calculation results. (a) Calculated wavelength-dependent electric field enhancement at the interface of the nanoblocks and the substrate. (b) Calculated electric field intensity distributions (left panels) and charge distributions (right panels) for both p-polarization (top panels) and s-polarization (bottom panels) at the corresponding peak wavelengths.
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Figure 4
Figure 4. Time-resolved PEEM measurements. (a) A schematic diagram of the setup for the time-resolved PEEM measurements. (b) Evolution of the PE intensity for both p- and s-polarized light excitation (corresponding to the dipole and quadrupole LSPR modes, respectively) within the phase delay of (0–20) × 2π rad (corresponding to the delay time of 0–56 fs). The inset in (b) shows the time-resolved PE signals expended in the phase delay within (2–6) × 2π rad. PEEM measured and numerical simulated PE intensity for the dipole mode (c) and the quadrupole mode (d) as a function of the delay time between pump and probe pulses. Careful analysis and comparison of the PEEM experimental data with calculations yield a dephasing time of 5 and 9 fs for the dipole and the quadrupole mode, respectively.
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4. 4
  Jain, P. K.; Huang, X. H.; El-Sayed, I. H.; El-Sayed, M. A. Noble Metals on the Nanoscale: Optical and Photothermal Properties and Some Applications in Imaging, Sensing, Biology, and Medicine Acc. Chem. Res. 2008, 41, 1578– 1586 DOI: 10.1021/ar7002804
  [ACS Full Text ], [CAS], Google Scholar
  4
  Noble Metals on the Nanoscale: Optical and Photothermal Properties and Some Applications in Imaging, Sensing, Biology, and Medicine
  Jain, Prashant K.; Huang, Xiaohua; El-Sayed, Ivan H.; El-Sayed, Mostafa A.
  Accounts of Chemical Research (2008), 41 (12), 1578-1586CODEN: ACHRE4; ISSN:0001-4842. (American Chemical Society)
  A review. Noble metal nanostructures attract much interest because of their unique properties, including large optical field enhancements resulting in the strong scattering and absorption of light. The enhancement in the optical and photothermal properties of noble metal nanoparticles arises from resonant oscillation of their free electrons in the presence of light, also known as localized surface plasmon resonance (LSPR). The plasmon resonance can either radiate light (Mie scattering), a process that finds great utility in optical and imaging fields, or be rapidly converted to heat (absorption); the latter mechanism of dissipation has opened up applications in several new areas. The ability to integrate metal nanoparticles into biol. systems has had greatest impact in biol. and biomedicine. In this Account, the authors discuss the plasmonic properties of gold and silver nanostructures and present examples of how they are being utilized for biodiagnostics, biophys. studies, and medical therapy. For instance, taking advantage of the strong LSPR scattering of gold nanoparticles conjugated with specific targeting mols. allows the mol.-specific imaging and diagnosis of diseases such as cancer. The authors emphasize in particular how the unique tunability of the plasmon resonance properties of metal nanoparticles through variation of their size, shape, compn., and medium allows chemists to design nanostructures geared for specific bio-applications. The authors discuss some interesting nanostructure geometries, including nanorods, nanoshells, and nanoparticle pairs, that exhibit dramatically enhanced and tunable plasmon resonances, making them highly suitable for bio-applications. Tuning the nanostructure shape (e.g., nanoprisms, nanorods, or nanoshells) is another means of enhancing the sensitivity of the LSPR to the nanoparticle environment and, thereby, designing effective biosensing agents. Metal nanoparticle pairs or assemblies display distance-dependent plasmon resonances as a result of field coupling. A universal scaling model, relating the plasmon resonance frequency to the interparticle distance in terms of the particle size, becomes potentially useful for measuring nanoscale distances (and their changes) in biol. systems. The strong plasmon absorption and photothermal conversion of gold nanoparticles has been exploited in cancer therapy through the selective localized photothermal heating of cancer cells. For nanorods or nanoshells, the LSPR can be tuned to the near-IR region, making it possible to perform in vivo imaging and therapy. The examples of the applications of noble metal nanostructures provided herein can be readily generalized to other areas of biol. and medicine because plasmonic nanomaterials exhibit great range, versatility, and systematic tunability of their optical attributes.
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5. 5
  Kawata, S.; Inouye, Y.; Verma, P. Plasmonics for Near-field Nano-Imaging and Superlensing Nat. Photonics 2009, 3, 388– 394 DOI: 10.1038/nphoton.2009.111
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  5
  Plasmonics for near-field nano-imaging and superlensing
  Kawata, Satoshi; Inouye, Yasushi; Verma, Prabhat
  Nature Photonics (2009), 3 (7), 388-394CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
  A review. Diffraction of light prevents optical microscopes from having spatial resoln. beyond a value comparable to the wavelength of the probing light. This essentially means that visible light cannot image nanomaterials. Here the authors review the mechanism for going beyond this diffraction limit and discuss how manipulation of light by surface plasmons propagating along the metal surface can help to achieve this. The interesting behavior of light under the influence of plasmons not only allows superlensing, in which perfect imaging is possible through a flat thin metal film, but can also provide nano-imaging of practical samples by using a localized surface plasmon mode at the tip of a metallic nanoprobe. The authors also discuss the current research status and some intriguing future possibilities.
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6. 6
  Yang, A. K.; Hoang, T. B.; Dridi, M.; Deeb, C.; Mikkelsen, M. H.; Schatz, G. C.; Odom, T. W. Real-Time Tunable Lasing from Plasmonic Nanocavity Arrays Nat. Commun. 2015, 6, 6939 DOI: 10.1038/ncomms7939
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  6
  Real-time tunable lasing from plasmonic nanocavity arrays
  Yang, Ankun; Hoang, Thang B.; Dridi, Montacer; Deeb, Claire; Mikkelsen, Maiken H.; Schatz, George C.; Odom, Teri W.
  Nature Communications (2015), 6 (), 6939CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
  Plasmon lasers can support ultrasmall mode confinement and ultrafast dynamics with device feature sizes below the diffraction limit. However, most plasmon-based nanolasers rely on solid gain materials (inorg. semiconducting nanowire or org. dye in a solid matrix) that preclude the possibility of dynamic tuning. Here, we report an approach to achieve real-time, tunable lattice plasmon lasing based on arrays of gold nanoparticles and liq. gain materials. Optically pumped arrays of gold nanoparticles surrounded by liq. dye mols. exhibit lasing emission that can be tuned as a function of the dielec. environment. Wavelength-dependent time-resolved expts. show distinct lifetime characteristics below and above the lasing threshold. By integrating gold nanoparticle arrays within microfluidic channels and flowing in liq. gain materials with different refractive indexes, we achieve dynamic tuning of the plasmon lasing wavelength. Tunable lattice plasmon lasers offer prospects to enhance and detect weak phys. and chem. processes on the nanoscale in real time.
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7. 7
  Atwater, H. A.; Polman, A. Plasmonics for Improved Photovoltaic Devices Nat. Mater. 2010, 9, 205– 213 DOI: 10.1038/nmat2629
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  7
  Plasmonics for improved photovoltaic devices
  Atwater, Harry A.; Polman, Albert
  Nature Materials (2010), 9 (3), 205-213CODEN: NMAACR; ISSN:1476-1122. (Nature Publishing Group)
  In this review, we survey recent advances at the intersection of plasmonics and photovoltaics and offer an outlook on the future of solar cells based on these principles. The emerging field of plasmonics has yielded methods for guiding and localizing light at the nanoscale, well below the scale of the wavelength of light in free space. Now plasmonics researchers are turning their attention to photovoltaics, where design approaches based on plasmonics can be used to improve absorption in photovoltaic devices, permitting a considerable redn. in the phys. thickness of solar photovoltaic absorber layers, and yielding new options for solar-cell design.
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8. 8
  Nishijima, Y.; Ueno, K.; Yokota, Y.; Murakoshi, K.; Misawa, H. Plasmon-Assisted Photocurrent Generation from Visible to Near-Infrared Wavelength Using a Au-Nanorods/TiO₂ Electrode J. Phys. Chem. Lett. 2010, 1, 2031– 2036 DOI: 10.1021/jz1006675
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  8
  Plasmon-Assisted Photocurrent Generation from Visible to Near-Infrared Wavelength Using a Au-Nanorods/TiO2 Electrode
  Nishijima, Yoshiaki; Ueno, Kosei; Yokota, Yukie; Murakoshi, Kei; Misawa, Hiroaki
  Journal of Physical Chemistry Letters (2010), 1 (13), 2031-2036CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
  Nanoparticles of noble metals exhibit localized surface plasmons (LSPs) assocd. with the enhancement of an electromagnetic field due to its localization in nanometric domains at the surface of nanoparticles. The authors demonstrate the plasmonic photoelec. conversion from visible to near-IR wavelength without deteriorating photoelec. conversion by using electrodes in which Au nanorods are elaborately arrayed on the surface of a TiO2 single crystal.
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9. 9
  Ueno, K.; Misawa, H. Plasmon-Enhanced Photocurrent Generation and Water Oxidation from Visible to Near-Infrared Wavelengths NPG Asia Mater. 2013, 5, e61 DOI: 10.1038/am.2013.42
  [Crossref], [CAS], Google Scholar
  9
  Plasmon-enhanced photocurrent generation and water oxidation from visible to near-infrared wavelengths
  Ueno, Kosei; Misawa, Hiroaki
  NPG Asia Materials (2013), 5 (Sept.), e61CODEN: NAMPCE; ISSN:1884-4057. (Nature Publishing Group)
  A review. This paper presents recent studies of plasmon-enhanced photoelec. conversion and H2O oxidn. by visible and near-IR light irradn. Since the discovery of the Honda-Fujishima effect in 1972, significant efforts were devoted to lengthening the light-energy conversion wavelength. In this context, plasmonic photoelec. conversion was recently demonstrated at visible-to-near-IR wavelengths without deteriorating photoelec. conversion by employing TiO2 (TiO2) single-crystal photoelectrodes, in which Au nanorods are elaborately arrayed on the surface. A KClO4 aq. soln. was employed as an electrolyte soln. without addnl. electron donors; thus, H2O mols. provided the electrons. The stoichiometric evolution of O and H2O2 as a result of the 4- or 2-electron oxidn. of H2O mols., resp., was accomplished with near-IR light irradn. using the plasmonic optical antenna effect. As there is very little overpotential for H2O oxidn., these results constitute a significant advancement in this field. This photoelec. conversion system could potentially be employed in artificial photosynthesis systems that exceed the photosynthetic capabilities of plants by allowing for photoconversion over a wide range of wavelengths.
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10. 10
  Clavero, C. Plasmon-Induced Hot-Electron Generation at Nanoparticle/Metal-Oxide Interfaces for Photovoltaic and Photocatalytic Devices Nat. Photonics 2014, 8, 95– 103 DOI: 10.1038/nphoton.2013.238
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  10
  Plasmon-induced hot-electron generation at nanoparticle/metal-oxide interfaces for photovoltaic and photocatalytic devices
  Clavero, Cesar
  Nature Photonics (2014), 8 (2), 95-103CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
  A review. Finding higher efficiency schemes for electron-hole sepn. is of paramount importance for realizing more efficient conversion of solar energy in photovoltaic and photocatalytic devices. Plasmonic energy conversion has been proposed as a promising alternative to conventional electron-hole sepn. in semiconductor devices. This emerging method is based on the generation of hot electrons in plasmonic nanostructures through electromagnetic decay of surface plasmons. Here, the fundamentals of hot-electron generation, injection and regeneration are reviewed, with special attention paid to recent progress towards photovoltaic devices. This new energy-conversion method potentially offers high conversion efficiencies, while keeping fabrication costs low. However, several considerations regarding the materials, architectures and fabrication methods used need to be carefully evaluated to advance this field.
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11. 11
  Tsuboi, Y.; Shimizu, R.; Shoji, T.; Kitamura, N. Near-Infrared Continuous-Wave Light Driving a Two-Photon Photochromic Reaction with the Assistance of Localized Surface Plasmon J. Am. Chem. Soc. 2009, 131, 12623– 12627 DOI: 10.1021/ja9016655
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12. 12
  Wu, B. T.; Ueno, K.; Yokota, Y.; Sun, K.; Zeng, H. P.; Misawa, H. Enhancement of a Two-Photon-Induced Reaction in Solution Using Light-Harvesting Gold Nanodimer Structures J. Phys. Chem. Lett. 2012, 3, 1443– 1447 DOI: 10.1021/jz300370b
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  12
  Enhancement of a Two-Photon-Induced Reaction in Solution Using Light-Harvesting Gold Nanodimer Structures
  Wu, Botao; Ueno, Kosei; Yokota, Yukie; Sun, Kai; Zeng, Heping; Misawa, Hiroaki
  Journal of Physical Chemistry Letters (2012), 3 (11), 1443-1447CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
  We performed a quant. anal. of plasmon-assisted two-photon photochromic reactions on light-harvesting gold nanodimer structures. Our strategy for the quant. anal. of two-photon-induced photochem. reactions on gold nanostructures is using not only a confined photochem. reaction chamber but also a soln. system. The strong intensification of near-field light at the nanogap positions on gold nanodimer pairs promoted two-photon absorption by a closed-form diarylethene deriv., resulting in highly efficient photochromic conversion to the open-form structure.
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13. 13
  Zhong, Y.; Ueno, K.; Mori, Y.; Shi, X.; Oshikiri, T.; Murakoshi, K.; Inoue, H.; Misawa, H. Plasmon-Assisted Water Splitting Using Two Sides of the Same SrTiO₃ Single-Crystal Substrate: Conversion of Visible Light to Chemical Energy Angew. Chem., Int. Ed. 2014, 53, 10350– 10354 DOI: 10.1002/anie.201404926
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  13
  Plasmon-Assisted Water Splitting Using Two Sides of the Same SrTiO3 Single-Crystal Substrate: Conversion of Visible Light to Chemical Energy
  Zhong, Yuqing; Ueno, Kosei; Mori, Yuko; Shi, Xu; Oshikiri, Tomoya; Murakoshi, Kei; Inoue, Haruo; Misawa, Hiroaki
  Angewandte Chemie, International Edition (2014), 53 (39), 10350-10354CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)
  A plasmon-induced water splitting system that operates under irradn. by visible light was successfully developed; the system is based on the use of both sides of the same strontium titanate (SrTiO3) single-crystal substrate. The water splitting system contains two soln. chambers to sep. hydrogen (H2) and oxygen (O2). To promote water splitting, a chem. bias was applied by regulating the pH values of the chambers. The quantity of H2 evolved from the surface of platinum, which was used as a redn. co-catalyst, was twice the quantity of O2 evolved from an Au-nanostructured surface. Thus, the stoichiometric evolution of H2 and O2 was clearly demonstrated. The hydrogen-evolution action spectrum closely corresponds to the plasmon resonance spectrum, indicating that the plasmon-induced charge sepn. at the Au/SrTiO3 interface promotes water oxidn. and the subsequent redn. of a proton on the backside of the SrTiO3 substrate. The chem. bias is significantly reduced by plasmonic effects, which indicates the possibility of constructing an artificial photosynthesis system with low energy consumption.
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14. 14
  Oshikiri, T.; Ueno, K.; Misawa, H. Plasmon-Induced Ammonia Synthesis through Nitrogen Photofixation with Visible Light Irradiation Angew. Chem., Int. Ed. 2014, 53, 9802– 9805 DOI: 10.1002/anie.201404748
  [Crossref], [CAS], Google Scholar
  14
  Plasmon-Induced Ammonia Synthesis through Nitrogen Photofixation with Visible Light Irradiation
  Oshikiri, Tomoya; Ueno, Kosei; Misawa, Hiroaki
  Angewandte Chemie, International Edition (2014), 53 (37), 9802-9805CODEN: ACIEF5; ISSN:1433-7851. (Wiley-VCH Verlag GmbH & Co. KGaA)
  We have successfully developed a plasmon-induced technique for ammonia synthesis that responds to visible light through a strontium titanate (SrTiO3) photoelectrode loaded with gold (Au) nanoparticles. The photoelectrochem. reaction cell was divided into two chambers to sep. the oxidized (anodic side) and reduced (cathodic side) products. To promote NH3 formation, a chem. bias was applied by regulating the pH value of these compartments, and ethanol was added to the anodic chamber as a sacrificial donor. The quantity of NH3 formed at the ruthenium surface, which was used as a co-catalyst for SrTiO3, increases linearly as a function of time under irradn. with visible light at wavelengths longer than 550 nm. The NH3 formation action spectrum approx. corresponds to the plasmon resonance spectrum. We deduced that plasmon-induced charge sepn. at the Au/SrTiO3 interface promotes oxidn. at the anodic chamber and subsequent nitrogen redn. on the cathodic side.
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15. 15
  You, E. A.; Zhou, W.; Suh, J. Y.; Huntington, M. D.; Odom, T. W. Polarization-Dependent Multipolar Plasmon Resonances in Anisotropic Multiscale Au Particles ACS Nano 2012, 6, 1786– 1794 DOI: 10.1021/nn204845z
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16. 16
  Imura, K.; Nagahara, T.; Okamoto, H. Plasmon Mode Imaging of Single Gold Nanorods J. Am. Chem. Soc. 2004, 126, 12730– 12731 DOI: 10.1021/ja047836c
  [ACS Full Text ], [CAS], Google Scholar
  16
  Plasmon Mode Imaging of Single Gold Nanorods
  Imura, Kohei; Nagahara, Tetsuhiko; Okamoto, Hiromi
  Journal of the American Chemical Society (2004), 126 (40), 12730-12731CODEN: JACSAT; ISSN:0002-7863. (American Chemical Society)
  We have investigated two-photon-induced photoluminescence images and spectra of single gold nanorods by using an apertured scanning near-field optical microscope. The obsd. PL spectrum of single gold nanorod can be explained by the radiative recombination of the electron-hole pair near the X and L symmetry points. PL images reveal characteristic features reflecting an eigenfunction of a specific plasmon mode as well as elec. field distributions around the nanorod.
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17. 17
  Imura, K.; Nagahara, T.; Okamoto, H. Near-field Optical Imaging of Plasmon Modes in Gold Nanorods J. Chem. Phys. 2005, 122, 154701 DOI: 10.1063/1.1873692
  [Crossref], [PubMed], [CAS], Google Scholar
  17
  Near-field optical imaging of plasmon modes in gold nanorods
  Imura, Kohei; Nagahara, Tetsuhiko; Okamoto, Hiromi
  Journal of Chemical Physics (2005), 122 (15), 154701/1-154701/5CODEN: JCPSA6; ISSN:0021-9606. (American Institute of Physics)
  We have investigated optical properties of single gold nanorods by using an apertured-type scanning near-field optical microscope. Near-field transmission spectrum of single gold nanorod shows several longitudinal surface plasmon resonances. Transmission images obsd. at these resonance wavelengths show oscillating pattern along the long axis of the nanorod. The no. of oscillation increases with decrement of observing wavelength. These spatial characteristics were well reproduced by calcd. local d.-of-states maps and were attributed to spatial characteristics of plasmon modes inside the nanorods. Dispersion relation for plasmons in gold nanorods was obtained by plotting the resonance frequencies of the plasmon modes vs. the wave vectors obtained from the transmission images.
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18. 18
  Denkova, D.; Verellen, N.; Silhanek, A. V.; Valev, V. K.; Van Dorpe, P.; Moshchalkov, V. V. Mapping Magnetic Near-Field Distributions of Plasmonic Nanoantennas ACS Nano 2013, 7, 3168– 3176 DOI: 10.1021/nn305589t
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19. 19
  Rossouw, D.; Couillard, M.; Vickery, J.; Kumacheva, E.; Botton, G. A. Multipolar Plasmonic Resonances in Silver Nanowire Antennas Imaged with a Subnanometer Electron Probe Nano Lett. 2011, 11, 1499– 1504 DOI: 10.1021/nl200634w
  [ACS Full Text ], [CAS], Google Scholar
  19
  Multipolar Plasmonic Resonances in Silver Nanowire Antennas Imaged with a Subnanometer Electron Probe
  Rossouw, D.; Couillard, M.; Vickery, J.; Kumacheva, E.; Botton, G. A.
  Nano Letters (2011), 11 (4), 1499-1504CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  We detect short-range surface plasmon-polariton (SR-SPP) resonances setup in individual silver nanoantenna structures at high-spatial resoln. with a scanning, subnanometer electron probe. Both even and odd multipolar resonant modes are resolved up to sixth order, and we measure their spatial distribution in relation to nanoantenna structures at energies down to 0.55 eV. Fabry-Perot type SR-SPP reflection phase shifts are calcd. from direct measurements of antinode spacings in high-resoln. plasmonic field maps. We observe resonant SR-SPP antinode bunching at nanoantenna terminals in high-order resonant modes, and antinode shifts in nonhomogeneous local environments. Finally, we achieve good agreement of our exptl. SR-SPP maps with numerical calcns. of photon excited near fields, using a novel integrated photon excitation geometry.
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20. 20
  Martin, J.; Kociak, M.; Mahfoud, Z.; Proust, J.; Gérard, D.; Plain, J. High-Resolution Imaging and Spectroscopy of Multipolar Plasmonic Resonances in Aluminum Nanoantennas Nano Lett. 2014, 14, 5517– 5523 DOI: 10.1021/nl501850m
  [ACS Full Text ], [CAS], Google Scholar
  20
  High-Resolution Imaging and Spectroscopy of Multipolar Plasmonic Resonances in Aluminum Nanoantennas
  Martin, Jerome; Kociak, Mathieu; Mahfoud, Zackaria; Proust, Julien; Gerard, Davy; Plain, Jerome
  Nano Letters (2014), 14 (10), 5517-5523CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  The authors report on the high resoln. imaging of multipolar plasmonic resonances in Al nanoantennas using EELS. Plasmonic resonances ranging from near-IR to UV are measured. The spatial distributions of the multipolar resonant modes are mapped and their energy dispersion is retrieved. The losses in the Al antennas are studied through the full width at half-max. of the resonances, unveiling the wt. of both interband and radiative damping mechanisms of the different multipolar resonances. In the blue-UV spectral range, high order resonant modes present a quality factor up to 8, 2 times higher than low order resonant modes at the same energy. Near-IR to UV tunable multipolar plasmonic resonances in Al nanoantennas with relatively high quality factors can be engineered. Al nanoantennas are thus an appealing alternative to Au or Ag ones in the visible and can be efficiently used for UV plasmonics.
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21. 21
  Hao, F.; Larsson, E. M.; Ali, T. A.; Sutherland, D. S.; Nordlander, P. Shedding Light on Dark Plasmons in Gold Nanorings Chem. Phys. Lett. 2008, 458, 262– 266 DOI: 10.1016/j.cplett.2008.04.126
  [Crossref], [CAS], Google Scholar
  21
  Shedding light on dark plasmons in gold nanorings
  Hao, Feng; Larsson, Elin M.; Ali, Tamer A.; Sutherland, Duncan S.; Nordlander, Peter
  Chemical Physics Letters (2008), 458 (4-6), 262-266CODEN: CHPLBC; ISSN:0009-2614. (Elsevier B.V.)
  The authors present an exptl. and theor. anal. of the optical properties of Au nanorings of different sizes and cross sections. For light polarized parallel to the ring, the optical spectrum can depend sensitively on the angle of incidence. For normal incidence, the spectrum was characterized by two dipolar ring resonances. As the angle of incidence becomes more oblique, several previously dark multipolar ring resonances appear in the spectra. The appearance of the multipolar resonances is a consequence of retardation and can be understood in simple general terms.
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22. 22
  Esteban, R.; Vogelgesang, R.; Dorfmüller, J.; Dmitriev, A.; Rockstuhl, C.; Etrich, C.; Kern, K. Direct Near-Field Optical Imaging of Higher Order Plasmonic Resonances Nano Lett. 2008, 8, 3155– 3159 DOI: 10.1021/nl801396r
  [ACS Full Text ], [CAS], Google Scholar
  22
  Direct Near-Field Optical Imaging of Higher Order Plasmonic Resonances
  Esteban, R.; Vogelgesang, R.; Dorfmueller, J.; Dmitriev, A.; Rockstuhl, C.; Etrich, C.; Kern, K.
  Nano Letters (2008), 8 (10), 3155-3159CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  The authors map in real space and by purely optical means near-field optical information of localized surface plasmon polariton (LSPP) resonances excited in nanoscopic particles. Careful polarization control enables apertureless scanning near-field optical microscopy (aSNOM) to image dipolar and quadrupolar LSPPs of the bare sample with high fidelity in both amplitude and phase. This establishes a routine method for in situ optical microscopy of plasmonic and other resonant structures under ambient conditions.
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23. 23
  Zhang, Y.; Jia, T. Q.; Zhang, S. A.; Feng, D. H.; Xu, Z. Z. Dipole, Quadrupole and Octupole Plasmon Resonance Modes in Non-Concentric Nanocrescent/Nanodisk Structure: Local Field Enhancement in the Visible and Near Infrared Regions Opt. Express 2012, 20, 2924– 2931 DOI: 10.1364/OE.20.002924
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24. 24
  Fang, Z. Y.; Cai, J. Y.; Yan, Z. B.; Nordlander, P.; Halas, N. J.; Zhu, X. Removing a Wedge from a Metallic Nanodisk Reveals a Fano Resonance Nano Lett. 2011, 11, 4475– 4479 DOI: 10.1021/nl202804y
  [ACS Full Text ], [CAS], Google Scholar
  24
  Removing a Wedge from a Metallic Nanodisk Reveals a Fano Resonance
  Fang, Zheyu; Cai, Junyi; Yan, Zhongbo; Nordlander, Peter; Halas, Naomi J.; Zhu, Xing
  Nano Letters (2011), 11 (10), 4475-4479CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  A wide variety of complex, multicomponent plasmonic nanostructures possess Fano resonances. Here the authors introduce a remarkably simple planar nanostructure, a single metallic nanodisk with a missing wedge-shaped slice, that supports a Fano resonance. In this geometry, the Fano line shape arises from the coupling between a hybridized plasmon resonance of the disk and a narrower quadrupolar mode supported by the edge of the missing wedge slice. As a consequence, both disk size and wedge angle control the properties of the resonance. A semianal. description of plasmon hybridization proves useful for analyzing the resulting line shape.
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25. 25
  Schnell, M.; García-Etxarri, A.; Huber, A. J.; Crozier, K.; Aizpurua, J.; Hillenbrand, R. Controlling the Near-Field Oscillations of Loaded Plasmonic Nanoantennas Nat. Photonics 2009, 3, 287– 291 DOI: 10.1038/nphoton.2009.46
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  25
  Controlling the near-field oscillations of loaded plasmonic nanoantennas
  Schnell, M.; Garcia-Etxarri, A.; Huber, A. J.; Crozier, K.; Aizpurua, J.; Hillenbrand, R.
  Nature Photonics (2009), 3 (5), 287-291CODEN: NPAHBY; ISSN:1749-4885. (Nature Publishing Group)
  Optical and IR antennas enable a variety of cutting-edge applications ranging from nanoscale photodetectors to highly sensitive biosensors. All these applications critically rely on the optical near-field interaction between the antenna and its load' (biomols. or semiconductors). However, it is largely unexplored how antenna loading affects the near-field response. Here, the authors use scattering-type near-field microscopy to monitor the evolution of the near-field oscillations of IR gap antennas progressively loaded with metallic bridges of varying size. The authors' results provide direct exptl. evidence that the local near-field amplitude and phase can be controlled by antenna loading, in excellent agreement with numerical calcns. By modeling the antenna loads as nanocapacitors and nanoinductors, the change of near-field patterns induced by the load can be understood within the framework of circuit theory. Targeted antenna loading provides an excellent means of engineering complex antenna configurations in coherent control applications, adaptive nano-optics and metamaterials.
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26. 26
  Tanaka, Y.; Ishiguro, H.; Fujiwara, H.; Yokota, Y.; Ueno, K.; Misawa, H.; Sasaki, K. Direct Imaging of Nanogap-Mode Plasmon-Resonant Fields Opt. Express 2011, 19, 7726– 7733 DOI: 10.1364/OE.19.007726
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27. 27
  Barnard, E. S.; Pala, R. A.; Brongersma, M. L. Photocurrent Mapping of Near-field Optical Antenna Resonances Nat. Nanotechnol. 2011, 6, 588– 593 DOI: 10.1038/nnano.2011.131
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  27
  Photocurrent mapping of near-field optical antenna resonances
  Barnard, Edward S.; Pala, Ragip A.; Brongersma, Mark L.
  Nature Nanotechnology (2011), 6 (9), 588-593CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)
  An increasing no. of photonics applications make use of nanoscale optical antennas that exhibit a strong, resonant interaction with photons of a specific frequency. The resonant properties of such antennas are conventionally characterized by far-field light scattering techniques. Many applications require quant. knowledge of the near-field behavior, and existing local field measurement techniques provide only relative, rather than abs., data. A photodetector platform that uses a Si-on-insulator substrate to spectrally and spatially map the abs. values of enhanced fields near any type of optical antenna by transducing local elec. fields into photocurrent is demonstrated. The resonant optical and materials properties are quantifiable of nanoscale (∼50 nm) and wavelength-scale (∼1 μm) metallic antennas as well as high refractive index semiconductor antennas. The data agree with light scattering measurements, full-field simulations, and intuitive resonator models.
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28. 28
  Nicoletti, O.; de la Peña, F.; Leary, R. K.; Holland, D. J.; Ducati, C.; Midgley, P. A. Three-Dimensional Imaging of Localized Surface Plasmon Resonances of Metal Nanoparticles Nature 2013, 502, 80– 84 DOI: 10.1038/nature12469
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  28
  Three-dimensional imaging of localized surface plasmon resonances of metal nanoparticles
  Nicoletti, Olivia; de la Pena, Francisco; Leary, Rowan K.; Holland, Daniel J.; Ducati, Caterina; Midgley, Paul A.
  Nature (London, United Kingdom) (2013), 502 (7469), 80-84CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
  The remarkable optical properties of metal nanoparticles are governed by the excitation of localized surface plasmon resonances (LSPRs). The sensitivity of each LSPR mode, whose spatial distribution and resonant energy depend on the nanoparticle structure, compn. and environment, has given rise to many potential photonic, optoelectronic, catalytic, photovoltaic, and gas- and bio-sensing applications. However, the precise interplay between the three-dimensional (3D) nanoparticle structure and the LSPRs is not always fully understood and a spectrally sensitive 3D imaging technique is needed to visualize the excitation on the nanometer scale. Here we show that 3D images related to LSPRs of an individual silver nanocube can be reconstructed through the application of electron energy-loss spectrum imaging, mapping the excitation across a range of orientations, with a novel combination of non-neg. matrix factorization, compressed sensing and electron tomog. Our results extend the idea of substrate-mediated hybridization of dipolar and quadrupolar modes predicted by theory, simulations, and electron and optical spectroscopy, and provide exptl. evidence of higher-energy mode hybridization. This work represents an advance both in the understanding of the optical response of noble-metal nanoparticles and in the probing, anal. and visualization of LSPRs.
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29. 29
  Leiderer, P.; Bartels, C.; König-Birk, J.; Mosbacher, M.; Boneberg, J. Imaging Optical Near-Fields of Nanostructures Appl. Phys. Lett. 2004, 85, 5370– 5372 DOI: 10.1063/1.1819990
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30. 30
  Ghenuche, P.; Cherukulappurath, S.; Taminiau, T. H.; van Hulst, N. F.; Quidant, R. Spectroscopic Mode Mapping of Resonant Plasmon Nanoantennas Phys. Rev. Lett. 2008, 101, 116805 DOI: 10.1103/PhysRevLett.101.116805
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  Spectroscopic Mode Mapping of Resonant Plasmon Nanoantennas
  Ghenuche, Petru; Cherukulappurath, Sudhir; Taminiau, Tim H.; van Hulst, Niek F.; Quidant, Romain
  Physical Review Letters (2008), 101 (11), 116805/1-116805/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
  The authors present spatially resolved spectral mode mapping of resonant plasmon gap antennas using two-photon luminescence microspectroscopy. The obtained maps are in good agreement with 3-dimensional calcns. of the antenna modes. The evolution of the modal field with wavelength, both in the gap and along the two coupled Au nanowires forming the antenna, is directly visualized. At resonance, the luminescence for the gap area is enhanced at least 80 times and a comparison with the antenna extremities shows a dynamical charge redistribution due to the near-field coupling between the two arms.
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31. 31
  Aeschlimann, M.; Brixner, T.; Fischer, A.; Kramer, C.; Melchior, P.; Pfeiffer, W.; Schneider, C.; Strüber, C.; Tuchscherer, P.; Voronine, D. V. Coherent Two-Dimensional Nanoscopy Science 2011, 333, 1723– 1726 DOI: 10.1126/science.1209206
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  Coherent Two-Dimensional Nanoscopy
  Aeschlimann, Martin; Brixner, Tobias; Fischer, Alexander; Kramer, Christian; Melchior, Pascal; Pfeiffer, Walter; Schneider, Christian; Strueber, Christian; Tuchscherer, Philip; Voronine, Dmitri V.
  Science (Washington, DC, United States) (2011), 333 (6050), 1723-1726CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)
  A spectroscopic method that dets. nonlinear quantum mech. response functions beyond the optical diffraction limit and allows direct imaging of nanoscale coherence is introduced. In established coherent 2-dimensional (2D) spectroscopy, 4-wave-mixing responses are measured using 3 ingoing waves and 1 outgoing wave; thus, the method is diffraction-limited in spatial resoln. In coherent 2D nanoscopy, 4 ingoing waves are used and the final state detected via photoemission electron microscopy, which has 50-nm spatial resoln. Local nanospectra from a corrugated Ag surface were recorded, and subwavelength 2D line shape variations were obsd. Plasmonic phase coherence of localized excitations persisted for ∼100 fs and exhibited coherent beats. The observations are best explained by a model in which coupled oscillators lead to Fano-like resonances in the hybridized dark- and bright-mode response.
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32. 32
  Kubo, A.; Onda, K.; Petek, H.; Sun, Z. J.; Jung, Y. S.; Kim, H. K. Femtosecond Imaging of Surface Plasmon Dynamics in a Nanostructured Silver Film Nano Lett. 2005, 5, 1123– 1127 DOI: 10.1021/nl0506655
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  32
  Femtosecond Imaging of Surface Plasmon Dynamics in a Nanostructured Silver Film
  Kubo, Atsushi; Onda, Ken; Petek, Hrvoje; Sun, Zhijun; Jung, Yun S.; Kim, Hong Koo
  Nano Letters (2005), 5 (6), 1123-1127CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  Light interacting with nanostructured metals excites the collective charge d. fluctuations known as surface plasmons (SP). Through excitation of the localized SP eigenmodes incident light is trapped on the nanometer spatial and femtosecond temporal scales and its field is enhanced. Here we demonstrate the imaging and quantum control of SP dynamics in a nanostructured silver film. By inducing and imaging the nonlinear two-photon photoemission from the sample with a pair of identical 10-fs laser pulses while scanning the pulse delay, we record a movie of SP fields at a rate of 330-as/frame.
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33. 33
  Kubo, A.; Pontius, N.; Petek, H. Femtosecond Microscopy of Surface Plasmon Polariton Wave Packet Evolution at the Silver/Vacuum Interface Nano Lett. 2007, 7, 470– 475 DOI: 10.1021/nl0627846
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  33
  Femtosecond Microscopy of Surface Plasmon Polariton Wave Packet Evolution at the Silver/Vacuum Interface
  Kubo, Atsushi; Pontius, Niko; Petek, Hrvoje
  Nano Letters (2007), 7 (2), 470-475CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  A movie of the dispersive and dissipative propagation of surface plasmon polariton (SPP) wave packets at a Ag/vacuum interface is recorded by the interferometric time-resolved photoemission electron microscopy with 60 nm spatial resoln. and 330 as frame interval. The evolution of SPP wave packets is imaged through a two-path interference created by a pair of 10 fs phase correlated pump-probe light pulses at 400 nm. The wave packet evolution is simulated using the complex dielec. function of Ag.
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34. 34
  Schertz, F.; Schmelzeisen, M.; Mohammadi, R.; Kreiter, M.; Elmers, H. J.; Schönhense, G. Near Field of Strongly Coupled Plasmons: Uncovering Dark Modes Nano Lett. 2012, 12, 1885– 1890 DOI: 10.1021/nl204277y
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  34
  Near Field of Strongly Coupled Plasmons: Uncovering Dark Modes
  Schertz, Florian; Schmelzeisen, Marcus; Mohammadi, Reza; Kreiter, Maximilian; Elmers, Hans-Joachim; Schoenhense, Gerd
  Nano Letters (2012), 12 (4), 1885-1890CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  Strongly coupled plasmons in a system of individual Au nanoparticles placed at sub-nm distance to a Au film (nanoparticle-on-plane, NPOP) are studied using 2 complementary single particle spectroscopy techniques. Optical scattering spectroscopy exclusively detects plasmon modes that couple to the far field via their dipole moment (bright modes). By using photoemission electron microscopy (PEEM), the authors detect in the identical NPOPs near-field modes that do not couple to the scattered far field (dark modes) and are characterized by a strongly enhanced nonlinear electron emission process. Both far- and near-field spectroscopy were carried out for identical individual nanostructures interacting via a sub-nm gap. Strongly resonant electron emission occurs at excitation wavelengths far off-resonant in the scattering spectra.
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35. 35
  Lemke, C.; Schneider, C.; Leißner, T.; Bayer, D.; Radke, J. W.; Fischer, A.; Melchior, P.; Evlyukhin, A. B.; Chichkov, B. N.; Reinhardt, C.; Bauer, M.; Aeschlimann, M. Spatiotemporal Characterization of SPP Pulse Propagation in Two-Dimensional Plasmonic Focusing Devices Nano Lett. 2013, 13, 1053– 1058 DOI: 10.1021/nl3042849
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  35
  Spatiotemporal Characterization of SPP Pulse Propagation in Two-Dimensional Plasmonic Focusing Devices
  Lemke, Christoph; Schneider, Christian; Leissner, Till; Bayer, Daniela; Radke, Joern W.; Fischer, Alexander; Melchior, Pascal; Evlyukhin, Andrey B.; Chichkov, Boris N.; Reinhardt, Carsten; Bauer, Michael; Aeschlimann, Martin
  Nano Letters (2013), 13 (3), 1053-1058CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  The spatiotemporal evolution of a SPP wave packet with femtosecond duration is exptl. studied in 2 different plasmonic focusing structures. A 2-dimensional reconstruction of the plasmonic field in space and time is possible by the numerical anal. of interferometric time-resolved photoemission electron microscopy data. The time-integrated and time-resolved view onto the wave packet dynamics allow 1 to characterize and compare the capabilities of 2-dimensional components for use in plasmonic devices operating with ultrafast pulses.
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36. 36
  Cinchetti, M.; Gloskovskii, A.; Nepjiko, S. A.; Schönhense, G.; Rochholz, H.; Kreiter, M. Photoemission Electron Microscopy as a Tool for the Investigation of Optical Near Fields Phys. Rev. Lett. 2005, 95, 047601 DOI: 10.1103/PhysRevLett.95.047601
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  36
  Photoemission electron microscopy as a tool for the investigation of optical near fields
  Cinchetti, M.; Gloskovskii, A.; Nepjiko, S. A.; Schonhense, G.; Rochholz, H.; Kreiter, M.
  Physical Review Letters (2005), 95 (4), 047601/1-047601/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
  Photoemission electron microscopy was used to image the electrons photoemitted from specially tailored Ag nanoparticles deposited on a Si substrate (with its native oxide SiOx). Photoemission was induced by illumination with a Hg UV lamp (photon energy cutoff ℏ ωUV = 5.0 eV, wavelength λUV = 250 nm) and with a Ti:sapphire femtosecond laser (ℏ ωl = 3.1 eV, λl = 400 nm, pulse width <200 fs), resp. While homogeneous photoelectron emission from the metal is obsd. upon illumination at energies above the Ag plasmon frequency, at lower photon energies the emission is localized at tips of the structure. This is interpreted as a signature of the local elec. field therefore providing a tool to map the optical near field with the resoln. of emission electron microscopy.
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37. 37
  Sun, Q.; Ueno, K.; Yu, H.; Kubo, A.; Matsuo, Y.; Misawa, H. Direct Imaging of the Near Field and Dynamics of Surface Plasmon Resonance on Gold Nanostructures Using Photoemission Electron Microscopy Light: Sci. Appl. 2013, 2, e118 DOI: 10.1038/lsa.2013.74
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  37
  Direct imaging of the near field and dynamics of surface plasmon resonance on gold nanostructures using photoemission electron microscopy
  Sun, Quan; Ueno, Kosei; Yu, Han; Kubo, Atsushi; Matsuo, Yasutaka; Misawa, Hiroaki
  Light: Science & Applications (2013), 2 (Dec.), e118CODEN: LSAIAZ; ISSN:2047-7538. (Nature Publishing Group)
  Localized surface plasmon resonance (LSPR) can be supported by metallic nanoparticles and engineered nanostructures. An understanding of the spatially resolved near-field properties and dynamics of LSPR is important, but remains exptl. challenging. We report exptl. studies toward this aim using photoemission electron microscopy (PEEM) with high spatial resoln. of sub-10 nm. Various engineered gold nanostructure arrays (such as rods, nanodisk-like particles and dimers) are investigated via PEEM using near-IR (NIR) femtosecond laser pulses as the excitation source. When the LSPR wavelengths overlap the spectrum of the femtosecond pulses, the LSPR is efficiently excited and promotes multiphoton photoemission, which is correlated with the local intensity of the metallic nanoparticles in the near field. Thus, the local field distribution of the LSPR on different Au nanostructures can be directly explored and discussed using the PEEM images. In addn., the dynamics of the LSPR is studied by combining interferometric time-resolved pump-probe technique and PEEM. Detailed information on the oscillation and dephasing of the LSPR field can be obtained. The results identify PEEM as a powerful tool for accessing the near-field mapping and dynamic properties of plasmonic nanostructures.
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38. 38
  Lecarme, O.; Sun, Q.; Ueno, K.; Misawa, H. Robust and Versatile Light Absorption at Near-Infrared Wavelengths by Plasmonic Aluminum Nanorods ACS Photonics 2014, 1, 538– 546 DOI: 10.1021/ph500096q
  [ACS Full Text ], [CAS], Google Scholar
  38
  Robust and Versatile Light Absorption at Near-Infrared Wavelengths by Plasmonic Aluminum Nanorods
  Lecarme, Olivier; Sun, Quan; Ueno, Kosei; Misawa, Hiroaki
  ACS Photonics (2014), 1 (6), 538-546CODEN: APCHD5; ISSN:2330-4022. (American Chemical Society)
  The authors study the far-field and near-field properties of Al nanorods fabricated by electron beam lithog. and exhibiting plasmonic resonance in the near-IR region. First, plasmonic modes within nanorod arrays can be tuned by geometrical parameters, allowing 1 to control the system transparency. Next, the light absorption in this structure is closely examd., and Al has great potential due to its unique interband transition at 800 nm. The roles of the dielec. confinement and the coupling between plasmonic resonance and the interband transition are particularly emphasized, as their adjustment can be used to switch from highly scattering particles to absorbing particles without a significant modification of the plasmonic resonance position. Finally, the authors image the plasmon-generated local field distribution in the Al nanostructures and observe, for the 1st time, the effect of the interband transition on the near-field behavior. The effect of the dielec. confinement is also numerically studied, as it is shown to play a significant role in near-field enhancement.
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39. 39
  Lamprecht, B.; Krenn, J. R.; Leitner, A.; Aussenegg, F. R. Resonant and Off-Resonant Light-Driven Plasmons in Metal Nanoparticles Studied by Femtosecond-resolution Third-harmonic Generation Phys. Rev. Lett. 1999, 83, 4421– 4424 DOI: 10.1103/PhysRevLett.83.4421
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  39
  Resonant and Off-Resonant Light-Driven Plasmons in Metal Nanoparticles Studied by Femtosecond-Resolution Third-Harmonic Generation
  Lamprecht, B.; Krenn, J. R.; Leitner, A.; Aussenegg, F. R.
  Physical Review Letters (1999), 83 (21), 4421-4424CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
  The authors report on a femtosecond-resoln. study of the plasmon fields in Au nanoparticles using 3rd-harmonic generation. Controlled resonant and off-resonant plasmon excitation is achieved by tailoring the nanoparticle sample by an electron-beam-lithog. method. Comparing the measured 3rd order interferometric autocorrelation function of the plasmon field with simulations based on a simple harmonic oscillator model the authors ext. the temporal characteristic of the plasmon oscillation. For off-resonant excitation of particle plasmons the authors find a beating between the driving laser field and the plasmon field which demonstrates clearly the nature of the plasmon as a collective electron oscillation.
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40. 40
  Hanke, T.; Krauss, G.; Träutlein, D.; Wild, B.; Bratschitsch, R.; Leitenstorfer, A. Efficient Nonlinear Light Emission of Single Gold Optical Antennas Driven by Few-Cycle Near-Infrared Pulses Phys. Rev. Lett. 2009, 103, 257404 DOI: 10.1103/PhysRevLett.103.257404
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  40
  Efficient Nonlinear Light Emission of Single Gold Optical Antennas Driven by Few-Cycle Near-Infrared Pulses
  Hanke, T.; Krauss, G.; Trautlein, D.; Wild, B.; Bratschitsch, R.; Leitenstorfer, A.
  Physical Review Letters (2009), 103 (25), 257404/1-257404/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
  Individual nanometer-sized plasmonic antennas are excited resonantly with few-cycle laser pulses in the near IR. Intense 3rd-harmonic emission of visible light prevails for fundamental photon energies <1.1 eV. Interband luminescence and 2nd harmonic generation occur solely at higher driving frequencies. The authors attribute these findings to multiphoton resonances with the d-band transitions of Au. The strong 3rd-order signal allows direct measurement of a subcycle plasmon dephasing time of 2 fs, highlighting the efficient radiation coupling and broadband response of the devices.
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41. 41
  Grubisic, A.; Schweikhard, V.; Baker, T. A.; Nesbitt, D. J. Coherent Multiphoton Photoelectron Emission from Single Au Nanorods: The Critical Role of Plasmonic Electric Near-Field Enhancement ACS Nano 2013, 7, 87– 99 DOI: 10.1021/nn305194n
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  41
  Coherent Multiphoton Photoelectron Emission from Single Au Nanorods: The Critical Role of Plasmonic Electric Near-Field Enhancement
  Grubisic, Andrej; Schweikhard, Volker; Baker, Thomas A.; Nesbitt, David J.
  ACS Nano (2013), 7 (1), 87-99CODEN: ANCAC3; ISSN:1936-0851. (American Chemical Society)
  Electron emission from individual Au nanorods deposited on In-Sn-oxide (ITO) following excitation with femtosecond laser pulses near the rod longitudinal plasmon resonance is studied via scanning photoionization microscopy. The measured electron signal strongly depends on the excitation laser polarization and wavelength. Correlated secondary electron microscopy (SEM) and dark-field microscopy (DFM) studies of the same nanorods unambiguously confirm that max. electron emission results from (i) laser polarization aligned with the rod long axis and (ii) laser wavelength resonant with the localized surface plasmon resonance. The exptl. results are in good agreement with quant. predictions for a coherent multiphoton photoelec. effect, which is identified as the predominant electron emission mechanism for metal nanoparticles under employed excitation conditions. According to this mechanism, the multiphoton photoemission rate is increased by over 10 orders of magnitude in the vicinity of a localized surface plasmon resonance, due to enhancement of the incident electromagnetic field in the particle near-field. These findings identify multiphoton photoemission as an extremely sensitive metric of local elec. fields (i.e., hot spots) in plasmonic nanoparticles/structures that can potentially be exploited for direct quantitation of local elec. field enhancement factors.
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42. 42
  Mårsell, E.; Losquin, A.; Svärd, R.; Miranda, M.; Guo, C.; Harth, A.; Lorek, E.; Mauritsson, J.; Arnold, C. L.; Xu, H. X.; L’Huillier, A.; Mikkelsen, A. Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna Nano Lett. 2015, 15, 6601– 6608 DOI: 10.1021/acs.nanolett.5b02363
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  42
  Nanoscale Imaging of Local Few-Femtosecond Near-Field Dynamics within a Single Plasmonic Nanoantenna
  Marsell Erik; Losquin Arthur; Svard Robin; Miranda Miguel; Guo Chen; Harth Anne; Lorek Eleonora; Mauritsson Johan; Arnold Cord L; Xu Hongxing; L'Huillier Anne; Mikkelsen Anders; Xu Hongxing
  Nano letters (2015), 15 (10), 6601-8 ISSN:.
  The local enhancement of few-cycle laser pulses by plasmonic nanostructures opens up for spatiotemporal control of optical interactions on a nanometer and few-femtosecond scale. However, spatially resolved characterization of few-cycle plasmon dynamics poses a major challenge due to the extreme length and time scales involved. In this Letter, we experimentally demonstrate local variations in the dynamics during the few strongest cycles of plasmon-enhanced fields within individual rice-shaped silver nanoparticles. This was done using 5.5 fs laser pulses in an interferometric time-resolved photoemission electron microscopy setup. The experiments are supported by finite-difference time-domain simulations of similar silver structures. The observed differences in the field dynamics across a single particle do not reflect differences in plasmon resonance frequency or dephasing time. They instead arise from a combination of retardation effects and the coherent superposition between multiple plasmon modes of the particle, inherent to a few-cycle pulse excitation. The ability to detect and predict local variations in the few-femtosecond time evolution of multimode coherent plasmon excitations in rationally synthesized nanoparticles can be used in the tailoring of nanostructures for ultrafast and nonlinear plasmonics.
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43. 43
  Grubisic, A.; Ringe, E.; Cobley, C. M.; Xia, Y. N.; Marks, L. D.; Van Duyne, R. P.; Nesbitt, D. J. Plasmonic Near-Electric Field Enhancement Effects in Ultrafast Photoelectron Emission: Correlated Spatial and Laser Polarization Microscopy Studies of Individual Ag Nanocubes Nano Lett. 2012, 12, 4823– 4829 DOI: 10.1021/nl302271u
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  Plasmonic Near-Electric Field Enhancement Effects in Ultrafast Photoelectron Emission: Correlated Spatial and Laser Polarization Microscopy Studies of Individual Ag Nanocubes
  Grubisic, Andrej; Ringe, Emilie; Cobley, Claire M.; Xia, Younan; Marks, Laurence D.; Van Duyne, Richard P.; Nesbitt, David J.
  Nano Letters (2012), 12 (9), 4823-4829CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
  Electron emission from single, supported Ag nanocubes excited with ultrafast laser pulses (λ = 800 nm) is studied via spatial and polarization correlated (i) dark field scattering microscopy (DFM), (ii) scanning photoionization microscopy (SPIM), and (iii) high-resoln. TEM (HRTEM). Laser-induced electron emission is found to peak for laser polarization aligned with cube diagonals, suggesting the crit. influence of plasmonic near-field enhancement of the incident elec. field on the overall electron yield. For laser pulses with photon energy below the metal work function, coherent multiphoton photoelectron emission (MPPE) is identified as the most probable mechanism responsible for electron emission from Ag nanocubes and likely metal nanoparticles/surfaces in general.
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44. 44
  Sönnichsen, C.; Franzl, T.; Wilk, T.; von Plessen, G.; Feldmann, J.; Wilson, O.; Mulvaney, P. Drastic Reduction of Plasmon Damping in Gold Nanorods Phys. Rev. Lett. 2002, 88, 077402 DOI: 10.1103/PhysRevLett.88.077402
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  Drastic Reduction of Plasmon Damping in Gold Nanorods
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  Physical Review Letters (2002), 88 (7), 077402/1-077402/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
  The dephasing of particle plasmons was studied using light-scattering spectroscopy on individual Au nanoparticles. The authors find a drastic redn. of the plasmon dephasing rate in nanorods as compared to small nanospheres due to a suppression of interband damping. The rods studied here also show very little radiation damping, due to their small vols. These findings imply large local-field enhancement factors and relatively high light-scattering efficiencies, making metal nanorods extremely interesting for optical applications. Comparison with theory shows that pure dephasing and interface damping give negligible contributions to the total plasmon dephasing rate.
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  Optical constants of the noble metals
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  The optical consts. n and k were obtained for Cu, Ag, and Au from reflection and transmission measurements on vacuum-evapd. thin films at room temp., in the spectral range 0.5-6.5 eV. The film-thickness range was 185-500 Å. Three optical measurements were inverted to obtain the film thickness d as well as n and k. The estd. error in d was ±2 Å, and that in n, k was <0.02 over most of the spectral range. The results in the film-thickness range 250-500 Å were independent of thickness, and were unchanged after vacuum annealing or aging in air. The free-electron optical effective masses and relaxation times derived from the results in the near ir agreed satisfactorily with previous values. The interband contribution to the imaginary part of the dielec. const. was obtained by subtracting the free-electron contribution. Some recent theor. calcns. were compared with the results for Cu and Au. In addn., some other recent expts. are crit. compared with the present results.
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The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acsnano.6b00715.
- PEEM images of the Au nanoblocks excited with five different wavelengths under three different incidence conditions, near-field photoemission spectra under normal incidence, near-field photoemission spectra of the sample for time-resolved PEEM measurements, characterization of the incident laser field on the PEEM sample position, modeling the time-resolved photoemission signal, and some supplementary calculations of time-resolved photoemission signal (PDF)
- nn6b00715_si_001.pdf (861.76 kb)
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Dissecting the Few-Femtosecond Dephasing Time of Dipole and Quadrupole Modes in Gold Nanoparticles Using Polarized Photoemission Electron Microscopy

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Characterization of Topography and Far-Field Spectra