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Ultrafast Transient Holographic Microscopy
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Nano Letters

Cite this: Nano Lett. 2021, 21, 4, 1666–1671
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https://doi.org/10.1021/acs.nanolett.0c04416
Published February 4, 2021

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Abstract

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Nanotechnology is increasingly being applied in many emerging technologies, ranging from metamaterials to next-generation nanodrugs. A key ingredient for its success is the ability to specifically tailor ultrafast nanoscale light–matter interactions over very large areas. Unfortunately, dynamic imaging by ultrafast nanoscopy so far remains limited to very small 2D areas. This shortcoming prevents connecting single-particle observations with large-scale functionality. Here, we address this experimental challenge by combining concepts of ultrafast spectroscopy, wide-field nanoscopy, and digital holography. We introduce an ultrafast holographic transient microscope for wide-field transient nanoscale imaging with high frequency all-optical signal demodulation. We simultaneously record ultrafast transient dynamics of many individual nano-objects and demonstrate time-resolved spectroscopy of gold nanoparticles over a large volume irrespective of their x–y–z position. Our results pave the way to single-shot 3D microscopy of 2D and 3D materials on arbitrary time scales from femtosecond carrier dynamics in optoelectronic materials to millisecond dynamics in complex tissues.

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Ultrafast nanoscopy is an emerging technology for studying transient phenomena on subwavelength scales (1−6) such as energy flow in semiconductor devices or the spectro-temporal dynamics of single nanoparticles and even single molecules. (7−9) Despite these advances, observations remain limited to very small 2D areas, which hinders single-shot capture of spatiotemporal images or the acquisition of sufficiently large data sets that allow quantifying the heterogeneous nature of many nanomaterials. As such, ultrafast studies of novel materials to visualize, for example, the temporal switching of metamaterials (10) or quantify light–matter interactions in strongly coupled systems (11) remain challenging to implement. Additionally, experiments addressing spatially more complex phenomena such as visualizing carrier diffusion in 3D (12) or quantifying the uptake and photoinduced heating of theranostic agents in tissue (9,13) are currently near-impossible to implement. Ideally, large field-of-view 3D transient nanoscopy would alleviate these limitations but requires high-frequency signal demodulation, which is currently incompatible with the typical frame rates of 2D cameras.
Here, we implement an all-optical ultrafast holographic transient (UHT) lock-in microscope that allows signal demodulation at arbitrary frequencies, independent of the camera frame rate. We demonstrate its broad applicability by simultaneously imaging dozens of individual gold nanoparticles (NPs) with diameters ranging from 20 to 100 nm, and simultaneously following their transient dynamics. We furthermore show that UHT microscopy is capable of computationally refocusing out-of-focus particles, thus paving the way toward 3D localization microspectroscopy over large volumes of view.
Figure 1a schematically depicts an experimental implementation of the UHT microscope, which can be conceptually separated into imaging and interference subsections. The former consists of collinear pump and probe pulses illuminating the sample and a dark-field microscope that images the sample-scattering onto a CMOS camera (Methods). As in a conventional transient absorption experiment, a chopper modulates the pump and the probe interrogates the sample in the presence and absence of photoexcitation as a function of pump–probe time delay.

Figure 1

Figure 1. UHT microscope: an all-optical lock-in camera. (a) Experimental implementation of UHT microscopy with transient pump-delayed-probe imaging, and interference with modulated reference beams, allowing all-optical lock-in wide-field imaging on a camera. SHG, second harmonic generation; NOPA, noncollinear optical parametric amplifier. (b) Chopping scheme employed, 1/f = 1 ms is the time between individual laser pulses with f being the repetition rate of the laser system. (c) Data-processing workflow allowing retrieval of the scattering images for the pumped and unpumped sample by Fourier filtering in k-space. (d) Fluctuations of the radius of the pumpOFF (blue) and pumpON (pink) interference signals, recorded at 10 frames-per-second (FPS), alongside their ratio (black, dashed). (e) Relative pumpOFF/pumpON signal fluctuations recorded at 100 FPS (pink) and 10 FPS (purple) compared to shot-noise distributions (blue dashed lines) exhibiting 104 and 105 photons, respectively.

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The UHT microscope relies on multiplexed off-axis holography (14−16) to avoid restricting the pump modulation frequency to half the camera frame rate (17) and allow simultaneous recording of both pumped and unpumped images in a single camera exposure (Figure 1a). We generate suitable reference waves for the holographic experiment by diffracting a fraction of the probe pulse with a 2D 0-π phase grating and relay-image two of the first diffraction orders onto the camera, where they interfere with the sample scattering (Methods). (16,18,19) A mechanical chopper, placed in the Fourier plane of the relay-imaging system, ensures that one diffraction order illuminates the camera when the pump is blocked and the other when the pump illuminates the sample (Figure 1a,b). This experimental implementation allows separating pumpOFF and pumpON images in a holographic postprocessing step, (16,20) as can be understood by considering the total signal acquired on the camera, Iimage
where ErOFF and ErON are the electric fields of the references waves in the absence and presence of the pump pulse and ESOFF and EsON are the corresponding signal waves; c.c. stands for complex conjugate. As indicated in Figure 1a, ErON and ErOFF exhibit different wavevectors thus moving the interference terms, ErOFF*EsOFF + ErON*EsON + c.c., to distinct positions in momentum-space. (21) They are hence easily accessible via a spatial Fourier transformation of the raw image, which reveals the diagonally shifted interference terms reminiscent of the microscope’s back-focal-plane with the dark-field stop being visible in its center covering approximately one-third of the radius (Figure 1c, Supporting Information and Methods). Fourier-filtering (20) is hence sufficient to isolate the images acquired in the presence and absence of the pump. The simultaneous recording of pumpON and pumpOFF images for consecutive pulses in a single exposure, furthermore, allows removing strongly correlated fluctuations by dividing the two (Figure 1d), and enables transient imaging near the shot-noise limit (Figure 1e). Our UHT microscope thus acts as an all-optical wide-field lock-in camera, which allows selecting arbitrary modulation frequencies and signal integration times with only the latter being determined by the camera exposure time. Compared to traditional lock-in amplifier-based demodulation approaches in a point-scanning configuration, (3,4) UHT microscopy directly demodulates entire 2D images, but crucially relies on the coherent nature of the signal of interest.
To demonstrate the capability of UHT microscopy to record temporally-resolved wide-field dynamics, we perform experiments on a sample composed of many individual 100 nm diameter gold NPs. Figure 2a shows an image acquired with a 540 nm probe pulse, where the diffraction-limited spots are due to scattering of individual NPs. A 400 nm pump pulse photoexcites the NPs and we simultaneously record pumpOFF and pumpON images as a function of pump-probe delay as outlined above. These image stacks allow accessing the transient dynamics of all individual NPs simultaneously by comparing their integrated scattering signal in the absence and presence of the pump (Figure 2b). At negative time delays, we observe nearly identical scattering signals, followed by a considerable pumpON signal decrease at positive delays rising within the ∼200 fs instrumental response function. The transient signal shows the typical picosecond cooling dynamics of metallic nanoparticles due to thermalization of the hot electron distribution with the phonon bath. (2,22,23)

Figure 2

Figure 2. Wide-field transient imaging of single nanoparticles. (a) PumpOFF image of individual 100 nm Au-NPs. (b) Time-delay dependent scattering signal magnitudes at a probe wavelength of 540 nm for the five individual particles encircled in (a) recorded in the presence (pink) and absence (blue) of the 400 nm pump pulse with a fluence of 1.1 mJ/cm2. (c) Transient images within the dashed-rectangle in (a) for three different probe wavelengths as a function of pump–probe delay. From 540 to 500 nm, the NP transient-contrast inverts from negative to positive; note the black circles highlighting some NPs with signal-scaling that are considerably different from the average behavior (see Supporting Information for transient images of the entire field-of-view).

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When tuning the probe wavelength from 540 to 500 nm across the spectral region of the localized surface plasmon resonance (LSPR), (23,24) we observe a sign inversion of the transient signal, computed as ΔS(t) = ArONAsON(t) – ArOFFAsOFF(t), where AsON (AsOFF) and ArON (ArOFF) are the electric field amplitudes of signal and reference waves, defined as , in the presence (absence) of the pump (Figure 2c and Supplementary Figure 1). Importantly, we directly uncover subtle details beyond the ensemble picture, as individual particles show distinctly different behavior with widely varying signals, an observation that is especially pronounced at 520 nm.
Next, to fully resolve the spectro-temporal differences, we record wavelength-resolved UHT images by tuning the probe from 500 to 651 nm, while keeping the pump at 400 nm (Methods and Supplementary Figure 3 for additional experiments performed on 200 nm NPs). Figure 3a shows the time-dependent transient scattering signal, , for 76 simultaneously measured single NPs alongside their mean signal (Methods). The slight differences in decay kinetics (Figure 3a) are due to the varying pump fluence on the individual NPs, which results in different NP-heating and hence cooling dynamics, as verified by conducting additional measurements at different excitation fluences (Supplementary Figure 6).

Figure 3

Figure 3. UHT imaging of single nanoparticle spectro-temporal dynamics. (a) Spectrally resolved transient dynamics of 76 individual 100 nm Au NPs (colored) alongside the mean dynamics (black). The transients are offset for clarity with the dashed line indicating ΔS/S(t) = 0 for the individual wavelengths. The wavelength dependent probe fluences are adjusted within the 0.1–0.4 mJ/cm2 range and the pump fluence is 1.1 mJ/cm2 (at 1/e). (b) Temporal representation of the decay dynamics of the averaged transient scattering spectra. (c) Histogram representation of the ΔS/S(t) signal obtained by analyzing each individual NP in the 100–900 fs temporal window.

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Beyond the heating-induced differences, the 520–540 nm spectral region highlights the need for single-particle level spectroscopy as the mean signal fails to capture the widely differing transients. While the particle-averaged transient dynamics are a good estimate for the mean sample performance (Figure 3b), the underlying single-particle data paint a much more diverse picture (Figure 3c). Importantly, the histogram-spread is not due to experimental noise but a direct result of the size and shape heterogeneity of the NPs as well as their interaction with their specific nanoscopic environment. (25)
In line with previous experiments on gold NPs that predominantly monitored either transient absorption or transient extinction changes, we observe a broadening of the LSPR which results in a net bleach of the transition. (26−28) The initially excited hot electron distribution rapidly thermalizes with the lattice phonons within a few picoseconds, resulting in bleach recovery. The residual ΔS/S(t) signal at long delays (>40 ps) is due to the vibrationally hot NPs which slowly cool via NP-substrate coupling over time-scales far exceeding our experimental observation window. (29)
Having assessed the capability of UHT microscopy to perform wide-field transient imaging and spectroscopy, we evaluate the sensitivity of our method. The interferometric detection of the scattered field amplitude makes UHT microscopy particularly effective for detecting small NPs. To test the limits of recording wide-field transient NP dynamics we perform experiments while gradually reducing the particle diameter to 20 nm.
Figure 4a compares the holographically recorded scattering images of representative Au NPs of different sizes. As we reduce the particle size it becomes increasingly difficult to distinguish NP scattering and background. For 20 nm NPs, recorded in wide-field transmission geometry with a spatially coherent light source, both image contributions are essentially identical thus rendering the confident identification of the Au NPs with a standard holographic microscope as difficult to impossible. However, UHT microscopy is capable of recording transient images over a wide range of NP sizes (Figure 4a,b) that could even be boosted by approximately 1 order of magnitude by exchanging our NA = 0.5 objective for a higher NA oil-immersion objective.

Figure 4

Figure 4. Signal scaling for different particle sizes. (a) Holographic (left) and transient scattering images (right) recorded for NP-diameters ranging from 100 to 20 nm using a 400 nm pump and a 540 nm probe pulse (see Methods for fluences). Circles indicate NPs, diamonds indicate a representative background region. (b) Time-traces of the particles highlighted in (a); the scale-bar indicates the relative scattering signal normalized to both pump intensity and probe amplitude. Blue lines indicate signals obtained at a background region and pink lines indicate signals due to NPs.

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Thus far, we have concentrated on spectroscopic and sensitivity aspects of UHT microscopy and ignored its holographic imaging capabilities. Beyond enabling wide-field lock-in detection, off-axis holography interferometrically measures both amplitude and phase information of an image. This direct access to the full electric field allows digital image processing, such as computational focusing postacquisition, which enables 3D particle localization over large volumes-of-view from a single image. (30)Figure 5a shows the typical information obtained from a hologram, processed as outlined previously (Figure 1c), for a sample containing 100 nm Au NPs placed at different relative distances with respect to the focal plane. The defocused NPs show the expected point-spread-function reminiscent of the imaging system used but the phase term reveals additional information. Depending on the precise location of the individual NPs with respect to the focal plane, we observe different amounts of spherical phase as well as a curvature inversion as we move through the focus.

Figure 5

Figure 5. Digital refocusing of out-of-focus nanoparticles. (a) Scattering amplitude and phase of 100 nm Au NPs imaged below (left), above (center) and approximately in (right) the focal plane. (b) Representative images of the digitally refocused particles. (c) Transient wide-field-dynamics for the as-recorded, −1860 nm out-of-focus, image (top) as well as the refocused image obtained by computational back-propagation into focus (bottom).

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We computationally refocus the out-of-focus images with the angular spectrum method (21,31) (Methods) and obtain near-identical images, irrespective of whether the particles are imaged near or far away from the image plane (Figure 5b). The same approach can be applied to UHT microscopy, allowing transient imaging and 3D localization of out-of-focus particles. Figure 5c validates this statement by comparing transient scattering images, recorded −1860 nm out-of-focus, of a 100 nm Au NP-sample with their refocused versions. While we see signs of the transient signal in the as-recorded image, the digitally refocused transient images show clear NP signatures comparable to the previously presented in-focus experiments (Figures 2–4). Importantly, while we purposely chose a small defocus value of less than 2 μm, to allow visual identification of the individual NPs in the image, even >30 μm defocused images are easily propagated back into focus. (30,32)
To summarize, we implemented a novel holographic transient, or UHT, microscope that allows performing wide-field pump–probe imaging. The platform yields complex images, comprised of both amplitude and phase terms, in a lock-in amplifier-like fashion irrespective of the camera’s integration time. We demonstrated the platform’s viability by simultaneously recording the spectro-temporally resolved transient dynamics of several tens of gold NPs with diameters as small as 20 nm and single-particle sensitivity. We deliberately chose the well-established gold NP system to allow direct intraplatform comparison with, for example, photothermal microscopes to aid the rapid adoption of the UHT technology by interested researchers. Beyond the NPs’ dynamics, the simultaneously recorded phase information allows digital image propagation, thus paving the way toward recording transient dynamics of complex 3D samples and potentially transient absorption tomography. These advances are an important step toward highly multiplexed 3D transient absorption microscopy and will enable rationalizing structure–function relationships beyond 2D projections. Additionally, our results are highly relevant for single-particle tracking applications where background and photobleaching-free imaging methodologies are highly sought after. Especially for live cell and tissue imaging, our transient single-shot wide-field alternative to traditional point-scanning (33,34) photothermal microscopy eliminates the unfavorable temperature loss to the high heat-capacity solvent water and will allow real-time background-free imaging of intracellular processes over arbitrary observation times.

Methods

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UHT Microscope

Spectrally tunable pulses are generated by a home-built noncollinear optical parametric amplifier (NOPA), pumped by a 1 kHz, 100 fs amplified Ti:sapphire laser, as described previously. (35) The 400 nm pump-pulse is directly obtained by frequency doubling the laser output. A 90:10 beam splitter generates the probe and the reference from the NOPA output. The former is made collinear with the pump-pulse and focused onto the sample by means of a F = 200 mm achromatic lens. A home-built transmission dark-field microscope (NA = 0.5, Olympus RMS20X-PF), equipped with a dark-field mask in proximity of its back-focal-plane and a 488 nm long-pass filter (488 nm EdgeBasic, Semrock), images the sample scattering onto a CMOS camera (acA2040-90um Basler ace, Basler AG) at a nominal magnification of 37×. To allow holographic imaging we propagate the 10% probe-fraction through a relay-imaging system (nominal magnification 0.5×) onto the same CMOS camera and place a 2D 0-π phase grating (25.6 grooves/mm) into the conjugate image plane to allow interference over the entire camera chip. (19) We block all but two of the four first diffraction orders and modulate these two by means of a mechanical chopper thus separating pumpOFF and pumpON interference terms as described in detail in the main text. The time-delay between signal and reference pulses is adjusted by maximizing the fringe contrast with a mechanical delay line. Pump–probe time-delay dependent images are recorded by means of a computer-controlled translation stage (M-531.PD1, Physik Instrumente).

Sample Preparation

A cover glass (#1.5) is cleaned by 10 min sonication in acetone, 10 min sonication in Milli-Q water, drying under a stream of N2, followed by a 5 min oxygen plasma treatment (Femto, Diener electronic GmbH). The cleaned glass is then incubated with PLL-g-PEG (SuSoS AG) for approximately 10 min, followed by a dilute Au NP-solution with the diameter of choice (citrate capped 20, 40, 80, 100, 200 nm all BBI Solutions). Once the NPs are bound, the residual solution is removed and the substrate is used for the optical experiments. Prior to performing UHT experiments, we characterized all samples using a k-scope which is capable of accurately sizing Au NPs in the 20–250 nm size-range. (36)

Experimental Parameters

Unless stated differently, the pump/probe fluences throughout the manuscript are given as 1/e values. For the experiments presented in Figure 4, the fluences are the following: 100 nm NPs, 1.03 mJ/cm2 pump, 0.15 mJ/cm2 probe; 80 nm NPs, 1.74 mJ/cm2 pump, 0.39 mJ/cm2 probe; 40 and 20 nm NPs, 1.74 mJ/cm2 pump, 1.59 mJ/cm2 probe.

Angular Spectrum Method

We perform image-propagation via the angular spectrum method. (21) Briefly, the processed N × N holograms are convolved with a propagation kernel of the form
where km = 2nπ /λ, with n = 1 being the refractive index of air. The discretized spatial frequencies are (kx,ky) = 2π/nΔx(x,y) for (−N/2 ≤ x,y < N/2) with Δx representing the magnified pixel size of the imaging system.

ΔS/S(t) and ΔS

Because of the dark-field nature of the UHT microscope, image regions without particles exhibit amplitudes close to zero. As a result, the intuitive differential scattering expression, , which reports on the relative scattering signal change due to photoexcitation, cannot be computed for images as for many points ArOFFAsOFF ∼ 0. To nevertheless show UHT images we employ the signal differences, ΔS(t) = ArONAsON(t) – ArOFFAsOFF(t) when images are reported where ArOFFAsOFF(t) is often close to zero in regions where no particles are present.

Supporting Information

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.0c04416.

  • Expanded version of Figure 2, information regarding the data processing of the holograms, additional experiments performed on 200 nm Au NPs, pump-fluence dependent measurements as well as pump and probe spectra (PDF)

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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 Authors
  • Authors
    • Franco V. A. Camargo - IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, Piazza L. da Vinci 32, 20133 Milano, Italy
    • Giulio Cerullo - IFN-CNR, Dipartimento di Fisica, Politecnico di Milano, Piazza L. da Vinci 32, 20133 Milano, Italy;  Orcidhttp://orcid.org/0000-0002-9534-2702
  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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Authors acknowledge support by the Spanish Ministry of Science, Innovation, and Universities (MCIU/AEI: RTI2018-099957-J-I00 and PGC2018-096875-B-I00), the Ministry of Science and Innovations (MICINN “Severo Ochoa” program for Centers of Excellence in R&D CEX2019-000910-S), the Catalan AGAUR (2017SGR1369), Fundació Privada Cellex, Fundació Privada Mir-Puig, and the Generalitat de Catalunya through the CERCA program. N.F.v.H. acknowledges the financial support by the European Commission (ERC Advanced Grant 670949-LightNet). G.C. acknowledges support by the European Union Horizon 2020 Programme under Grant Agreement 881603 Graphene Core 3.

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    Single-mol. spectroscopy aims to unveil often hidden but potentially very important contributions of single entities to a system's ensemble response. Albeit contributing tremendously to our ever growing understanding of mol. processes, the fundamental question of temporal evolution, or change, has thus far been inaccessible, thus painting a static picture of a dynamic world. Here, we finally resolve this dilemma by performing ultrafast time-resolved transient spectroscopy on a single mol. By tracing the femtosecond evolution of excited electronic state spectra of single mols. over hundreds of nanometers of bandwidth at room temp., we reveal their nonlinear ultrafast response in an effective three-pulse scheme with fluorescence detection. A first excitation pulse is followed by a phase-locked de-excitation pulse pair, providing spectral encoding with 25 fs temporal resoln. This exptl. realization of true single-mol. transient spectroscopy demonstrates that two-dimensional electronic spectroscopy of single mols. is exptl. within reach. Frequency-resolved transient excited-state absorption of a single mol. is measured at room temp. The dynamic Stokes shift and vibrational cooling are directly measured with 25 fs temporal resoln. and a spectral detection bandwidth of hundreds of meV.
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    Guo, Z. Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy. Science (Washington, DC, U. S.) 2017, 356, 59– 62,  DOI: 10.1126/science.aam7744
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    Long-range hot-carrier transport in hybrid perovskites visualized by ultrafast microscopy
    Guo, Zhi; Wan, Yan; Yang, Mengjin; Snaider, Jordan; Zhu, Kai; Huang, Libai
    Science (Washington, DC, United States) (2017), 356 (6333), 59-62CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)
    The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 ps was obsd. in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. The authors report direct visualization of hot-carrier migration in methylammonium lead iodide (CH3NH3PbI3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was obsd. to correlate with excess kinetic energy, resulting in up to 230 nm transport distance that could overcome grain boundaries. The nonequil. transport persisted over tens of picoseconds and ∼600 nm before reaching the diffusive transport limit. These results suggest potential applications of hot-carrier devices based on hybrid perovskites.
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    Delor, M.; Weaver, H. L.; Yu, Q. Q.; Ginsberg, N. S. Imaging material functionality through three-dimensional nanoscale tracking of energy flow. Nat. Mater. 2020, 19, 56– 62,  DOI: 10.1038/s41563-019-0498-x
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    Imaging material functionality through three-dimensional nanoscale tracking of energy flow
    Delor, Milan; Weaver, Hannah L.; Yu, QinQin; Ginsberg, Naomi S.
    Nature Materials (2020), 19 (1), 56-62CODEN: NMAACR; ISSN:1476-1122. (Nature Research)
    The ability of energy carriers to move between atoms and mols. underlies biochem. and material function. Understanding and controlling energy flow, however, requires observing it on ultrasmall and ultrafast spatio-temporal scales, where energetic and structural roadblocks dictate the fate of energy carriers. Here, we developed a non-invasive optical scheme that leverages non-resonant interferometric scattering to track tiny changes in material polarizability created by energy carriers. We thus map evolving energy carrier distributions in four dimensions of spacetime with few-nanometer lateral precision and directly correlate them with material morphol. We visualize exciton, charge and heat transport in polyacene, silicon and perovskite semiconductors and elucidate how disorder affects energy flow in three dimensions. For example, we show that morphol. boundaries in polycryst. metal halide perovskites possess lateral- and depth-dependent resistivities, blocking lateral transport for surface but not bulk carriers. We also reveal strategies for interpreting energy transport in disordered environments that will direct the design of defect-tolerant materials for the semiconductor industry of tomorrow.
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    Shaltout, A. M.; Shalaev, V. M.; Brongersma, M. L. Spatiotemporal light control with active metasurfaces. Science (Washington, DC, U. S.) 2019, 364, eaat3100
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    Chikkaraddy, R. Single-molecule strong coupling at room temperature in plasmonic nanocavities. Nature 2016, 535, 127– 130,  DOI: 10.1038/nature17974
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    Single-molecule strong coupling at room temperature in plasmonic nanocavities
    Chikkaraddy, Rohit; de Nijs, Bart; Benz, Felix; Barrow, Steven J.; Scherman, Oren A.; Rosta, Edina; Demetriadou, Angela; Fox, Peter; Hess, Ortwin; Baumberg, Jeremy J.
    Nature (London, United Kingdom) (2016), 535 (7610), 127-130CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
    Photon emitters placed in an optical cavity experience an environment that changes how they are coupled to the surrounding light field. In the weak-coupling regime, the extn. of light from the emitter is enhanced. But more profound effects emerge when single-emitter strong coupling occurs: mixed states are produced that are part light, part matter, forming building blocks for quantum information systems and for ultralow-power switches and lasers. Such cavity quantum electrodynamics has until now been the preserve of low temps. and complicated fabrication methods, compromising its use. Here, by scaling the cavity vol. to less than 40 cubic nanometers and using host-guest chem. to align one to ten protectively isolated methylene-blue mols., we reach the strong-coupling regime at room temp. and in ambient conditions. Dispersion curves from more than 50 such plasmonic nanocavities display characteristic light-matter mixing, with Rabi frequencies of 300 millielectronvolts for ten methylene-blue mols., decreasing to 90 millielectronvolts for single mols.-matching quant. models. Statistical anal. of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-mol. strong coupling. This dressing of mols. with light can modify photochem., opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chem. bonds.
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    Ginsberg, N. S.; Tisdale, W. A. Spatially resolved photogenerated exciton and charge transport in emerging semiconductors. Annu. Rev. Phys. Chem. 2020, 71, 1– 30,  DOI: 10.1146/annurev-physchem-052516-050703
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    Spatially Resolved Photogenerated Exciton and Charge Transport in Emerging Semiconductors
    Ginsberg, Naomi S.; Tisdale, William A.
    Annual Review of Physical Chemistry (2020), 71 (), 1-30CODEN: ARPLAP; ISSN:0066-426X. (Annual Reviews)
    A review. We review recent advances in the characterization of electronic forms of energy transport in emerging semiconductors. The approaches described all temporally and spatially resolve the evolution of initially localized populations of photogenerated excitons or charge carriers. We first provide a comprehensive background for describing the phys. origin and nature of electronic energy transport both microscopically and from the perspective of the observer. We introduce the new family of far-field, time-resolved optical microscopies developed to directly resolve not only the extent of this transport but also its potentially temporally and spatially dependent rate. We review a representation of examples from the recent literature, including investigation of energy flow in colloidal quantum dot solids, org. semiconductors, org.-inorg. metal halide perovskites, and 2D transition metal dichalcogenides. These examples illustrate how traditional parameters like diffusivity are applicable only within limited spatiotemporal ranges and how the techniques at the core of this review,esp. when taken together, are revealing a more complete picture of the spatiotemporal evolution of energy transport in complex semiconductors, even as a function of their structural heterogeneities.
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    Nanomaterials for Theranostics: Recent Advances and Future Challenges
    Lim, Eun-Kyung; Kim, Taekhoon; Paik, Soonmyung; Haam, Seungjoo; Huh, Yong-Min; Lee, Kwangyeol
    Chemical Reviews (Washington, DC, United States) (2015), 115 (1), 327-394CODEN: CHREAY; ISSN:0009-2665. (American Chemical Society)
    There is no expanded citation for this reference.
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    Kühn, J. Real-time dual-wavelength digital holographic microscopy with a single hologram acquisition. Opt. Express 2007, 15, 7231– 7242,  DOI: 10.1364/OE.15.007231
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    Colomb, T. Polarization microscopy by use of digital holography: Application to optical-fiber birefringence measurements. Appl. Opt. 2005, 44, 4461– 4469,  DOI: 10.1364/AO.44.004461
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    Polarization microscopy by use of digital holography: application to optical-fiber birefringence measurements
    Colomb Tristan; Durr Florian; Cuche Etienne; Marquet Pierre; Limberger Hans G; Salathe Rene-Paul; Depeursinge Christian
    Applied optics (2005), 44 (21), 4461-9 ISSN:1559-128X.
    We present a digital holographic microscope that permits one to image polarization state. This technique results from the coupling of digital holographic microscopy and polarization digital holography. The interference between two orthogonally polarized reference waves and the wave transmitted by a microscopic sample, magnified by a microscope objective, is recorded on a CCD camera. The off-axis geometry permits one to reconstruct separately from this single hologram two wavefronts that are used to image the object-wave Jones vector. We applied this technique to image the birefringence of a bent fiber. To evaluate the precision of the phase-difference measurement, the birefringence induced by internal stress in an optical fiber is measured and compared to the birefringence profile captured by a standard method, which had been developed to obtain high-resolution birefringence profiles of optical fibers.
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    Rubin, M.; Dardikman, G.; Mirsky, S. K.; Turko, N. A.; Shaked, N. T. Six-pack off-axis holography. Opt. Lett. 2017, 42, 4611– 4614,  DOI: 10.1364/OL.42.004611
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    Six-pack off-axis holography
    Rubin Moran; Dardikman Gili; Mirsky Simcha K; Turko Nir A; Shaked Natan T
    Optics letters (2017), 42 (22), 4611-4614 ISSN:.
    We present a new holographic concept, named six-pack holography (6PH), in which we compress six off-axis holograms into a single multiplexed off-axis hologram without loss of magnification or resolution. The multiplexed hologram contains straight off-axis fringes with six different orientations, and can be generated optically or digitally. We show that since the six different complex wavefronts do not overlap in the spatial frequency domain, they can be fully reconstructed. 6PH allows more than 50% improvement in the spatial bandwidth consumption when compared to the best multiplexing method proposed so far. We expect the 6PH concept to be useful for a variety of applications, such as field-of-view multiplexing, wavelength multiplexing, temporal multiplexing, multiplexing for super-resolution imaging, and others.
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    Schnedermann, C. Sub-10 fs Time-Resolved Vibronic Optical Microscopy. J. Phys. Chem. Lett. 2016, 7, 4854– 4859,  DOI: 10.1021/acs.jpclett.6b02387
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    Sub-10 fs Time-Resolved Vibronic Optical Microscopy
    Schnedermann, Christoph; Lim, Jong Min; Wende, Torsten; Duarte, Alex S.; Ni, Limeng; Gu, Qifei; Sadhanala, Aditya; Rao, Akshay; Kukura, Philipp
    Journal of Physical Chemistry Letters (2016), 7 (23), 4854-4859CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
    Fmtosecond wide-field transient absorption microscopy combining sub-10 fs pump and probe pulses covering the complete visible (500-650 nm) and near-IR (650-950 nm) spectrum with diffraction-limited optical resoln. is introduced. The capabilities of the system were demonstrated by reporting the spatially- and spectrally-resolved transient electronic response of MAPbI3-xClx perovskite films and reveal significant quenching of the transient bleach signal at grain boundaries. The unprecedented temporal resoln. enables one to directly observe the formation of band-gap renormalization, completed in 25 fs after photoexcitation. The authors acquire hyperspectral Raman maps of TIPS pentacene films with sub-400 nm spatial and sub-15 cm-1 spectral resoln. covering the 100-2000 cm-1 window. The approach opens up the possibility of studying ultrafast dynamics on nanometer length and femtosecond time scales in a variety of 2-dimensional and nanoscopic systems.
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    Bon, P.; Maucort, G.; Wattellier, B.; Monneret, S. Quadriwave lateral shearing interferometry for quantitative phase microscopy of living cells. Opt. Express 2009, 17, 13080– 13094,  DOI: 10.1364/OE.17.013080
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    Quadriwave lateral shearing interferometry for quantitative phase microscopy of living cells
    Bon, Pierre; Maucort, Guillaume; Wattellier, Benoit; Monneret, Serge
    Optics Express (2009), 17 (15), 13080-13094CODEN: OPEXFF; ISSN:1094-4087. (Optical Society of America)
    Phase imaging with a high-resoln. wavefront sensor is considered. This is based on a quadriwave lateral shearing interferometer mounted on a non-modified transmission white-light microscope. The measurement technol. is explained both in the scope of wave optics and geometrical optics in order to discuss its implementation on a conventional microscope. In particular we consider the effect of a non spatially coherent source on the phase-image signal-to-noise ratio. Precise measurements of the phase-shift introduced by microscopic beads or giant unilamellar vesicles validate the principle and show the accuracy of the methods. Diffraction limited images of living COS-7 cells are then presented, with a particular focus on the membrane and organelle dynamics.
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    Maznev, A. A.; Crimmins, T. F.; Nelson, K. A. How to make femtosecond pulses overlap. Opt. Lett. 1998, 23, 1378– 1380,  DOI: 10.1364/OL.23.001378
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    How to make femtosecond pulses overlap
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    Optics letters (1998), 23 (17), 1378-80 ISSN:0146-9592.
    Normally, femtosecond light pulses that cross at a nonzero angle overlap over only a small region in space. This limitation can be overcome by the use of diffraction orders of a grating. We consider an arrangement in which, on diffraction of a femtosecond pulse by a grating, two beams that correspond to the first-order diffraction maxima are recombined at the image plane by a system of two confocal lenses. In this arrangement the beams overlap over the their full aperture, with the short duration of the pulses being preserved. We demonstrate the use of this setup as a simple autocorrelator and discuss a possible application to time-resolved vibrational spectroscopy.
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    Takeda, M.; Ina, H.; Kobayashi, S. Fourier-transform method of fringe-pattern analysis for computer-based topography and interferometry. J. Opt. Soc. Am. 1982, 72, 156,  DOI: 10.1364/JOSA.72.000156
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    Pelton, M.; Liu, M.; Park, S.; Scherer, N. F.; Guyot-Sionnest, P. Ultrafast resonant optical scattering from single gold nanorods: Large nonlinearities and plasmon saturation. Phys. Rev. B: Condens. Matter Mater. Phys. 2006, 73, 1– 6,  DOI: 10.1103/PhysRevB.73.155419
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    Baida, H.; Mongin, D.; Christofilos, D.; Bachelier, G.; Crut, A.; Maioli, P.; Del Fatti, N.; Vallee, F. Ultrafast nonlinear optical response of a single gold nanorod near its surface plasmon resonance. Phys. Rev. Lett. 2011, 107, 1– 5,  DOI: 10.1103/PhysRevLett.107.057402
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    Itoh, T.; Asahi, T.; Masuhara, H. Femtosecond light scattering spectroscopy of single gold nanoparticles. Appl. Phys. Lett. 2001, 79, 1667– 1669,  DOI: 10.1063/1.1402962
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    Femtosecond light scattering spectroscopy of single gold nanoparticles
    Itoh, Tamitake; Asahi, Tsuyoshi; Masuhara, Hiroshi
    Applied Physics Letters (2001), 79 (11), 1667-1669CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
    The authors have developed an ultrafast, light-scattering spectroscopic system combining a conventional microscope with a pump-probe setup. The surface plasmon resonance band for an individual gold particles with a mean radius of 40 nm was measured. The results on the pump-probe expt. demonstrate that both the electron-phonon and the phonon-phonon coupling processes in the individual gold particles take place with the lifetimes of 4 ps and >25 ps, resp.
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    Piatkowski, L.; Gellings, E.; van Hulst, N. F. Broadband single-molecule excitation spectroscopy. Nat. Commun. 2016, 7, 10411,  DOI: 10.1038/ncomms10411
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    Broadband single-molecule excitation spectroscopy
    Piatkowski, Lukasz; Gellings, Esther; van Hulst, Niek F.
    Nature Communications (2016), 7 (), 10411CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
    Over the past 25 years, single-mol. spectroscopy has developed into a widely used tool in multiple disciplines of science. The diversity of routinely recorded emission spectra does underpin the strength of the single-mol. approach in resolving the heterogeneity and dynamics, otherwise hidden in the ensemble. In early cryogenic studies single mols. were identified by their distinct excitation spectra, yet measuring excitation spectra at room temp. remains challenging. Here we present a broadband Fourier approach that allows rapid recording of excitation spectra of individual mols. under ambient conditions and that is robust against blinking and bleaching. Applying the method we show that the excitation spectra of individual mols. exhibit an extreme distribution of solvatochromic shifts and distinct spectral shapes. Importantly, we demonstrate that the sensitivity and speed of the broadband technique is comparable to that of emission spectroscopy putting both techniques side-by-side in single-mol. spectroscopy.
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    Voisin, C.; Del Fatti, N.; Christofilos, D.; Vallee, F. Ultrafast electron dynamics and optical nonlinearities in metal nanoparticles. J. Phys. Chem. B 2001, 105, 2264– 2280,  DOI: 10.1021/jp0038153
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    Ultrafast Electron Dynamics and Optical Nonlinearities in Metal Nanoparticles
    Voisin, Christophe; Del Fatti, Natalia; Christofilos, Dimitris; Vallee, Fabrice
    Journal of Physical Chemistry B (2001), 105 (12), 2264-2280CODEN: JPCBFK; ISSN:1089-5647. (American Chemical Society)
    The femtosecond optical response of noble metal nanoparticles and its connection to the ultrafast electron dynamics are discussed in light of the results of high-sensitivity femtosecond pump-probe expts. The phys. origins of the nonlinear responses in the vicinity of the surface plasmon resonance and interband transition threshold are analyzed using extension of the theor. models used in the bulk materials. These responses contain information on the electron interaction processes (electron-electron and electron-phonon scattering) that can thus be directly studied in the time domain. Their size and environment dependences are discussed, and the results are compared to the ones in the bulk materials. Time-resolved techniques also permit direct study of the vibrational modes of metal nanoparticles and, in particular, the detn. of their damping, which is a sensitive probe of the nature of the surrounding matrix and of the interface quality. A review with 153 refs.
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    Hodak, J. H.; Henglein, A.; Hartland, G. V. Photophysics of nanometer sized metal particles: Electron-phonon coupling and coherent excitation of breathing vibrational modes. J. Phys. Chem. B 2000, 104, 9954– 9965,  DOI: 10.1021/jp002256x
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    Photophysics of Nanometer Sized Metal Particles: Electron-Phonon Coupling and Coherent Excitation of Breathing Vibrational Modes
    Hodak, Jose H.; Henglein, Arnim; Hartland, Gregory V.
    Journal of Physical Chemistry B (2000), 104 (43), 9954-9965CODEN: JPCBFK; ISSN:1089-5647. (American Chemical Society)
    The wide variety of applications of metal nanoparticles has motivated many studies of their properties. Some important practical issues are how the size, compn. and structure of these materials affect their catalytic and optical properties. The authors review with 84 refs. the authors' recent work on the photophysics of metal nanoparticles. The systems that were studied include Au particles with sizes ranging from 2 nm diam. (several hundred atoms) to 120 nm diam., and bimetallic core-shell particles composed of Au, Ag, Pt and/or Pb. These particles, which have a rather narrow size distribution, were prepd. by radiolytic techniques. By performing time-resolved laser measurements the authors were able to study the coupling between the electrons and phonons in the particles, and their low frequency breathing modes. These expts. show that for Au the time scale for electron-phonon coupling does not depend on size, in contrast to metals such as Ga and Ag. However, the frequency of the acoustic breathing modes strongly depends on the size of the particles, as well as their compn. These modes are impulsively excited by the rapid lattice heating that accompanies ultrafast laser excitation. The subsequent coherent nuclear motion modulates the transmitted probe laser intensity, giving a beat signal in the authors' expts. Unlike quantum-beats in mols. or semiconductors, this signal can be completely understood by classical mechanics.
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    Link, S.; El-Sayed, M. A. Optical Properties and Ultrafast Dynamics of Metallic Nanocrystals. Annu. Rev. Phys. Chem. 2003, 54, 331– 366,  DOI: 10.1146/annurev.physchem.54.011002.103759
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    Optical properties and ultrafast dynamics of metallic nanocrystals
    Link, Stephan; El-Sayed, Mostafa A.
    Annual Review of Physical Chemistry (2003), 54 (), 331-366CODEN: ARPLAP; ISSN:0066-426X. (Annual Reviews Inc.)
    A review. Noble metal particles have long fascinated scientists because of their intense color, which led to their application in stained glass windows as early as the Middle Ages. The recent resurrection of colloidal and cluster chem. has brought about the strive for new materials that allow a bottoms-up approach of building improved and new devices with nanoparticles or artificial atoms. In this review, the authors discuss some of the properties of individual and some assembled metallic nanoparticles with a focus on their interaction with continuous-wave and pulsed laser light of different energies. The potential application of the plasmon resonance as sensors is discussed.
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    Baffou, G.; Quidant, R. Thermo-plasmonics: Using metallic nanostructures as nano-sources of heat. Laser Photonics Rev. 2013, 7, 171– 187,  DOI: 10.1002/lpor.201200003
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    Thermo-plasmonics: using metallic nanostructures as nano-sources of heat
    Baffou, Guillaume; Quidant, Romain
    Laser & Photonics Reviews (2013), 7 (2), 171-187CODEN: LPRAB8; ISSN:1863-8880. (Wiley-VCH Verlag GmbH & Co. KGaA)
    A review. Recent years have seen a growing interest in using metal nanostructures to control temp. on the nanoscale. Under illumination at its plasmonic resonance, a metal nanoparticle features enhanced light absorption, turning it into an ideal nano-source of heat, remotely controllable using light. Such a powerful and flexible photothermal scheme is the basis of thermo-plasmonics. Here, the recent progress of this emerging and fast-growing field is reviewed. First, the physics of heat generation in metal nanoparticles is described, under both continuous and pulsed illumination. The second part is dedicated to numerical and exptl. methods that have been developed to further understand and engineer plasmonic-assisted heating processes on the nanoscale. Finally, some of the most recent applications based on the heat generated by gold nanoparticles are surveyed, namely photothermal cancer therapy, nano-surgery, drug delivery, photothermal imaging, protein tracking, photoacoustic imaging, nano-chem. and optofluidics.
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    Memmolo, P. Recent advances in holographic 3D particle tracking. Adv. Opt. Photonics 2015, 7, 713– 755,  DOI: 10.1364/AOP.7.000713
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    Poon, T.-C.; Liu, J.-P. Introduction to Modern Digital Holography with MATLAB; Cambridge University Press: Cambridge, U.K., 2014.
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    Latychevskaia, T.; Fink, H.-W. Holographic time-resolved particle tracking by means of three-dimensional volumetric deconvolution. Opt. Express 2014, 22, 20994– 21003,  DOI: 10.1364/OE.22.020994
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    Latychevskaia, Tatiana; Fink, Hans-Werner
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  • Abstract

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    Figure 1

    Figure 1. UHT microscope: an all-optical lock-in camera. (a) Experimental implementation of UHT microscopy with transient pump-delayed-probe imaging, and interference with modulated reference beams, allowing all-optical lock-in wide-field imaging on a camera. SHG, second harmonic generation; NOPA, noncollinear optical parametric amplifier. (b) Chopping scheme employed, 1/f = 1 ms is the time between individual laser pulses with f being the repetition rate of the laser system. (c) Data-processing workflow allowing retrieval of the scattering images for the pumped and unpumped sample by Fourier filtering in k-space. (d) Fluctuations of the radius of the pumpOFF (blue) and pumpON (pink) interference signals, recorded at 10 frames-per-second (FPS), alongside their ratio (black, dashed). (e) Relative pumpOFF/pumpON signal fluctuations recorded at 100 FPS (pink) and 10 FPS (purple) compared to shot-noise distributions (blue dashed lines) exhibiting 104 and 105 photons, respectively.

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    Figure 2

    Figure 2. Wide-field transient imaging of single nanoparticles. (a) PumpOFF image of individual 100 nm Au-NPs. (b) Time-delay dependent scattering signal magnitudes at a probe wavelength of 540 nm for the five individual particles encircled in (a) recorded in the presence (pink) and absence (blue) of the 400 nm pump pulse with a fluence of 1.1 mJ/cm2. (c) Transient images within the dashed-rectangle in (a) for three different probe wavelengths as a function of pump–probe delay. From 540 to 500 nm, the NP transient-contrast inverts from negative to positive; note the black circles highlighting some NPs with signal-scaling that are considerably different from the average behavior (see Supporting Information for transient images of the entire field-of-view).

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    Figure 3

    Figure 3. UHT imaging of single nanoparticle spectro-temporal dynamics. (a) Spectrally resolved transient dynamics of 76 individual 100 nm Au NPs (colored) alongside the mean dynamics (black). The transients are offset for clarity with the dashed line indicating ΔS/S(t) = 0 for the individual wavelengths. The wavelength dependent probe fluences are adjusted within the 0.1–0.4 mJ/cm2 range and the pump fluence is 1.1 mJ/cm2 (at 1/e). (b) Temporal representation of the decay dynamics of the averaged transient scattering spectra. (c) Histogram representation of the ΔS/S(t) signal obtained by analyzing each individual NP in the 100–900 fs temporal window.

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    Figure 4

    Figure 4. Signal scaling for different particle sizes. (a) Holographic (left) and transient scattering images (right) recorded for NP-diameters ranging from 100 to 20 nm using a 400 nm pump and a 540 nm probe pulse (see Methods for fluences). Circles indicate NPs, diamonds indicate a representative background region. (b) Time-traces of the particles highlighted in (a); the scale-bar indicates the relative scattering signal normalized to both pump intensity and probe amplitude. Blue lines indicate signals obtained at a background region and pink lines indicate signals due to NPs.

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    Figure 5

    Figure 5. Digital refocusing of out-of-focus nanoparticles. (a) Scattering amplitude and phase of 100 nm Au NPs imaged below (left), above (center) and approximately in (right) the focal plane. (b) Representative images of the digitally refocused particles. (c) Transient wide-field-dynamics for the as-recorded, −1860 nm out-of-focus, image (top) as well as the refocused image obtained by computational back-propagation into focus (bottom).

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      Guo, Zhi; Wan, Yan; Yang, Mengjin; Snaider, Jordan; Zhu, Kai; Huang, Libai
      Science (Washington, DC, United States) (2017), 356 (6333), 59-62CODEN: SCIEAS; ISSN:0036-8075. (American Association for the Advancement of Science)
      The Shockley-Queisser limit for solar cell efficiency can be overcome if hot carriers can be harvested before they thermalize. Recently, carrier cooling time up to 100 ps was obsd. in hybrid perovskites, but it is unclear whether these long-lived hot carriers can migrate long distance for efficient collection. The authors report direct visualization of hot-carrier migration in methylammonium lead iodide (CH3NH3PbI3) thin films by ultrafast transient absorption microscopy, demonstrating three distinct transport regimes. Quasiballistic transport was obsd. to correlate with excess kinetic energy, resulting in up to 230 nm transport distance that could overcome grain boundaries. The nonequil. transport persisted over tens of picoseconds and ∼600 nm before reaching the diffusive transport limit. These results suggest potential applications of hot-carrier devices based on hybrid perovskites.
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    9. 9
      Delor, M.; Weaver, H. L.; Yu, Q. Q.; Ginsberg, N. S. Imaging material functionality through three-dimensional nanoscale tracking of energy flow. Nat. Mater. 2020, 19, 56– 62,  DOI: 10.1038/s41563-019-0498-x
      9
      Imaging material functionality through three-dimensional nanoscale tracking of energy flow
      Delor, Milan; Weaver, Hannah L.; Yu, QinQin; Ginsberg, Naomi S.
      Nature Materials (2020), 19 (1), 56-62CODEN: NMAACR; ISSN:1476-1122. (Nature Research)
      The ability of energy carriers to move between atoms and mols. underlies biochem. and material function. Understanding and controlling energy flow, however, requires observing it on ultrasmall and ultrafast spatio-temporal scales, where energetic and structural roadblocks dictate the fate of energy carriers. Here, we developed a non-invasive optical scheme that leverages non-resonant interferometric scattering to track tiny changes in material polarizability created by energy carriers. We thus map evolving energy carrier distributions in four dimensions of spacetime with few-nanometer lateral precision and directly correlate them with material morphol. We visualize exciton, charge and heat transport in polyacene, silicon and perovskite semiconductors and elucidate how disorder affects energy flow in three dimensions. For example, we show that morphol. boundaries in polycryst. metal halide perovskites possess lateral- and depth-dependent resistivities, blocking lateral transport for surface but not bulk carriers. We also reveal strategies for interpreting energy transport in disordered environments that will direct the design of defect-tolerant materials for the semiconductor industry of tomorrow.
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    10. 10
      Shaltout, A. M.; Shalaev, V. M.; Brongersma, M. L. Spatiotemporal light control with active metasurfaces. Science (Washington, DC, U. S.) 2019, 364, eaat3100
      There is no corresponding record for this reference.
    11. 11
      Chikkaraddy, R. Single-molecule strong coupling at room temperature in plasmonic nanocavities. Nature 2016, 535, 127– 130,  DOI: 10.1038/nature17974
      11
      Single-molecule strong coupling at room temperature in plasmonic nanocavities
      Chikkaraddy, Rohit; de Nijs, Bart; Benz, Felix; Barrow, Steven J.; Scherman, Oren A.; Rosta, Edina; Demetriadou, Angela; Fox, Peter; Hess, Ortwin; Baumberg, Jeremy J.
      Nature (London, United Kingdom) (2016), 535 (7610), 127-130CODEN: NATUAS; ISSN:0028-0836. (Nature Publishing Group)
      Photon emitters placed in an optical cavity experience an environment that changes how they are coupled to the surrounding light field. In the weak-coupling regime, the extn. of light from the emitter is enhanced. But more profound effects emerge when single-emitter strong coupling occurs: mixed states are produced that are part light, part matter, forming building blocks for quantum information systems and for ultralow-power switches and lasers. Such cavity quantum electrodynamics has until now been the preserve of low temps. and complicated fabrication methods, compromising its use. Here, by scaling the cavity vol. to less than 40 cubic nanometers and using host-guest chem. to align one to ten protectively isolated methylene-blue mols., we reach the strong-coupling regime at room temp. and in ambient conditions. Dispersion curves from more than 50 such plasmonic nanocavities display characteristic light-matter mixing, with Rabi frequencies of 300 millielectronvolts for ten methylene-blue mols., decreasing to 90 millielectronvolts for single mols.-matching quant. models. Statistical anal. of vibrational spectroscopy time series and dark-field scattering spectra provides evidence of single-mol. strong coupling. This dressing of mols. with light can modify photochem., opening up the exploration of complex natural processes such as photosynthesis and the possibility of manipulating chem. bonds.
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    12. 12
      Ginsberg, N. S.; Tisdale, W. A. Spatially resolved photogenerated exciton and charge transport in emerging semiconductors. Annu. Rev. Phys. Chem. 2020, 71, 1– 30,  DOI: 10.1146/annurev-physchem-052516-050703
      12
      Spatially Resolved Photogenerated Exciton and Charge Transport in Emerging Semiconductors
      Ginsberg, Naomi S.; Tisdale, William A.
      Annual Review of Physical Chemistry (2020), 71 (), 1-30CODEN: ARPLAP; ISSN:0066-426X. (Annual Reviews)
      A review. We review recent advances in the characterization of electronic forms of energy transport in emerging semiconductors. The approaches described all temporally and spatially resolve the evolution of initially localized populations of photogenerated excitons or charge carriers. We first provide a comprehensive background for describing the phys. origin and nature of electronic energy transport both microscopically and from the perspective of the observer. We introduce the new family of far-field, time-resolved optical microscopies developed to directly resolve not only the extent of this transport but also its potentially temporally and spatially dependent rate. We review a representation of examples from the recent literature, including investigation of energy flow in colloidal quantum dot solids, org. semiconductors, org.-inorg. metal halide perovskites, and 2D transition metal dichalcogenides. These examples illustrate how traditional parameters like diffusivity are applicable only within limited spatiotemporal ranges and how the techniques at the core of this review,esp. when taken together, are revealing a more complete picture of the spatiotemporal evolution of energy transport in complex semiconductors, even as a function of their structural heterogeneities.
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    13. 13
      Lim, E.-K. Nanomaterials for Theranostics: Recent Advances and Future Challenges. Chem. Rev. 2015, 115, 327– 394,  DOI: 10.1021/cr300213b
      13
      Nanomaterials for Theranostics: Recent Advances and Future Challenges
      Lim, Eun-Kyung; Kim, Taekhoon; Paik, Soonmyung; Haam, Seungjoo; Huh, Yong-Min; Lee, Kwangyeol
      Chemical Reviews (Washington, DC, United States) (2015), 115 (1), 327-394CODEN: CHREAY; ISSN:0009-2665. (American Chemical Society)
      There is no expanded citation for this reference.
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    14. 14
      Kühn, J. Real-time dual-wavelength digital holographic microscopy with a single hologram acquisition. Opt. Express 2007, 15, 7231– 7242,  DOI: 10.1364/OE.15.007231
      There is no corresponding record for this reference.
    15. 15
      Colomb, T. Polarization microscopy by use of digital holography: Application to optical-fiber birefringence measurements. Appl. Opt. 2005, 44, 4461– 4469,  DOI: 10.1364/AO.44.004461
      15
      Polarization microscopy by use of digital holography: application to optical-fiber birefringence measurements
      Colomb Tristan; Durr Florian; Cuche Etienne; Marquet Pierre; Limberger Hans G; Salathe Rene-Paul; Depeursinge Christian
      Applied optics (2005), 44 (21), 4461-9 ISSN:1559-128X.
      We present a digital holographic microscope that permits one to image polarization state. This technique results from the coupling of digital holographic microscopy and polarization digital holography. The interference between two orthogonally polarized reference waves and the wave transmitted by a microscopic sample, magnified by a microscope objective, is recorded on a CCD camera. The off-axis geometry permits one to reconstruct separately from this single hologram two wavefronts that are used to image the object-wave Jones vector. We applied this technique to image the birefringence of a bent fiber. To evaluate the precision of the phase-difference measurement, the birefringence induced by internal stress in an optical fiber is measured and compared to the birefringence profile captured by a standard method, which had been developed to obtain high-resolution birefringence profiles of optical fibers.
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    16. 16
      Rubin, M.; Dardikman, G.; Mirsky, S. K.; Turko, N. A.; Shaked, N. T. Six-pack off-axis holography. Opt. Lett. 2017, 42, 4611– 4614,  DOI: 10.1364/OL.42.004611
      16
      Six-pack off-axis holography
      Rubin Moran; Dardikman Gili; Mirsky Simcha K; Turko Nir A; Shaked Natan T
      Optics letters (2017), 42 (22), 4611-4614 ISSN:.
      We present a new holographic concept, named six-pack holography (6PH), in which we compress six off-axis holograms into a single multiplexed off-axis hologram without loss of magnification or resolution. The multiplexed hologram contains straight off-axis fringes with six different orientations, and can be generated optically or digitally. We show that since the six different complex wavefronts do not overlap in the spatial frequency domain, they can be fully reconstructed. 6PH allows more than 50% improvement in the spatial bandwidth consumption when compared to the best multiplexing method proposed so far. We expect the 6PH concept to be useful for a variety of applications, such as field-of-view multiplexing, wavelength multiplexing, temporal multiplexing, multiplexing for super-resolution imaging, and others.
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    17. 17
      Schnedermann, C. Sub-10 fs Time-Resolved Vibronic Optical Microscopy. J. Phys. Chem. Lett. 2016, 7, 4854– 4859,  DOI: 10.1021/acs.jpclett.6b02387
      17
      Sub-10 fs Time-Resolved Vibronic Optical Microscopy
      Schnedermann, Christoph; Lim, Jong Min; Wende, Torsten; Duarte, Alex S.; Ni, Limeng; Gu, Qifei; Sadhanala, Aditya; Rao, Akshay; Kukura, Philipp
      Journal of Physical Chemistry Letters (2016), 7 (23), 4854-4859CODEN: JPCLCD; ISSN:1948-7185. (American Chemical Society)
      Fmtosecond wide-field transient absorption microscopy combining sub-10 fs pump and probe pulses covering the complete visible (500-650 nm) and near-IR (650-950 nm) spectrum with diffraction-limited optical resoln. is introduced. The capabilities of the system were demonstrated by reporting the spatially- and spectrally-resolved transient electronic response of MAPbI3-xClx perovskite films and reveal significant quenching of the transient bleach signal at grain boundaries. The unprecedented temporal resoln. enables one to directly observe the formation of band-gap renormalization, completed in 25 fs after photoexcitation. The authors acquire hyperspectral Raman maps of TIPS pentacene films with sub-400 nm spatial and sub-15 cm-1 spectral resoln. covering the 100-2000 cm-1 window. The approach opens up the possibility of studying ultrafast dynamics on nanometer length and femtosecond time scales in a variety of 2-dimensional and nanoscopic systems.
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    18. 18
      Bon, P.; Maucort, G.; Wattellier, B.; Monneret, S. Quadriwave lateral shearing interferometry for quantitative phase microscopy of living cells. Opt. Express 2009, 17, 13080– 13094,  DOI: 10.1364/OE.17.013080
      18
      Quadriwave lateral shearing interferometry for quantitative phase microscopy of living cells
      Bon, Pierre; Maucort, Guillaume; Wattellier, Benoit; Monneret, Serge
      Optics Express (2009), 17 (15), 13080-13094CODEN: OPEXFF; ISSN:1094-4087. (Optical Society of America)
      Phase imaging with a high-resoln. wavefront sensor is considered. This is based on a quadriwave lateral shearing interferometer mounted on a non-modified transmission white-light microscope. The measurement technol. is explained both in the scope of wave optics and geometrical optics in order to discuss its implementation on a conventional microscope. In particular we consider the effect of a non spatially coherent source on the phase-image signal-to-noise ratio. Precise measurements of the phase-shift introduced by microscopic beads or giant unilamellar vesicles validate the principle and show the accuracy of the methods. Diffraction limited images of living COS-7 cells are then presented, with a particular focus on the membrane and organelle dynamics.
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    19. 19
      Maznev, A. A.; Crimmins, T. F.; Nelson, K. A. How to make femtosecond pulses overlap. Opt. Lett. 1998, 23, 1378– 1380,  DOI: 10.1364/OL.23.001378
      19
      How to make femtosecond pulses overlap
      Maznev A A; Crimmins T F; Nelson K A
      Optics letters (1998), 23 (17), 1378-80 ISSN:0146-9592.
      Normally, femtosecond light pulses that cross at a nonzero angle overlap over only a small region in space. This limitation can be overcome by the use of diffraction orders of a grating. We consider an arrangement in which, on diffraction of a femtosecond pulse by a grating, two beams that correspond to the first-order diffraction maxima are recombined at the image plane by a system of two confocal lenses. In this arrangement the beams overlap over the their full aperture, with the short duration of the pulses being preserved. We demonstrate the use of this setup as a simple autocorrelator and discuss a possible application to time-resolved vibrational spectroscopy.
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    20. 20
      Takeda, M.; Ina, H.; Kobayashi, S. Fourier-transform method of fringe-pattern analysis for computer-based topography and interferometry. J. Opt. Soc. Am. 1982, 72, 156,  DOI: 10.1364/JOSA.72.000156
      There is no corresponding record for this reference.
    21. 21
      Goodman, J. W. Introduction to Fourier optics; W.H. Freeman & Co Ltd: New York, 2005.
      There is no corresponding record for this reference.
    22. 22
      Pelton, M.; Liu, M.; Park, S.; Scherer, N. F.; Guyot-Sionnest, P. Ultrafast resonant optical scattering from single gold nanorods: Large nonlinearities and plasmon saturation. Phys. Rev. B: Condens. Matter Mater. Phys. 2006, 73, 1– 6,  DOI: 10.1103/PhysRevB.73.155419
      There is no corresponding record for this reference.
    23. 23
      Baida, H.; Mongin, D.; Christofilos, D.; Bachelier, G.; Crut, A.; Maioli, P.; Del Fatti, N.; Vallee, F. Ultrafast nonlinear optical response of a single gold nanorod near its surface plasmon resonance. Phys. Rev. Lett. 2011, 107, 1– 5,  DOI: 10.1103/PhysRevLett.107.057402
      There is no corresponding record for this reference.
    24. 24
      Itoh, T.; Asahi, T.; Masuhara, H. Femtosecond light scattering spectroscopy of single gold nanoparticles. Appl. Phys. Lett. 2001, 79, 1667– 1669,  DOI: 10.1063/1.1402962
      24
      Femtosecond light scattering spectroscopy of single gold nanoparticles
      Itoh, Tamitake; Asahi, Tsuyoshi; Masuhara, Hiroshi
      Applied Physics Letters (2001), 79 (11), 1667-1669CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
      The authors have developed an ultrafast, light-scattering spectroscopic system combining a conventional microscope with a pump-probe setup. The surface plasmon resonance band for an individual gold particles with a mean radius of 40 nm was measured. The results on the pump-probe expt. demonstrate that both the electron-phonon and the phonon-phonon coupling processes in the individual gold particles take place with the lifetimes of 4 ps and >25 ps, resp.
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    25. 25
      Piatkowski, L.; Gellings, E.; van Hulst, N. F. Broadband single-molecule excitation spectroscopy. Nat. Commun. 2016, 7, 10411,  DOI: 10.1038/ncomms10411
      25
      Broadband single-molecule excitation spectroscopy
      Piatkowski, Lukasz; Gellings, Esther; van Hulst, Niek F.
      Nature Communications (2016), 7 (), 10411CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
      Over the past 25 years, single-mol. spectroscopy has developed into a widely used tool in multiple disciplines of science. The diversity of routinely recorded emission spectra does underpin the strength of the single-mol. approach in resolving the heterogeneity and dynamics, otherwise hidden in the ensemble. In early cryogenic studies single mols. were identified by their distinct excitation spectra, yet measuring excitation spectra at room temp. remains challenging. Here we present a broadband Fourier approach that allows rapid recording of excitation spectra of individual mols. under ambient conditions and that is robust against blinking and bleaching. Applying the method we show that the excitation spectra of individual mols. exhibit an extreme distribution of solvatochromic shifts and distinct spectral shapes. Importantly, we demonstrate that the sensitivity and speed of the broadband technique is comparable to that of emission spectroscopy putting both techniques side-by-side in single-mol. spectroscopy.
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    26. 26
      Voisin, C.; Del Fatti, N.; Christofilos, D.; Vallee, F. Ultrafast electron dynamics and optical nonlinearities in metal nanoparticles. J. Phys. Chem. B 2001, 105, 2264– 2280,  DOI: 10.1021/jp0038153
      26
      Ultrafast Electron Dynamics and Optical Nonlinearities in Metal Nanoparticles
      Voisin, Christophe; Del Fatti, Natalia; Christofilos, Dimitris; Vallee, Fabrice
      Journal of Physical Chemistry B (2001), 105 (12), 2264-2280CODEN: JPCBFK; ISSN:1089-5647. (American Chemical Society)
      The femtosecond optical response of noble metal nanoparticles and its connection to the ultrafast electron dynamics are discussed in light of the results of high-sensitivity femtosecond pump-probe expts. The phys. origins of the nonlinear responses in the vicinity of the surface plasmon resonance and interband transition threshold are analyzed using extension of the theor. models used in the bulk materials. These responses contain information on the electron interaction processes (electron-electron and electron-phonon scattering) that can thus be directly studied in the time domain. Their size and environment dependences are discussed, and the results are compared to the ones in the bulk materials. Time-resolved techniques also permit direct study of the vibrational modes of metal nanoparticles and, in particular, the detn. of their damping, which is a sensitive probe of the nature of the surrounding matrix and of the interface quality. A review with 153 refs.
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    27. 27
      Hodak, J. H.; Henglein, A.; Hartland, G. V. Photophysics of nanometer sized metal particles: Electron-phonon coupling and coherent excitation of breathing vibrational modes. J. Phys. Chem. B 2000, 104, 9954– 9965,  DOI: 10.1021/jp002256x
      27
      Photophysics of Nanometer Sized Metal Particles: Electron-Phonon Coupling and Coherent Excitation of Breathing Vibrational Modes
      Hodak, Jose H.; Henglein, Arnim; Hartland, Gregory V.
      Journal of Physical Chemistry B (2000), 104 (43), 9954-9965CODEN: JPCBFK; ISSN:1089-5647. (American Chemical Society)
      The wide variety of applications of metal nanoparticles has motivated many studies of their properties. Some important practical issues are how the size, compn. and structure of these materials affect their catalytic and optical properties. The authors review with 84 refs. the authors' recent work on the photophysics of metal nanoparticles. The systems that were studied include Au particles with sizes ranging from 2 nm diam. (several hundred atoms) to 120 nm diam., and bimetallic core-shell particles composed of Au, Ag, Pt and/or Pb. These particles, which have a rather narrow size distribution, were prepd. by radiolytic techniques. By performing time-resolved laser measurements the authors were able to study the coupling between the electrons and phonons in the particles, and their low frequency breathing modes. These expts. show that for Au the time scale for electron-phonon coupling does not depend on size, in contrast to metals such as Ga and Ag. However, the frequency of the acoustic breathing modes strongly depends on the size of the particles, as well as their compn. These modes are impulsively excited by the rapid lattice heating that accompanies ultrafast laser excitation. The subsequent coherent nuclear motion modulates the transmitted probe laser intensity, giving a beat signal in the authors' expts. Unlike quantum-beats in mols. or semiconductors, this signal can be completely understood by classical mechanics.
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    28. 28
      Link, S.; El-Sayed, M. A. Optical Properties and Ultrafast Dynamics of Metallic Nanocrystals. Annu. Rev. Phys. Chem. 2003, 54, 331– 366,  DOI: 10.1146/annurev.physchem.54.011002.103759
      28
      Optical properties and ultrafast dynamics of metallic nanocrystals
      Link, Stephan; El-Sayed, Mostafa A.
      Annual Review of Physical Chemistry (2003), 54 (), 331-366CODEN: ARPLAP; ISSN:0066-426X. (Annual Reviews Inc.)
      A review. Noble metal particles have long fascinated scientists because of their intense color, which led to their application in stained glass windows as early as the Middle Ages. The recent resurrection of colloidal and cluster chem. has brought about the strive for new materials that allow a bottoms-up approach of building improved and new devices with nanoparticles or artificial atoms. In this review, the authors discuss some of the properties of individual and some assembled metallic nanoparticles with a focus on their interaction with continuous-wave and pulsed laser light of different energies. The potential application of the plasmon resonance as sensors is discussed.
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    29. 29
      Baffou, G.; Quidant, R. Thermo-plasmonics: Using metallic nanostructures as nano-sources of heat. Laser Photonics Rev. 2013, 7, 171– 187,  DOI: 10.1002/lpor.201200003
      29
      Thermo-plasmonics: using metallic nanostructures as nano-sources of heat
      Baffou, Guillaume; Quidant, Romain
      Laser & Photonics Reviews (2013), 7 (2), 171-187CODEN: LPRAB8; ISSN:1863-8880. (Wiley-VCH Verlag GmbH & Co. KGaA)
      A review. Recent years have seen a growing interest in using metal nanostructures to control temp. on the nanoscale. Under illumination at its plasmonic resonance, a metal nanoparticle features enhanced light absorption, turning it into an ideal nano-source of heat, remotely controllable using light. Such a powerful and flexible photothermal scheme is the basis of thermo-plasmonics. Here, the recent progress of this emerging and fast-growing field is reviewed. First, the physics of heat generation in metal nanoparticles is described, under both continuous and pulsed illumination. The second part is dedicated to numerical and exptl. methods that have been developed to further understand and engineer plasmonic-assisted heating processes on the nanoscale. Finally, some of the most recent applications based on the heat generated by gold nanoparticles are surveyed, namely photothermal cancer therapy, nano-surgery, drug delivery, photothermal imaging, protein tracking, photoacoustic imaging, nano-chem. and optofluidics.
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    30. 30
      Memmolo, P. Recent advances in holographic 3D particle tracking. Adv. Opt. Photonics 2015, 7, 713– 755,  DOI: 10.1364/AOP.7.000713
      There is no corresponding record for this reference.
    31. 31
      Poon, T.-C.; Liu, J.-P. Introduction to Modern Digital Holography with MATLAB; Cambridge University Press: Cambridge, U.K., 2014.
      There is no corresponding record for this reference.
    32. 32
      Latychevskaia, T.; Fink, H.-W. Holographic time-resolved particle tracking by means of three-dimensional volumetric deconvolution. Opt. Express 2014, 22, 20994– 21003,  DOI: 10.1364/OE.22.020994
      32
      Holographic time-resolved particle tracking by means of three-dimensional volumetric deconvolution
      Latychevskaia, Tatiana; Fink, Hans-Werner
      Optics Express (2014), 22 (17), 20994-21003, 10 pp.CODEN: OPEXFF; ISSN:1094-4087. (Optical Society of America)
      Holog. particle image velocimetry allows tracking particle trajectories in time and space by means of holog. However, the drawback of the technique is that in the three-dimensional particle distribution reconstructed from a hologram, the individual particles can hardly be resolved due to the superimposed out-of-focus signal from neighboring particles. We demonstrate here a three-dimensional volumetric deconvolution applied to the reconstructed wavefront which results in resolving all particles simultaneously in three-dimensions. Moreover, we apply the three-dimensional volumetric deconvolution to reconstructions of a time-dependent sequence of holograms of an ensemble of polystyrene spheres moving in water. From each hologram we simultaneously resolve all particles in the ensemble in three dimensions and from the sequence of holograms we obtain the time-resolved trajectories of individual polystyrene spheres.
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    33. 33
      Pache, C. Fast three-dimensional imaging of gold nanoparticles in living cells with photothermal optical lock-in Optical Coherence Microscopy. Opt. Express 2012, 20, 21385,  DOI: 10.1364/OE.20.021385
      33
      Fast three-dimensional imaging of gold nanoparticles in living cells with photothermal optical lock-in Optical Coherence Microscopy
      Pache, Christophe; Bocchio, Noelia L.; Bouwens, Arno; Villiger, Martin; Berclaz, Corinne; Goulley, Joan; Gibson, Matthew I.; Santschi, Christian; Lasser, Theo
      Optics Express (2012), 20 (19), 21385-21399CODEN: OPEXFF; ISSN:1094-4087. (Optical Society of America)
      We introduce photothermal optical lock-in Optical Coherence Microscopy (poli-OCM), a volumetric imaging technique, which combines the depth sectioning of OCM with the high sensitivity of photothermal microscopy while maintaining the fast acquisition speed inherent to OCM. We report on the detection of single 40 nm gold particles with a 0.5 μm lateral and 2 μm axial resoln. over a 50 μm depth of field and the three-dimensional localization of gold colloids within living cells. In combination with intrinsic sample contrast measured with dark-field OCM, poli-OCM offers a versatile platform for functional cell imaging.
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    34. 34
      Lasne, D. Single Nanoparticle Photothermal Tracking (SNaPT) of 5-nm gold beads in live cells. Biophys. J. 2006, 91, 4598– 4604,  DOI: 10.1529/biophysj.106.089771
      34
      Single nanoparticle photothermal tracking (SNaPT) of 5-nm gold beads in live cells
      Lasne, David; Blab, Gerhard A.; Berciaud, Stephane; Heine, Martin; Groc, Laurent; Choquet, Daniel; Cognet, Laurent; Lounis, Brahim
      Biophysical Journal (2006), 91 (12), 4598-4604CODEN: BIOJAU; ISSN:0006-3495. (Biophysical Society)
      Tracking individual nano-objects in live cells during arbitrary long times is a ubiquitous need in modern biol. The authors present here a method for tracking individual 5-nm gold nanoparticles on live cells. It relies on the photothermal effect and the detection of the Laser Induced Scattering around a NanoAbsorber (LISNA). The key point for recording trajectories at video rate is the use of a triangulation procedure. The effectiveness of the method is tested against single fluorescent mol. tracking in live COS7 cells on subsecond timescales. The authors further demonstrate recordings for several minutes of AMPA receptors trajectories on the plasma membrane of live neurons. Single Nanoparticle Photothermal Tracking has the unique potential to record arbitrary long trajectory of membrane proteins using nonfluorescent nanometer-sized labels.
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      https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BD28XhtlWgurfF&md5=6e812751882b89327f802d134e7dd08e
    35. 35
      Manzoni, C.; Polli, D.; Cerullo, G. Two-color pump-probe system broadly tunable over the visible and the near infrared with sub-30 fs temporal resolution. Rev. Sci. Instrum. 2006, 77, 023103,  DOI: 10.1063/1.2167128
      35
      Two-color pump-probe system broadly tunable over the visible and the near infrared with sub-30 fs temporal resolution
      Manzoni, Cristian; Polli, Dario; Cerullo, Giulio
      Review of Scientific Instruments (2006), 77 (2), 023103/1-023103/9CODEN: RSINAK; ISSN:0034-6748. (American Institute of Physics)
      An ultrafast spectroscopy system based on 2 synchronized noncollinear optical parametric amplifiers (NOPAs) is described. Each NOPA can be independently configured to generate ultrabroadband sub-10 fs visible pulses, tunable 15 fs visible pulses (500-720 nm), tunable 15-30 fs near-IR pulses (900-1500 nm), and 15-20 fs blue pulses (430-480 nm). This system enables to perform pump-probe expts. over nearly two octaves of spectrum with unprecedented temporal resoln. The authors present application examples highlighting the capability of this instrument to track excited-state dynamics occurring on the sub-100 fs time scale: electron transfer in polymer-fullerene blends, intersubband energy relaxation in C nanotubes, and internal conversion in carotenoids.
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    36. 36
      Ortiz-Orruño, U.; Jo, A.; Lee, H.; van Hulst, N. F.; Liebel, M. Precise nanosizing with high dynamic range holography. Nano Lett. 2021, 21, 317– 322,  DOI: 10.1021/acs.nanolett.0c03699
      36
      Precise Nanosizing with High Dynamic Range Holography
      Ortiz-Orruno, Unai; Jo, Ala; Lee, Hakho; van Hulst, Niek F.; Liebel, Matz
      Nano Letters (2021), 21 (1), 317-322CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
      Optical sensing is 1 of the key enablers of modern diagnostics. Esp. label-free imaging modalities hold great promise as they eliminate labeling procedures prior to anal. However, scattering signals of nanometric particles scale with their vol. square. This unfavorable scaling makes it extremely difficult to quant. characterize intrinsically heterogeneous clin. samples, such as extracellular vesicles, as their signal variation easily exceeds the dynamic range of currently available cameras. Here, the authors introduce off-axis k-space holog. that circumvents this limitation. By imaging the back-focal plane of microscope, the authors project the scattering signal of all particles onto all camera pixels, thus dramatically boosting the achievable dynamic range to up to 110 dB. The authors validate platform by detecting and quant. sizing metallic and dielec. particles over a 200 x 200μm field of view and demonstrate that independently performed signal calibrations allow correctly sizing particles made from different materials. Finally, the authors present quant. size distributions of extracellular vesicle samples.
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  • Supporting Information

    Supporting Information

    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.0c04416.

    • Expanded version of Figure 2, information regarding the data processing of the holograms, additional experiments performed on 200 nm Au NPs, pump-fluence dependent measurements as well as pump and probe spectra (PDF)


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