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SUPER Scheme in Action: Experimental Demonstration of Red-Detuned Excitation of a Quantum Emitter

  • Yusuf Karli
    Yusuf Karli
    Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
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    Orcidhttps://orcid.org/0000-0001-8987-828X
  • , 
  • Florian Kappe
    Florian Kappe
    Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
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  • Vikas Remesh*
    Vikas Remesh
    Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
    *Email: [email protected]
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  • , 
  • Thomas K. Bracht
    Thomas K. Bracht
    Institut für Festkörpertheorie, Universität Münster, Münster 48149, Germany
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  • , 
  • Julian Münzberg
    Julian Münzberg
    Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
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  • , 
  • Saimon Covre da Silva
    Saimon Covre da Silva
    Institute of Semiconductor and Solid State Physics, Johannes Kepler University Linz, Linz 4040, Austria
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  • Tim Seidelmann
    Tim Seidelmann
    Theoretische Physik III, Universität Bayreuth, Bayreuth 95440, Germany
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  • Vollrath Martin Axt
    Vollrath Martin Axt
    Theoretische Physik III, Universität Bayreuth, Bayreuth 95440, Germany
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  • Armando Rastelli
    Armando Rastelli
    Institute of Semiconductor and Solid State Physics, Johannes Kepler University Linz, Linz 4040, Austria
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  • Doris E. Reiter
    Doris E. Reiter
    Institut für Festkörpertheorie, Universität Münster, Münster 48149, Germany
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    Orcidhttps://orcid.org/0000-0002-3648-353X
  • , and 
  • Gregor Weihs
    Gregor Weihs
    Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
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Cite this: Nano Lett. 2022, 22, 16, 6567–6572
Publication Date (Web):July 6, 2022
https://doi.org/10.1021/acs.nanolett.2c01783

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Abstract

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The quest for the perfect single-photon source includes finding the optimal protocol for exciting the quantum emitter. Coherent optical excitation was, up until now, achieved by tuning the laser pulses to the transition frequency of the emitter, either directly or in average. Recently, it was theoretically discovered that an excitation with two red-detuned pulses is also possible where neither of which would yield a significant upper-level population individually. We show that the so-called swing-up of quantum emitter population (SUPER) scheme can be implemented experimentally with similar properties to existing schemes by precise amplitude shaping of a broadband pulse. Because of its truly off-resonant nature, this scheme has the prospect of powering high-purity photon sources with superior photon count rate.

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The future of photonic quantum technologies relies on bright, photostable, and on-demand sources of single and indistinguishable photons. To achieve the on-demand character, a deterministic state preparation of the excited state is required. The most prominent scheme for coherent optical control is the Rabi scheme, where a laser pulse tuned to the transition energy, called the π-pulse, inverts the quantum emitter population. As soon as the laser energy is detuned, the inversion fidelity drops drastically. (1) Consequently, all coherent excitation schemes to achieve a high population inversion either have a frequency component at (2−7) or are in average (8,9) resonant with the transition frequency of the quantum emitter. From this picture, a truly off-resonant excitation scheme is not desirable, even though these have the advantage of requiring only spectral filtering instead of challenging methods based on polarization filtering. Surprisingly, it was recently theoretically demonstrated that there exists a swing-up mechanism in the so-called Swing-UP of quantum EmitteR population (SUPER) scheme. (10) The SUPER scheme relies on the coherent coupling of two red-detuned lasers to coherently excite the emitter, while an individual pulse would not lead to any upper-level occupation. Up until now, this scheme existed only as a theoretical possibility. In this Letter, we show that the SUPER scheme works in a simple, yet elegant experiment to excite a quantum emitter, relying on amplitude-shaping of a broadband laser pulse.

As the quantum emitters, we choose semiconductor quantum dots because they have emerged as a promising platform for quantum communication devices with excellent performance characteristics. (11−20) Quantum dots benefit from their excellent photostability, nearly Fourier-limited emission line width and growth technologies that allow easy integration into nanoscale devices. (21−25)

Our results prove that the SUPER scheme is an efficient method to excite a quantum dot to its excited state with the same efficiency as the Rabi scheme. The off-resonant nature of this excitation bears the potential for a wide range of applications where a resonant excitation should be avoided, in particular for using quantum dots as photon sources.

We start by briefly summarizing the idea of the SUPER scheme. (10) We consider a quantum dot as a two-level system consisting of ground |g⟩ and exciton state |x⟩, separated by an energy ℏω0. This system is driven by a pulsed laser encoded in the time-dependent term Ω(t). Within the dipole and rotating wave approximations, the Hamiltonian for this system reads

(1)
The SUPER scheme requires two laser pulses that are both red-detuned (Δ1 and Δ2) from the exciton state by several millielectronvolts. In the following, we will always refer to the pulse with the smaller detuning as first pulse, that is, |Δ1| < |Δ2|. Considering a Gaussian-shaped excitation pulse, we define the generalized Rabi frequency as , where Ωi is the resonant Rabi frequency of either pulse given at the maximum of the pulse temporal envelope. In the SUPER scheme, one achieves a gradual rise in the exciton population by modulating the Rabi frequency, through the beating of the two detuned pulses. If the difference between the two detunings coincides with the Rabi frequency of the first pulse, that is,, implying the condition |Δ2| > 2|Δ1|, the SUPER mechanism results in a complete population inversion of the quantum emitter. (10)

The experimental implementation of the SUPER scheme relies on frequency-domain amplitude shaping. In the calculation, instead of specifying the single laser pulse parameters explicitly, Ω(t) is obtained by an inverse Fourier transform of the laser spectrum that is multiplied by an amplitude mask to describe the pulse shaping process. Starting point is a Gaussian frequency spectrum

(2)
with a spectral full width at half maximum (fwhm) of , centered around a detuning of ℏ(ωC – ω0) = −8.4 meV and an integrated resonant pulse area of α̃ = 26π. The amplitude function is approximated by two normalized Gaussian functions
(3)

This results in two contributions to the resulting spectrum at ωi with variable transmission Ĩi. From this, we define the detunings as Δi = ℏ(ωi – ω0). The spectral width is chosen to 0.2 meV for all calculations. To account for experimental imperfections of the pulse-shaping process, a transmission of 5% between the two peaks is added. Note that the transmission Ĩi is for the electric field in contrast to the experimental scenario where Ii (called transmissivity) is the intensity, that is, Ii corresponds to (Ĩi)2. A representative amplitude-shaped spectrum of the intensity is shown in Figure 1a. To calculate the exciton occupation, we derive the equations of motion from the Hamiltonian using the von-Neumann equation, which is then numerically integrated. (10) Because the phonon influence on the SUPER scheme has been shown to be weak, (26) we neglect phonons in the present calculations. In Figure 1b, we show an exemplary time dynamics at Δ1 = –4.9 meV, Δ2 = −11.12 meV and I1 = 0.5, I2 = 0.96.

Figure 1

Figure 1. Concept of SUPER scheme: (a) Spectrum of the broadband excitation pulse (red dashed curve) and an exemplary pulse pair (blue solid curve) after spectral shaping with transmissivities I1 = 0.5 and I2 = 0.96 at detunings Δ1 = −4.9 meV and Δ2 = −11.12 meV. Black arrow denotes the position of the targeted exciton state. (b) Calculated dynamics of the exciton population using the shaped spectrum. Inset shows the energy level scheme with detunings. |g⟩ , ground state, |x⟩, exciton state.

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To experimentally obtain the two red-detuned pulses with appropriate detunings, we implement frequency-domain amplitude shaping with a folded 4f pulse shaper equipped with a programmable spatial light modulator (SLM, CRi, 128 pixels). The experimental setup is summarized in Figure 2. A broadband Ti:sapphire laser (MIRA 900, Coherent) produces 120 fs long, Gaussian-shaped pulses with the central wavelength of 802 nm, pulse energy of ∼4 nJ and a peak power of ∼12 kW. The collimated laser beam that enters the 4f pulse shaper is first dispersed by a blazed diffraction grating (1800 lines/mm, Newport), and then focused onto the SLM with a curved mirror (f = 500 mm), such that each pixel is assigned a narrow laser spectral window of ∼0.09 nm (0.17 meV in energy, for details see SI). The amplitude-shaped laser beam travels the same path back and leaves the pulse shaper toward the cryostat with the quantum dot. The inset in Figure 2 shows a representative amplitude-shaped spectrum.

Figure 2

Figure 2. Sketch of the experimental setup: The laser beam is guided to a folded 4f pulse shaper equipped with a spatial light modulator (SLM) for amplitude-shaping the broadband spectrum (gray shade, inset). Incoming and outgoing beams are shown as separate paths for clarity. The shaped pulse-pair is directed with a beam splitter (BS) to the cryostat that holds the quantum dot at 8 K. Emitted photons from the quantum dot are sent through a bandpass filter (BPF) and a notch filter (NF) to either the spectrometer or with an additional fiber beam splitter (FBS) to the superconducting nanowire single-photon detectors (SNSPD) to record the photon coincidences. On the basis of above-band excitation, the quantum dot exciton emission line (X, green) is identified. An exemplary pulse-pair with detunings Δ1 (orange) and Δ2 (red) is also shown.

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To characterize the detunings of the two pulses with respect to the exciton line, we first performed above-band gap excitation of the quantum dot. The resulting emission spectrum is shown as a green curve in Figure 2. A sharp exciton-emission line (X) is identified at 798.66 nm, surrounded by phonon sidebands and substrate emission. Based on this, we can choose the detunings Δ1 and Δ2. Figure 2 also shows the unshaped laser spectrum as gray-shaded area. Its sharp edge on the high energy sideis due to a razor blade mounted behind the SLM to suppress the laser spectral tail that is resonant with the quantum dot emission line. The intensities of both pulses can be tuned individually by varying the transmissivities of the SLM pixels from 0 to 1, denoted as I1 and I2. For our experiments, the intensities of the second pulse at Δ2 = −10.6 meV range from 0.7 μW (I2 = 0) to 18.8 μW (I2 = 1) while the first pulse intensity I1 was fixed to 15.5 μW, measured at the cryostat window.

Our sample consists of GaAs/AlGaAs quantum dots obtained by the Al-droplet etching method. (27,28) The dots are embedded in the center of a λ-cavity placed between a bottom (top) distributed Bragg reflector consisting of 9(2) pairs of λ/4 thick Al0.95Ga0.05As/Al0.2Ga0.8As layers. The sample is kept in a closed-cycle cryostat with base temperature 8 K on a three-axis piezoelectric stage (ANPx101/ANPz102, attocube systems AG). The shaped pulse pair is focused onto the quantum dot with a cold aspheric lens (NA = 0.77, Edmund Optics) and the emission is collected via the same path backward, through a combination of a bandpass filter (808 nm, fwhm 3 nm, Layertec) and a notch filter (BNF-805-OD3, fwhm 0.3 nm, Optigrate) to a single-photon sensitive spectrometer (Acton SP-2750, Roper Scientific) equipped with a liquid nitrogen-cooled charge-coupled device camera (Spec10 CCD, Princeton Instruments) or superconducting nanowire single-photon detectors (SNSPD, Eos, Single Quantum). For estimating the wavelength-independent background, we integrate the photon counts on the high-energy sideband of the exciton emission peak (for a detailed discussion, see Figure S1 in SI).

To measure the SUPER scheme, we fix the detuning and the transmissivity of the first pulse to Δ1 = −4.9 meV and I1 = 0.5, respectively. We then vary the transmissivity of the second pulse (I2), and record the emitted spectra for various detunings (Δ2). The results are displayed as a two-dimensional map in Figure 3a, as a function of Δ2 and I2, where the color scale denotes the integrated photon counts. Every automated transmissivity scan (that is, individual columns in Figure 3a) records emitted spectra for 100 different I2 values, and the experiment is performed for 11 different Δ2 values. All the data shown are background-corrected as described in Figure S1 in SI. At zero intensity of the second pulse, that is, I2 = 0, only negligible photon counts are recorded, implying that no excitation occurs in the absence of the second pulse, even if the first pulse is present. By increasing I2 from 0 to 1, the exciton counts gradually increase, specifically for detunings around Δ2 = −10 to −11 meV. We find a clear region of high photon counts demonstrating that the exciton state becomes occupied by the two-pulse excitation. To validate further that the exciton state only gets populated when both pulses are switched on, we set I1 = 0, and perform the I2 – Δ2 scan, as in Figure 3a, which does not result in any significant exciton emission (see Figure S3a in SI).

Figure 3

Figure 3. Exciton population achieved by the SUPER scheme: (a) Measured photon counts at exciton emission energy as a function of the detuning Δ2 and the transmissivity I2 of the second pulse. The first pulse is fixed to Δ1 = −4.9 meV and I1 = 0.5. The scale shows the integrated exciton counts after correcting for background. The red dot indicates the parameters used in the photon quality experiment (Figure 4). (b) Theoretically calculated exciton (X) population based on a two-level system. (c) Vertical line-cuts through the 2D map for Δ2 = −10.5 meV (blue), –10.6 meV (red), and −10.9 meV (green). The dashed red line indicates the parameters at which the photon quality measurements are performed.

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Therefore, we conclude that under the action of two pulses below the absorption edge of the quantum dot an excitation via the SUPER scheme has taken place. The calculated dynamics of the two-level system under the red-detuned two-pulse excitation is shown in Figure 3b. The experimentally observed high exciton occupation at Δ2 ≈ −10.5 meV with a diagonal trend toward larger Δ2 and I2, shows excellent agreement with the theoretical results. The calculated maximum exciton occupation is ∼97% in the considered parameter window. For both experiment and theory, the condition that |Δ2| > 2|Δ1| holds.

Figure 3c shows line plots of the measured exciton occupation for Δ2 = −10.5, −10.6, and −10.9 meV featuring another interesting behavior: for the largest detuning Δ2 = −10.9 meV (green line), we find that the exciton counts increase monotonically with increasing I2. For Δ2 = −10.6 meV (red line), we find an increase in exciton counts up to I2 = 0.64, after which it decreases again. The most striking observation is for Δ2 = −10.5 meV (blue line), which shows close to 1.5 oscillations from I2 = 0–1 with a maximum at I2 = 0.4 and a minimum at I2 = 0.7. All these findings provide compelling evidence that the recorded exciton emission is due to the coherent excitation with two red-detuned pulses.

Following the experimental verification, here we discuss how the SUPER scheme compares to other schemes and its scope for quantum technologies. While a detailed comparison with all existing schemes goes beyond the scope of this paper, we investigate a different dot in the same sample under resonant two-photon-excitation (TPE) and SUPER excitation conditions. To perform TPE, we tune the excitation wavelength to the biexciton transition by shifting the amplitude mask in the SLM. The integrated photon counts at the exciton-emission energy obtained by the TPE (Figure 4a, blue circles) show coherent Rabi oscillation, as has been observed in similar works. (29) Most importantly, the maxima of both oscillations coincide, clearly demonstrating that SUPER reaches the same efficiency as TPE. Furthermore, in Figure 4b we show the emission spectra of the quantum dot under TPE (top panel) and SUPER excitation (bottom panel). The TPE spectrum shows the exciton and biexciton emission peaks in addition to the scattered laser energy, while the SUPER spectrum shows the exciton emission peak and the first detuned pulse. As expected, the exciton emission lines in both spectra coincide. Notably, the first detuned pulse in SUPER is clearly distant from the biexciton energy and has no chance of exciting any transition other than the targeted exciton state.

Figure 4

Figure 4. Scope of SUPER scheme: (a) Measured photon counts at the exciton-emission energy (red crosses) under SUPER excitation in contrast to resonant TPE (blue circles). The x-axes values show corresponding power measured with a 1% beam sampler near the cryostat window. (b) Quantum dot emission spectra under TPE (top panel) and SUPER excitation (bottom panel). The TPE emission spectrum shows residual laser scattering and the SUPER emission spectrum shows the first detuned pulse. (c) Single photon characteristics under SUPER excitation as shown by g(2)(0) = 0.06(1). The dark green dots show the measured data, while the orange curves denote the fit.

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Furthermore, we verify that the SUPER scheme can be used to generate single photons. For this, we choose excitation parameters yielding maximal occupation (indicated by the red dot in Figure 3), that is, we set Δ1 = −4.9 meV, I1 = 0.5, Δ2 = −10.6 meV, and I2 = 0.64. We then measure the single-photon characteristics in a Hanbury Brown and Twiss (HBT) setup. The results are displayed in Figure 4b. We achieve a g(2)(0) = 0.06(1), which is a very promising result toward the goal of producing high quality single photons, considering that the experiments are performed at T = 8 K. Under s-shell resonant excitation, we observed a g(2)(0) = 0.016 (30) on the same quantum dot. We find that the recorded g(2)(0) under SUPER is slightly higher than under s-shell resonant excitation due to the laser scattering background, considering that the excitation power in SUPER is much higher compared to s-shell resonant excitation. We are, however, confident that scattered laser light can be suppressed better with moderate experimental effort.

It is also worthwhile to discuss SUPER in comparison to existing resonant or near-resonant excitation schemes. (7) Among those, coherent schemes include Rabi rotations, (2,3,31,32) chirped excitations exploiting the adiabatic rapid passage effect, (5,6,33−37) and dichromatic excitation. (8,9,38) Preparation of the exciton state can also be achieved by TPE to the biexciton state followed by a timed stimulation of the biexciton-to-exciton transition. (39−41) Although all of these schemes have their own advantages and disadvantages, the superiority of SUPER is that it circumvents the need for polarization filtering and is quite flexible regarding the chosen detuning values. While polarization filtering is also uncalled for in the dichromatic scheme, a clear advantage of SUPER is that both pulses are red-detuned and therefore no higher-lying states of the quantum dot will be directly addressed.

Another group of state-preparation schemes are phonon-assisted processes, (19,27,42−46) which require an additional particle, the phonon, to function. Hence, those schemes are incoherent, which might be disadvantageous when preparing superposition states. In addition, the laser pulses in phonon-assisted schemes are blue-detuned. Therefore, SUPER might also be a viable alternative to these schemes.

In conclusion, this work demonstrates that a red-detuned pulse pair can populate the exciton state in a quantum dot relying on the SUPER mechanism. This is astonishing given that a single pulse at these far detunings does not lead to a population inversion. In particular, the excitation below the absorption edge removes the stringent need of polarization filtering. Our simple yet elegant implementation of this new technique through amplitude shaping contributes toward an effortless method for generating high-purity single photons.

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The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.2c01783.

  • Experimental details; background estimation; normalization of the pulse intensities; verification of the two-pulse effect; optimizing the first pulse intensity; lifetime and intrinsic line width; radiative efficiency (PDF)

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  • Corresponding Author
    • Vikas Remesh - Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria;  Email: [email protected]
  • Authors
    • Yusuf Karli - Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria;  Orcidhttps://orcid.org/0000-0001-8987-828X
    • Florian Kappe - Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
    • Thomas K. Bracht - Institut für Festkörpertheorie, Universität Münster, Münster 48149, Germany
    • Julian Münzberg - Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
    • Saimon Covre da Silva - Institute of Semiconductor and Solid State Physics, Johannes Kepler University Linz, Linz 4040, Austria
    • Tim Seidelmann - Theoretische Physik III, Universität Bayreuth, Bayreuth 95440, Germany
    • Vollrath Martin Axt - Theoretische Physik III, Universität Bayreuth, Bayreuth 95440, Germany
    • Armando Rastelli - Institute of Semiconductor and Solid State Physics, Johannes Kepler University Linz, Linz 4040, Austria
    • Doris E. Reiter - Institut für Festkörpertheorie, Universität Münster, Münster 48149, Germany;  Present Address: Condensed Matter Theory, Department of Physics, TU Dortmund, Dortmund, 44221, Germany;  Orcidhttps://orcid.org/0000-0002-3648-353X
    • Gregor Weihs - Institut für Experimentalphysik, Universität Innsbruck, Innsbruck 6020, Austria
  • Author Contributions

    Y.K. and F.K. contributed equally.

  • Funding

    Open Access is funded by the Austrian Science Fund (FWF).

  • Notes
    The authors declare no competing financial interest.

Acknowledgments

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The authors acknowledge Marita Wagner, Tommaso Faleo, Ron Stepanek (Meadowlark Optics Inc.), and Bernd Eppich (BeamXpert GmbH) for valuable discussions during the experiment and preparation of the manuscript. Y.K., F.K., V.R., J. M., and G. W. acknowledge financial support through FWF projects FG 5, I4380 (AEQuDot), TAI-556N (DarkEneT), and W1259 (DK-ALM Atoms, Light, and Molecules). T.K.B. and D.E.R. acknowledge financial support from the German Research Foundation DFG through project 428026575 (AEQuDot). A.R. and S.F.C.d.S. acknowledge C. Schimpf for fruitful discussions, the FWF projects FG 5, P 30459, I 4320, the Linz Institute of Technology (LIT) and the European Union’s Horizon 2020 research, and innovation program under Grant Agreements 899814 (Qurope) and 871130 (ASCENT+).

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    Wu, Y.; Piper, I. M.; Ediger, M.; Brereton, P.; Schmidgall, E. R.; Eastham, P. R.; Hugues, M.; Hopkinson, M.; Phillips, R. T. Population inversion in a single InGaAs quantum dot using the method of adiabatic rapid passage. Phys. Rev. Lett. 2011, 106, 67401,  DOI: 10.1103/PhysRevLett.106.067401
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    Population Inversion in a Single InGaAs Quantum Dot Using the Method of Adiabatic Rapid Passage
    Wu, Yanwen; Piper, I. M.; Ediger, M.; Brereton, P.; Schmidgall, E. R.; Eastham, P. R.; Hugues, M.; Hopkinson, M.; Phillips, R. T.
    Physical Review Letters (2011), 106 (6), 067401/1-067401/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
    Prepn. of a specific quantum state is a required step for a variety of proposed quantum applications. The authors report an exptl. demonstration of optical quantum state inversion in a single semiconductor quantum dot using adiabatic rapid passage. This method is insensitive to variation in the optical coupling in contrast with earlier work based on Rabi oscillations. When the pulse power exceeds a threshold for inversion, the final state is independent of power. This provides a new tool for prepg. quantum states in semiconductor dots and has a wide range of potential uses.
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  7. 7
    Lüker, S.; Reiter, D. E. A review on optical excitation of semiconductor quantum dots under the influence of phonons. Semicond. Sci. Technol. 2019, 34, 063002,  DOI: 10.1088/1361-6641/ab1c14
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    A review on optical excitation of semiconductor quantum dots under the influence of phonons
    Lueker, Sebastian; Reiter, Doris E.
    Semiconductor Science and Technology (2019), 34 (6), 063002CODEN: SSTEET; ISSN:0268-1242. (IOP Publishing Ltd.)
    A review. The prepn. of excitonic states in semiconductor quantum dots is a prerequisite for the application of quantum dots in quantum information technol., e.g., as source of single or entangled photons. For quantum dots embedded in the semiconductor matrix, the interaction with phonons significantly modifies the ideal prepn. schemes. Due to the electron-phonon interaction Rabi rotations and the population inversion induced by excitation with chirped pulses can be damped, while an active use of phonons allows for a phonon-assisted state prepn. Under certain conditions the reappearance regime can be entered, in which the phonon influence is negligible. For a quantum dot in a cavity, the properties of the emitted light can also be modified by the phonons. In this review, the effects of electron-phonon interaction on the different optical state prepn. protocols are explained and the latest exptl. and theor. results implementing these protocols are presented.
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  8. 8
    He, Y. M.; Wang, H.; Wang, C.; Chen, M. C.; Ding, X.; Qin, J.; Duan, Z. C.; Chen, S.; Li, J. P.; Liu, R. Z.; Schneider, C.; Atatüre, M.; Höfling, S.; Lu, C. Y.; Pan, J. W. Coherently driving a single quantum two-level system with dichromatic laser pulses. Nat. Phys. 2019, 15, 941– 946,  DOI: 10.1038/s41567-019-0585-6
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    Coherently driving a single quantum two-level system with dichromatic laser pulses
    He, Yu-Ming; Wang, Hui; Wang, Can; Chen, M.-C.; Ding, Xing; Qin, Jian; Duan, Z.-C.; Chen, Si; Li, J.-P.; Liu, Run-Ze; Schneider, C.; Atature, Mete; Hofling, Sven; Lu, Chao-Yang; Pan, Jian-Wei
    Nature Physics (2019), 15 (9), 941-946CODEN: NPAHAX; ISSN:1745-2473. (Nature Research)
    The excitation of individual two-level quantum systems using an electromagnetic field is an elementary tool of quantum optics, with widespread applications across quantum technologies. The efficient excitation of a single two-level system usually requires the driving field to be at the same frequency as the transition between the two quantum levels. However, in solid-state implementations, the scattered laser light can dominate over the single photons emitted by the two-level system, imposing a challenge for single-photon sources. Here, we propose a background-free method for the coherent excitation and control of a two-level quantum system using a phase-locked dichromatic electromagnetic field with no spectral overlap with the optical transition. We demonstrate this method exptl. by stimulating single-photon emission from a single quantum dot embedded in a micropillar, reaching single-photon purity of 0.988(1) and indistinguishability of 0.962(6). The phase-coherent nature of our two-color excitation scheme is demonstrated by the dependence of the resonance fluorescence intensity on the relative phase between the two pulses. Our two-color excitation method represents an addnl. and useful tool for the study of atom-photon interaction, and the generation of spectrally isolated indistinguishable single photons.
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  9. 9
    Koong, Z. X.; Scerri, E.; Rambach, M.; Cygorek, M.; Brotons-Gisbert, M.; Picard, R.; Ma, Y.; Park, S. I.; Song, J. D.; Gauger, E. M.; Gerardot, B. D. Coherent Dynamics in Quantum Emitters under Dichromatic Excitation. Phys. Rev. Lett. 2021, 126, 47403,  DOI: 10.1103/PhysRevLett.126.047403
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    9
    Coherent Dynamics in Quantum Emitters under Dichromatic Excitation
    Koong, Z. X.; Scerri, E.; Rambach, M.; Cygorek, M.; Brotons-Gisbert, M.; Picard, R.; Ma, Y.; Park, S. I.; Song, J. D.; Gauger, E. M.; Gerardot, B. D.
    Physical Review Letters (2021), 126 (4), 047403CODEN: PRLTAO; ISSN:1079-7114. (American Physical Society)
    We characterize the coherent dynamics of a two-level quantum emitter driven by a pair of sym. detuned phase-locked pulses. The promise of dichromatic excitation is to spectrally isolate the excitation laser from the quantum emission, enabling background-free photon extn. from the emitter. While excitation is not possible without spectral overlap between the exciting pulse and the quantum emitter transition for ideal two-level systems due to cancellation of the accumulated pulse area, we find that any addnl. interactions that interfere with cancellation of the accumulated pulse area may lead to a finite stationary population inversion. Our spectroscopic results of a solid-state two-level system show that, while coupling to lattice vibrations helps to improve the inversion efficiency up to 50% under sym. driving, coherent population control and a larger amt. of inversion are possible using asym. dichromatic excitation, which we achieve by adjusting the ratio of the intensities between the red- and blue-detuned pulses. Our measured results, supported by simulations using a real-time path-integral method, offer a new perspective toward realizing efficient, background-free photon generation and extn.
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  10. 10
    Bracht, T. K.; Cosacchi, M.; Seidelmann, T.; Cygorek, M.; Vagov, A.; Axt, V. M.; Heindel, T.; Reiter, D. E. Swing-Up of Quantum Emitter Population Using Detuned Pulses. PRX Quantum 2021, 2, 40354,  DOI: 10.1103/PRXQuantum.2.040354
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    Gazzano, O.; Michaelis De Vasconcellos, S.; Arnold, C.; Nowak, A.; Galopin, E.; Sagnes, I.; Lanco, L.; Lemaître, A.; Senellart, P. Bright solid-state sources of indistinguishable single photons. Nat. Commun. 2013, 4, 1425,  DOI: 10.1038/ncomms2434
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    11
    Bright solid-state sources of indistinguishable single photons
    Gazzano O; Michaelis de Vasconcellos S; Arnold C; Nowak A; Galopin E; Sagnes I; Lanco L; Lemaitre A; Senellart P
    Nature communications (2013), 4 (), 1425 ISSN:.
    Bright sources of indistinguishable single photons are strongly needed for the scalability of quantum information processing. Semiconductor quantum dots are promising systems to build such sources. Several works demonstrated emission of indistinguishable photons while others proposed various approaches to efficiently collect them. Here we combine both properties and report on the fabrication of ultrabright sources of indistinguishable single photons, thanks to deterministic positioning of single quantum dots in well-designed pillar cavities. Brightness as high as 0.79±0.08 collected photon per pulse is demonstrated. The indistinguishability of the photons is investigated as a function of the source brightness and the excitation conditions. We show that a two-laser excitation scheme allows reducing the fluctuations of the quantum dot electrostatic environment under high pumping conditions. With this method, we obtain 82±10% indistinguishability for a brightness as large as 0.65±0.06 collected photon per pulse.
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  12. 12
    Ding, X.; He, Y.; Duan, Z. C.; Gregersen, N.; Chen, M. C.; Unsleber, S.; Maier, S.; Schneider, C.; Kamp, M.; Höfling, S.; Lu, C. Y.; Pan, J. W. On-Demand Single Photons with High Extraction Efficiency and Near-Unity Indistinguishability from a Resonantly Driven Quantum Dot in a Micropillar. Phys. Rev. Lett. 2016, 116, 20401,  DOI: 10.1103/PhysRevLett.116.020401
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    12
    On-Demand Single Photons with High Extraction Efficiency and Near-Unity Indistinguishability from a Resonantly Driven Quantum Dot in a Micropillar
    Ding Xing; He Yu; Duan Z-C; Chen M-C; Hofling Sven; Lu Chao-Yang; Pan Jian-Wei; Ding Xing; He Yu; Duan Z-C; Chen M-C; Lu Chao-Yang; Pan Jian-Wei; Ding Xing; He Yu; Duan Z-C; Chen M-C; Lu Chao-Yang; Pan Jian-Wei; Gregersen Niels; Unsleber S; Maier S; Schneider Christian; Kamp Martin; Hofling Sven; Hofling Sven
    Physical review letters (2016), 116 (2), 020401 ISSN:.
    Scalable photonic quantum technologies require on-demand single-photon sources with simultaneously high levels of purity, indistinguishability, and efficiency. These key features, however, have only been demonstrated separately in previous experiments. Here, by s-shell pulsed resonant excitation of a Purcell-enhanced quantum dot-micropillar system, we deterministically generate resonance fluorescence single photons which, at π pulse excitation, have an extraction efficiency of 66%, single-photon purity of 99.1%, and photon indistinguishability of 98.5%. Such a single-photon source for the first time combines the features of high efficiency and near-perfect levels of purity and indistinguishabilty, and thus opens the way to multiphoton experiments with semiconductor quantum dots.
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    Senellart, P.; Solomon, G.; White, A. High-performance semiconductor quantum-dot single-photon sources. Nat. Nanotechnol. 2017, 12, 1026– 1039,  DOI: 10.1038/nnano.2017.218
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    13
    High-performance semiconductor quantum-dot single-photon sources
    Senellart, Pascale; Solomon, Glenn; White, Andrew
    Nature Nanotechnology (2017), 12 (11), 1026-1039CODEN: NNAABX; ISSN:1748-3387. (Nature Research)
    A review. Single photons are a fundamental element of most quantum optical technologies. The ideal single-photon source is an on-demand, deterministic, single-photon source delivering light pulses in a well-defined polarization and spatiotemporal mode, and contg. exactly one photon. In addn., for many applications, there is a quantum advantage if the single photons are indistinguishable in all their degrees of freedom. Single-photon sources based on parametric down-conversion are currently used, and while excellent in many ways, scaling to large quantum optical systems remains challenging. In 2000, semiconductor quantum dots were shown to emit single photons, opening a path towards integrated single-photon sources. Here, we review the progress achieved in the past few years, and discuss remaining challenges. The latest quantum dot-based single-photon sources are edging closer to the ideal single-photon source, and have opened new possibilities for quantum technologies.
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  14. 14
    Schweickert, L.; Jöns, K. D.; Zeuner, K. D.; Covre Da Silva, S. F.; Huang, H.; Lettner, T.; Reindl, M.; Zichi, J.; Trotta, R.; Rastelli, A.; Zwiller, V. On-demand generation of background-free single photons from a solid-state source. Appl. Phys. Lett. 2018, 112, 093106,  DOI: 10.1063/1.5020038
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    14
    On-demand generation of background-free single photons from a solid-state source
    Schweickert, Lucas; Joens, Klaus D.; Zeuner, Katharina D.; Covre da Silva, Saimon Filipe; Huang, Huiying; Lettner, Thomas; Reindl, Marcus; Zichi, Julien; Trotta, Rinaldo; Rastelli, Armando; Zwiller, Val
    Applied Physics Letters (2018), 112 (9), 093106/1-093106/4CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
    True on-demand high-repetition-rate single-photon sources are highly sought after for quantum information processing applications. Any coherently driven 2-level quantum system suffers from a finite reexcitation probability under pulsed excitation, causing undesirable multi-photon emission. A solid-state source of on-demand single photons yielding a raw 2nd-order coherence of g(2)(0) = (7.5 ± 1.6) × 10-5 without any background subtraction or data processing is presented. To this date, this is the lowest value of g(2)(0) reported for any single-photon source even compared to the previously reported best background subtracted values. This result was achieved on GaAs/AlGaAs quantum dots embedded in a low-Q planar cavity by using (i) a 2-photon excitation process and (ii) a filtering and detection setup featuring 2 superconducting single-photon detectors with ultralow dark-count rates of (0.0056 ± 0.0007) s-1 and (0.017 ± 0.001) s-1, resp. Reexcitation processes are dramatically suppressed by (i), while (ii) removes false coincidences resulting in a negligibly low noise floor. (c) 2018 American Institute of Physics.
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    Rodt, S.; Reitzenstein, S.; Heindel, T. Deterministically fabricated solid-state quantum-light sources. J. Phys.: Condens. Matter 2020, 32, 153003,  DOI: 10.1088/1361-648X/ab5e15
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    15
    Deterministically fabricated solid-state quantum-light sources
    Rodt, Sven; Reitzenstein, Stephan; Heindel, Tobias
    Journal of Physics: Condensed Matter (2020), 32 (15), 153003CODEN: JCOMEL; ISSN:0953-8984. (IOP Publishing Ltd.)
    A review. The controlled generation of non-classical states of light is a challenging task at the heart of quantum optics. Aside from the mere spirit of science, the related research is strongly driven by applications in photonic quantum technologies, including the fields of quantum communication, quantum computation, and quantum metrol. In this context, the realization of integrated solid-state-based quantum-light sources is of particular interest, due to the prospects for scalability and device integration. This topical review focuses on solid-state quantum-light sources which are fabricated in a deterministic fashion. In this framework we cover quantum emitters represented by semiconductor quantum dots, color centers in diamond, and defect-/strain-centers in two-dimensional materials. First, we introduce the topic of quantum-light sources and non-classical light generation for applications in photonic quantum technologies, motivating the need for the development of scalable device technologies to push the field towards real-world applications. In the second part, we summarize material systems hosting quantum emitters in the solid-state. The third part reviews deterministic fabrication techniques and comparatively discusses their advantages and disadvantages. The techniques are classified in bottom-up approaches, exploiting the site-controlled positioning of the quantum emitters themselves, and top-down approaches, allowing for the precise alignment of photonic microstructures to pre-selected quantum emitters. Special emphasis is put on the progress achieved in the development of in situ techniques, which significantly pushed the performance of quantum-light sources towards applications. Addnl., we discuss hybrid approaches, exploiting pick-and-place techniques or wafer-bonding. The fourth part presents state-of-the-art quantum-dot quantum-light sources based on the fabrication techniques presented in the previous sections, which feature engineered functionality and enhanced photon collection efficiency. The article closes by highlighting recent applications of deterministic solid-state-based quantum-light sources in the fields of quantum communication, quantum computing, and quantum metrol., and by discussing future perspectives in the field of solid-state quantum-light sources.
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    Srocka, N.; Mrowiński, P.; Große, J.; von Helversen, M.; Heindel, T.; Rodt, S.; Reitzenstein, S. Deterministically fabricated quantum dot single-photon source emitting indistinguishable photons in the telecom O-band. Appl. Phys. Lett. 2020, 116, 231104,  DOI: 10.1063/5.0010436
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    16
    Deterministically fabricated quantum dot single-photon source emitting indistinguishable photons in the telecom O-band
    Srocka, N.; Mrowinski, P.; Grosse, J.; von Helversen, M.; Heindel, T.; Rodt, S.; Reitzenstein, S.
    Applied Physics Letters (2020), 116 (23), 231104CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
    The authors develop and study single-photon sources based on InGaAs quantum dots (QDs) emitting in the telecom O-band. Quantum devices are fabricated using in situ electron beam lithog. in combination with thermocompression bonding to realize a backside Au mirror. The structures are based on InGaAs/GaAs heterostructures, where the QD emission is red shifted toward the telecom O-band at 1.3μm via a strain-reducing layer. QDs pre-selected by cathodoluminescence mapping are embedded into mesa structures with a backside Au mirror for enhanced photon-extn. efficiency. Photon-autocorrelation measurements under pulsed nonresonant wetting-layer excitation are performed at temps. up to 40 K, showing pure single-photon emission, which makes the devices compatible with stand-alone operation using Stirling cryocoolers. Using pulsed p-shell excitation, the authors realize single-photon emission with a high multi-photon suppression of g(2)(0) = 0.027 ± 0.005, an as-measured 2-photon interference visibility of (12 ± 4)%, a post-selected visibility of (96 ± 10)%, and an assocd. coherence time of (212 ± 25) ps. Also, the structures show an extn. efficiency of ∼5%, which is comparable to values expected from numeric simulations of this photonic structure. Further improvements of the devices will enable implementations of quantum communication via optical fibers. (c) 2020 American Institute of Physics.
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    Wang, B. Y.; Denning, E. V.; Gür, U. M.; Lu, C. Y.; Gregersen, N. Micropillar single-photon source design for simultaneous near-unity efficiency and indistinguishability. Phys. Rev. B 2020, 102, 125301,  DOI: 10.1103/PhysRevB.102.125301
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    Micropillar single-photon source design for simultaneous near-unity efficiency and indistinguishability
    Wang, Bi-Ying; Denning, Emil V.; Gur, Ugur Meric; Lu, Chao-Yang; Gregersen, Niels
    Physical Review B (2020), 102 (12), 125301CODEN: PRBHB7; ISSN:2469-9969. (American Physical Society)
    We present a numerical investigation of the performance of the micropillar cavity single-photon source in terms of collection efficiency and indistinguishability of the emitted photons in the presence of non-Markovian phonon-induced decoherence. We analyze the physics governing the efficiency using a single-mode model, and we optimize efficiency ε and the indistinguishability η on an equal footing by computing εη as function of the micropillar design parameters. We show that εη is limited to ~ 0.96 for the ideal geometry due to an inherent tradeoff between efficiency and indistinguishability. Finally, we subsequently consider the influence of realistic fabrication imperfections and Markovian pure dephasing noise on the performance.
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    Tomm, N.; Javadi, A.; Antoniadis, N. O.; Najer, D.; Löbl, M. C.; Korsch, A. R.; Schott, R.; Valentin, S. R.; Wieck, A. D.; Ludwig, A.; Warburton, R. J. A bright and fast source of coherent single photons. Nat. Nanotechnol. 2021, 16, 399– 403,  DOI: 10.1038/s41565-020-00831-x
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    18
    A bright and fast source of coherent single photons
    Tomm, Natasha; Javadi, Alisa; Antoniadis, Nadia Olympia; Najer, Daniel; Lobl, Matthias Christian; Korsch, Alexander Rolf; Schott, Rudiger; Valentin, Sascha Rene; Wieck, Andreas Dirk; Ludwig, Arne; Warburton, Richard John
    Nature Nanotechnology (2021), 16 (4), 399-403CODEN: NNAABX; ISSN:1748-3387. (Nature Portfolio)
    A single-photon source is an enabling technol. in device-independent quantum communication, quantum simulation, and linear optics-based and measurement-based quantum computing. These applications employ many photons and place stringent requirements on the efficiency of single-photon creation. The scaling on efficiency is typically an exponential function of the no. of photons. Schemes taking full advantage of quantum superpositions also depend sensitively on the coherence of the photons, i.e., their indistinguishability. Here, we report a single-photon source with a high end-to-end efficiency. We employ gated quantum dots in an open, tunable microcavity. The gating provides control of the charge and elec. tuning of the emission frequency; the high-quality material ensures low noise; and the tunability of the microcavity compensates for the lack of control in quantum dot position and emission frequency. Transmission through the top mirror is the dominant escape route for photons from the microcavity, and this output is well matched to a single-mode fiber. With this design, we can create a single photon at the output of the final optical fiber on-demand with a probability of up to 57% and with an av. two-photon interference visibility of 97.5%. Coherence persists in trains of thousands of photons with single-photon creation at a repetition rate of 1 GHz.
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    Thomas, S. E. Bright Polarized Single-Photon Source Based on a Linear Dipole. Phys. Rev. Lett. 2021, 126, 233601,  DOI: 10.1103/PhysRevLett.126.233601
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    19
    Bright Polarized Single-Photon Source Based on a Linear Dipole
    Thomas, S. E.; Billard, M.; Coste, N.; Wein, S. C.; Priya; Ollivier, H.; Krebs, O.; Tazairt, L.; Harouri, A.; Lemaitre, A.; Sagnes, I.; Anton, C.; Lanco, L.; Somaschi, N.; Loredo, J. C.; Senellart, P.
    Physical Review Letters (2021), 126 (23), 233601CODEN: PRLTAO; ISSN:1079-7114. (American Physical Society)
    Semiconductor quantum dots in cavities are promising single-photon sources. Here, we present a path to deterministic operation, by harnessing the intrinsic linear dipole in a neutral quantum dot via phonon-assisted excitation. This enables emission of fully polarized single photons, with a measured degree of linear polarization up to 0.994±0.007, and high population inversion-85% as high as resonant excitation. We demonstrate a single-photon source with a polarized first lens brightness of 0.50±0.01, a single-photon purity of 0.954±0.001, and single-photon indistinguishability of 0.909±0.004.
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    Lu, C.-Y.; Pan, J.-W. Quantum-dot single-photon sources for the quantum internet. Nat. Nanotechol. 2021, 16, 1294– 1296,  DOI: 10.1038/s41565-021-01033-9
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    Lodahl, P.; Mahmoodian, S.; Stobbe, S. Interfacing single photons and single quantum dots with photonic nanostructures. Rev. Mod. Phys. 2015, 87, 347– 400,  DOI: 10.1103/RevModPhys.87.347
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    Interfacing single photons and single quantum dots with photonic nanostructures
    Lodahl, Peter; Mahmoodian, Sahand; Stobbe, Soren
    Reviews of Modern Physics (2015), 87 (2), 347-400CODEN: RMPHAT; ISSN:0034-6861. (American Physical Society)
    Photonic nanostructures provide a means of tailoring the interaction between light and matter and the past decade has witnessed tremendous exptl. and theor. progress on this subject. In particular, the combination with semiconductor quantum dots has proven successful. This manuscript reviews quantum optics with excitons in single quantum dots embedded in photonic nanostructures. The ability to engineer the light-matter interaction strength in integrated photonic nanostructures enables a range of fundamental quantum-electrodynamics expts. on, e.g.. spontaneous- emission control, modified Lamb shifts, and enhanced dipole-dipole interaction. Furthermore, highly efficient single-photon sources and giant photon nonlinearities may be implemented with immediate applications for photonic quantum-information processing. This review summarizes the general theor. framework of photon emission including the role of dephasing processes and applies it to photonic nanostructures of current interest, such as photonic-crystal cavities and waveguides, dielec. nanowires, and plasmonic waveguides. The introduced concepts are generally applicable in quantum nanophotonics and apply to a large extent also to other quantum emitters, such as mols., nitrogen vacancy centers, or atoms. Finally, the progress and future prospects of applications in quantum-information processing are considered.
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    Dusanowski, Ł.; Köck, D.; Shin, E.; Kwon, S. H.; Schneider, C.; Höfling, S. Purcell-Enhanced and Indistinguishable Single-Photon Generation from Quantum Dots Coupled to On-Chip Integrated Ring Resonators. Nano Lett. 2020, 20, 6357– 6363,  DOI: 10.1021/acs.nanolett.0c01771
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    22
    Purcell-Enhanced and Indistinguishable Single-Photon Generation from Quantum Dots Coupled to On-Chip Integrated Ring Resonators
    Dusanowski, Lukasz; Koeck, Dominik; Shin, Eunso; Kwon, Soon-Hong; Schneider, Christian; Hoefling, Sven
    Nano Letters (2020), 20 (9), 6357-6363CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
    Integrated photonic circuits provide a versatile toolbox of functionalities for advanced quantum optics applications. Here, we demonstrate an essential component of such a system in the form of a Purcell-enhanced single-photon source based on a quantum dot coupled to a robust on-chip integrated resonator. For that, we develop GaAs monolithic ring cavities based on distributed Bragg reflector ridge waveguides. Under resonant excitation conditions, we observe an over 2-fold spontaneous emission rate enhancement using Purcell effect and gain a full coherent optical control of a QD-two-level system via Rabi oscillations. Furthermore, we demonstrate an on-demand single-photon generation with strongly suppressed multiphoton emission probability as low as 1% and two-photon interference with visibility up to 95%. This integrated single-photon source can be readily scaled up, promising a realistic pathway for scalable on-chip linear optical quantum simulation, quantum computation, and quantum networks.
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  23. 23
    Uppu, R.; Pedersen, F. T.; Wang, Y.; Olesen, C. T.; Papon, C.; Zhou, X.; Midolo, L.; Scholz, S.; Wieck, A. D.; Ludwig, A.; Lodahl, P. Scalable integrated single-photon source. Sci. Adv. 2020, 6, eabc8268  DOI: 10.1126/sciadv.abc8268
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    Elshaari, A. W.; Pernice, W.; Srinivasan, K.; Benson, O.; Zwiller, V. Hybrid integrated quantum photonic circuits. Nat. Photonics 2020, 14, 285– 298,  DOI: 10.1038/s41566-020-0609-x
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    Hybrid integrated quantum photonic circuits
    Elshaari, Ali W.; Pernice, Wolfram; Srinivasan, Kartik; Benson, Oliver; Zwiller, Val
    Nature Photonics (2020), 14 (5), 285-298CODEN: NPAHBY; ISSN:1749-4885. (Nature Research)
    Abstr.: Recent developments in chip-based photonic quantum circuits have radically impacted quantum information processing. However, it is challenging for monolithic photonic platforms to meet the stringent demands of most quantum applications. Hybrid platforms combining different photonic technologies in a single functional unit have great potential to overcome the limitations of monolithic photonic circuits. Our Review summarizes the progress of hybrid quantum photonics integration, discusses important design considerations, including optical connectivity and operation conditions, and highlights several successful realizations of key phys. resources for building a quantum teleporter. We conclude by discussing the roadmap for realizing future advanced large-scale hybrid devices, beyond the solid-state platform, which hold great potential for quantum information applications.
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  25. 25
    Bounouar, S.; Davanco, M.; Reitzenstein, S. Semicond. Semimet.; Elsevier, 2020; Vol. 105; pp 153– 234.
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    Bracht, T. K.; Seidelmann, T.; Kuhn, T.; Axt, V. M.; Reiter, D. E. Phonon Wave Packet Emission during State Preparation of a Semiconductor Quantum Dot using Different Schemes. Phys. Status Solidi B 2022, 259, 2100649,  DOI: 10.1002/pssb.202100649
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    26
    Phonon Wave Packet Emission during State Preparation of a Semiconductor Quantum Dot using Different Schemes
    Bracht, Thomas K.; Seidelmann, Tim; Kuhn, Tilmann; Axt, Vollrath Martin; Reiter, Doris E.
    Physica Status Solidi B: Basic Solid State Physics (2022), 259 (6), 2100649CODEN: PSSBBD; ISSN:0370-1972. (Wiley-VCH Verlag GmbH & Co. KGaA)
    The carrier-phonon interaction in semiconductor quantum dots (QDs) can greatly affect the optical prepn. of the excited state. For resonant excitation used in the Rabi prepn. scheme, the polaron is formed accompanied by the emission of a phonon wave packet, leading to a degrdn. of prepn. fidelity. In this article, phonon wave packets for different coherent excitation schemes are analyzed. One example is the adiabatic rapid passage scheme relying on a chirped excitation. Herein, also a phonon wave packet is emitted, but the prepn. fidelity can still be approx. unity. A focus is on the phonon impact on a recently proposed swing-up scheme, induced by two detuned pulses. Similar to the Rabi scheme, a degrdn. and a phonon wave packet emission are found, despite the detuning. If the swing-up frequency coincides with the max. of the phonon spectral d., a series of wave packets is emitted yielding an even stronger degrdn. The insight gained from our results further helps in designing an optimal prepn. scheme for QDs.
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    Huber, D.; Reindl, M.; Huo, Y.; Huang, H.; Wildmann, J. S.; Schmidt, O. G.; Rastelli, A.; Trotta, R. Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots. Nat. Commun. 2017, 8, 15506,  DOI: 10.1038/ncomms15506
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    Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots
    Huber, Daniel; Reindl, Marcus; Huo, Yongheng; Huang, Huiying; Wildmann, Johannes S.; Schmidt, Oliver G.; Rastelli, Armando; Trotta, Rinaldo
    Nature Communications (2017), 8 (), 15506CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
    The development of scalable sources of non-classical light is fundamental to unlocking the technol. potential of quantum photonics. Semiconductor quantum dots are emerging as near-optimal sources of indistinguishable single photons. However, their performance as sources of entangled-photon pairs are still modest compared to parametric down converters. Photons emitted from conventional Stranski-Krastanov InGaAs quantum dots have shown non-optimal levels of entanglement and indistinguishability. For quantum networks, both criteria must be met simultaneously. Here, we show that this is possible with a system that has received limited attention so far: GaAs quantum dots. They can emit triggered polarization-entangled photons with high purity (g(2)(0) = 0.002±0.002), high indistinguishability (0.93±0.07 for 2 ns pulse sepn.) and high entanglement fidelity (0.94±0.01). Our results show that GaAs might be the material of choice for quantum-dot entanglement sources in future quantum technologies.
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  28. 28
    da Silva, S. F. C.; Undeutsch, G.; Lehner, B.; Manna, S.; Krieger, T. M.; Reindl, M.; Schimpf, C.; Trotta, R.; Rastelli, A. GaAs quantum dots grown by droplet etching epitaxy as quantum light sources. Appl. Phys. Lett. 2021, 119, 120502,  DOI: 10.1063/5.0057070
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    GaAs quantum dots grown by droplet etching epitaxy as quantum light sources
    da Silva, Saimon Filipe Covre; Undeutsch, Gabriel; Lehner, Barbara; Manna, Santanu; Krieger, Tobias M.; Reindl, Marcus; Schimpf, Christian; Trotta, Rinaldo; Rastelli, Armando
    Applied Physics Letters (2021), 119 (12), 120502CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
    A review. This Perspective presents an overview on the epitaxial growth and optical properties of GaAs quantum dots obtained with the droplet etching method as high-quality sources of quantum light. We illustrate recent achievements regarding the generation of single photons and polarization entangled photon pairs and the use of these sources in applications of central importance in quantum communication such as entanglement swapping and quantum key distribution. (c) 2021 American Institute of Physics.
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    Jayakumar, H.; Predojević, A.; Huber, T.; Kauten, T.; Solomon, G. S.; Weihs, G. Deterministic photon pairs and coherent optical control of a single quantum dot. Phys. Rev. Lett. 2013, 110, 135505,  DOI: 10.1103/PhysRevLett.110.135505
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    Deterministic photon pairs and coherent optical control of a single quantum dot
    Jayakumar, Harishankar; Predojevic, Ana; Huber, Tobias; Kauten, Thomas; Solomon, Glenn S.; Weihs, Gregor
    Physical Review Letters (2013), 110 (13), 135505/1-135505/5CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
    The strong confinement of semiconductor excitons in a quantum dot gives rise to atomlike behavior. The full benefit of such a structure is best obsd. in resonant excitation where the excited state can be deterministically populated and coherently manipulated. Because of the large refractive index and device geometry it remains challenging to observe resonantly excited emission that is free from laser scattering in III/V self-assembled quantum dots. Here we exploit the biexciton binding energy to create an extremely clean single photon source via two-photon resonant excitation of an InAs/GaAs quantum dot. We observe complete suppression of the excitation laser and multiphoton emissions. Addnl., we perform full coherent control of the ground-biexciton state qubit and observe an extended coherence time using an all-optical echo technique. The deterministic coherent photon pair creation makes this system suitable for the generation of time-bin entanglement and expts. on the interaction of photons from dissimilar sources.
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    Münzberg, J.; Draxl, F.; da Silva, S. F. C.; Karli, Y.; Manna, S.; Rastelli, A.; Weihs, G.; Keil, R. Fast and efficient demultiplexing of single photons from a quantum dot with resonantly enhanced electro-optic modulators. APL Photonics 2022, 2203, 08682,  DOI: 10.1063/5.0091867
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    Ramsay, A. J.; Gopal, A. V.; Gauger, E. M.; Nazir, A.; Lovett, B. W.; Fox, A. M.; Skolnick, M. S. Damping of exciton Rabi rotations by acoustic phonons in optically excited InGaAs/GaAs quantum dots. Phys. Rev. Lett. 2010, 104, 17402,  DOI: 10.1103/PhysRevLett.104.017402
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    Damping of exciton Rabi rotations by acoustic phonons in optically excited InGaAs/GaAs quantum dots
    Ramsay, A. J.; Gopal, Achanta Venu; Gauger, E. M.; Nazir, A.; Lovett, B. W.; Fox, A. M.; Skolnick, M. S.
    Physical Review Letters (2010), 104 (1), 017402/1-017402/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
    Exptl. evidence identifying acoustic phonons as the principal source of the excitation-induced-dephasing (EID) responsible for the intensity damping of quantum dot excitonic Rabi rotations is reported. The rate of EID is extd. from temp. dependent Rabi rotation measurements of the ground-state excitonic transition, and is in close quant. agreement with an acoustic-phonon model.
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    He, Y.-M.; He, Y.; Wei, Y.-J.; Wu, D.; Atatüre, M.; Schneider, C.; Höfling, S.; Kamp, M.; Lu, C.-Y.; Pan, J.-W. On-demand semiconductor single-photon source with near-unity indistinguishability. Nat. Nanotechnol. 2013, 8, 213,  DOI: 10.1038/nnano.2012.262
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    On-demand semiconductor single-photon source with near-unity indistinguishability
    He, Yu-Ming; He, Yu; Wei, Yu-Jia; Wu, Dian; Atatuere, Mete; Schneider, Christian; Hoefling, Sven; Kamp, Martin; Lu, Chao-Yang; Pan, Jian-Wei
    Nature Nanotechnology (2013), 8 (3), 213-217CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)
    Single-photon sources based on semiconductor quantum dots offer distinct advantages for quantum information, including a scalable solid-state platform, ultrabrightness and interconnectivity with matter qubits. A key prerequisite for their use in optical quantum computing and solid-state networks is a high level of efficiency and indistinguishability. Pulsed resonance fluorescence was anticipated as the optimum condition for the deterministic generation of high-quality photons with vanishing effects of dephasing. Here, the authors generate pulsed single photons on demand from a single, microcavity-embedded quantum dot under s-shell excitation with 3 ps laser pulses. The π pulse-excited resonance-fluorescence photons have <0.3% background contribution and a vanishing 2-photon emission probability. Nonpostselective Hong-Ou-Mandel interference between 2 successively emitted photons is obsd. with a visibility of 0.97(2), comparable to trapped atoms and ions. Two single photons are further used to implement a high-fidelity quantum controlled-NOT gate.
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    Mathew, R.; Dilcher, E.; Gamouras, A.; Ramachandran, A.; Yang, H. Y. S.; Freisem, S.; Deppe, D.; Hall, K. C. Subpicosecond adiabatic rapid passage on a single semiconductor quantum dot: Phonon-mediated dephasing in the strong-driving regime. Phys. Rev. B 2014, 90, 35316,  DOI: 10.1103/PhysRevB.90.035316
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    Subpicosecond adiabatic rapid passage on a single semiconductor quantum dot: phonon-mediated dephasing in the strong-driving regime
    Mathew, Reuble; Dilcher, Eric; Gamouras, Angela; Ramachandran, Ajan; Yang, Hong Yi Shi; Freisem, Sabine; Deppe, Dennis; Hall, Kimberley C.
    Physical Review B: Condensed Matter and Materials Physics (2014), 90 (3), 035316CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
    We demonstrate adiabatic rapid passage on a subpicosecond time scale in a single semiconductor quantum dot, enabling the exploration of a regime of strong (and rapidly varying) Rabi energies for optical control of excitons. An obsd. dependence of the exciton inversion efficiency on the sign of the pulse chirp demonstrates the dominance of phonon-mediated dephasing, which is suppressed for pos. chirp at low temp. Our findings will support the realization of dynamical decoupling strategies and suggest that multiphonon emission and/or non-Markovian effects should be taken into account.
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    Wei, Y. J.; He, Y. M.; Chen, M. C.; Hu, Y. N.; He, Y.; Wu, D.; Schneider, C.; Kamp, M.; Höfling, S.; Lu, C. Y.; Pan, J. W. Deterministic and robust generation of single photons from a single quantum dot with 99.5% indistinguishability using adiabatic rapid passage. Nano Lett. 2014, 14, 6515– 6519,  DOI: 10.1021/nl503081n
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    Deterministic and Robust Generation of Single Photons from a Single Quantum Dot with 99.5% Indistinguishability Using Adiabatic Rapid Passage
    Wei, Yu-Jia; He, Yu-Ming; Chen, Ming-Cheng; Hu, Yi-Nan; He, Yu; Wu, Dian; Schneider, Christian; Kamp, Martin; Hofling, Sven; Lu, Chao-Yang; Pan, Jian-Wei
    Nano Letters (2014), 14 (11), 6515-6519CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
    Single photons are attractive candidates of quantum bits (qubits) for quantum computation and are the best messengers in quantum networks. Future scalable, fault-tolerant photonic quantum technologies demand both stringently high levels of photon indistinguishability and generation efficiency. Here, the authors demonstrate deterministic and robust generation of pulsed resonance fluorescence single photons from a single semiconductor quantum dot using adiabatic rapid passage, a method robust against fluctuation of driving pulse area and dipole moments of solid-state emitters. The emitted photons are background-free, have a vanishing 2-photon emission probability of 0.3% and a raw (cor.) 2-photon Hong-Ou-Mandel interference visibility of 97.9% (99.5%), reaching a precision that places single photons at the threshold for fault-tolerant surface-code quantum computing. This single-photon source can be readily scaled up to multiphoton entanglement and used for quantum metrol., boson sampling, and linear optical quantum computing.
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    Debnath, A.; Meier, C.; Chatel, B.; Amand, T. High-fidelity biexciton generation in quantum dots by chirped laser pulses. Phys. Rev. B 2013, 88, 201305,  DOI: 10.1103/PhysRevB.88.201305
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    High-fidelity biexciton generation in quantum dots by chirped laser pulses
    Debnath, A.; Meier, C.; Chatel, B.; Amand, T.
    Physical Review B: Condensed Matter and Materials Physics (2013), 88 (20), 201305/1-201305/5CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
    We present a detailed theor. anal. of biexciton state generation in InAs-GaAs quantum dots by strong, chirped laser pulses. Specifically, we derive an accurate anal. expression, which not only provides a clear phys. picture of the process, but also allows identifications of laser parameter regimes where efficient biexciton generation should be possible, even at temps. ≤80 K. The results are confirmed by numerical simulations, in very good agreement with the model proposed. A clear choice of parameters is proposed, which might pave the way towards the optimal design of high-fidelity sources of entangled photon pairs based on individual quantum dots.
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    Kaldewey, T.; Lüker, S.; Kuhlmann, A. V.; Valentin, S. R.; Ludwig, A.; Wieck, A. D.; Reiter, D. E.; Kuhn, T.; Warburton, R. J. Coherent and robust high-fidelity generation of a biexciton in a quantum dot by rapid adiabatic passage. Phys. Rev. B 2017, 95, 161302  DOI: 10.1103/PhysRevB.95.161302
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    Coherent and robust high-fidelity generation of a biexciton in a quantum dot by rapid adiabatic passage
    Kaldewey, Timo; Lueker, Sebastian; Kuhlmann, Andreas V.; Valentin, Sascha R.; Ludwig, Arne; Wieck, Andreas D.; Reiter, Doris E.; Kuhn, Tilmann; Warburton, Richard J.
    Physical Review B (2017), 95 (16), 161302/1-161302/5CODEN: PRBHB7; ISSN:2469-9969. (American Physical Society)
    Abiexciton in a semiconductor quantum dot is a source of polarization-entangled photons with high potential for implementation in scalable systems. Several approaches for nonresonant, resonant, and quasiresonant biexciton prepn. exist, but all have their own disadvantages; for instance, low fidelity, timing jitter, incoherence, or sensitivity to exptl. parameters. We demonstrate a coherent and robust technique to generate a biexciton in an InGaAs quantum dot with a fidelity close to 1. The main concept is the application of rapid adiabatic passage to the ground-state-exciton-biexciton system. We reinforce our exptl. results with simulations which include a microscopic coupling to phonons.
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    Wilbur, G.; Binai-Motlagh, A.; Clarke, A.; Ramachandran, A.; Milson, N.; Healey, J.; O’Neal, S.; Deppe, D.; Hall, K. Spectrally-modified frequency-swept pulses for optically-driven quantum light sources. 2022, 2203.01385, arXiv(Quantum Physics), https://arxiv.org/abs/2203.01385, (accessed March 02, 2022).
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    Peiris, M.; Konthasinghe, K.; Yu, Y.; Niu, Z. C.; Muller, A. Bichromatic resonant light scattering from a quantum dot. Phys. Rev. B 2014, 89, 155305,  DOI: 10.1103/PhysRevB.89.155305
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    Bichromatic resonant light scattering from a quantum dot
    Peiris, M.; Konthasinghe, K.; Yu, Y.; Niu, Z. C.; Muller, A.
    Physical Review B: Condensed Matter and Materials Physics (2014), 89 (15), 155305/1-155305/6CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
    We report on resonant light scattering expts. in which a single InAs quantum dot is exposed to two independently tunable continuous-wave lasers while the scattered light is analyzed background free, with high spectral and temporal resoln. In contrast to the well-known monochromatic case exhibiting Rabi oscillations, in this bichromatic case the addnl. field introduces oscillations at half the difference of the laser frequencies and harmonics thereof, persisting beyond the natural lifetime. The familiar "dressed-states" ladder now contains an infinite no. of levels per manifold. With suitable averaging, the rich resulting spectra and second-order correlations can be reproduced accurately using the Bloch equations and the quantum regression theorem.
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    Sbresny, F.; Hanschke, L.; Schöll, E.; Rauhaus, W.; Scaparra, B.; Boos, K.; Casalengua, E. Z.; Riedl, H.; Del Valle, E.; Finley, J. J. Stimulated generation of indistinguishable single photons from a quantum ladder system. Phys. Rev. Lett. 2022, 128, 093603,  DOI: 10.1103/PhysRevLett.128.093603
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    Stimulated Generation of Indistinguishable Single Photons from a Quantum Ladder System
    Sbresny, Friedrich; Hanschke, Lukas; Schoell, Eva; Rauhaus, William; Scaparra, Bianca; Boos, Katarina; Zubizarreta Casalengua, Eduardo; Riedl, Hubert; del Valle, Elena; Finley, Jonathan J.; Joens, Klaus D.; Mueller, Kai
    Physical Review Letters (2022), 128 (9), 093603CODEN: PRLTAO; ISSN:1079-7114. (American Physical Society)
    We propose a scheme for the generation of highly indistinguishable single photons using semiconductor quantum dots and demonstrate its performance and potential. The scheme is based on the resonant two-photon excitation of the biexciton followed by stimulation of the biexciton to selectively prep. an exciton. Quantum-optical simulations and expts. are in good agreement and show that the scheme provides significant advantages over previously demonstrated excitation methods. The two-photon excitation of the biexciton suppresses re-excitation and enables ultralow multiphoton errors, while the precisely timed stimulation pulse results in very low timing jitter of the photons, and consequently, high indistinguishability. In addn., the polarization of the stimulation pulse allows us to deterministically program the polarization of the emitted photon (H or V). This ensures that all emission of interest occurs in the polarization of the detection channel, resulting in higher brightness than cross-polarized resonant excitation.
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    Wei, Y.; Liu, S.; Li, X.; Yu, Y.; Su, X.; Li, S.; Shang, X.; Liu, H.; Hao, H.; Ni, H.; Yu, S.; Niu, Z.; Iles-Smith, J.; Liu, J.; Wang, X. Tailoring solid-state single-photon sources with stimulated emissions. Nat. Nanotechnol. 2022, 17, 470– 476,  DOI: 10.1038/s41565-022-01092-6
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    Tailoring solid-state single-photon sources with stimulated emissions
    Wei, Yuming; Liu, Shunfa; Li, Xueshi; Yu, Ying; Su, Xiangbin; Li, Shulun; Shang, Xiangjun; Liu, Hanqing; Hao, Huiming; Ni, Haiqiao; Yu, Siyuan; Niu, Zhichuan; Iles-Smith, Jake; Liu, Jin; Wang, Xuehua
    Nature Nanotechnology (2022), 17 (5), 470-476CODEN: NNAABX; ISSN:1748-3387. (Nature Portfolio)
    The coherent interaction of electromagnetic fields with solid-state two-level systems can yield deterministic quantum light sources for photonic quantum technologies. To date, the performance of semiconductor single-photon sources based on three-level systems is limited mainly due to a lack of high photon indistinguishability. Here we tailor the cavity-enhanced spontaneous emission from a ladder-type three-level system in a single epitaxial quantum dot through stimulated emission. After populating the biexciton (XX) of the quantum dot through two-photon resonant excitation, we use another laser pulse to selectively depopulate the XX state into an exciton (X) state with a predefined polarization. The stimulated XX-X emission modifies the X decay dynamics and improves the characteristics of a polarized single-photon source, such as a source brightness of 0.030(2), a single-photon purity of 0.998(1) and an indistinguishability of 0.926(4). Our method can be readily applied to existing quantum dot single-photon sources and expands the capabilities of three-level systems for advanced quantum photonic functionalities.
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    Yan, J.; Liu, S.; Lin, X.; Ye, Y.; Yu, J.; Wang, L.; Yu, Y.; Zhao, Y.; Meng, Y.; Hu, X. Double-pulse generation of indistinguishable single photons with optically controlled polarization. Nano Lett. 2022, 22, 1483– 1490,  DOI: 10.1021/acs.nanolett.1c03543
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    Double-Pulse Generation of Indistinguishable Single Photons with Optically Controlled Polarization
    Yan, Junyong; Liu, Shunfa; Lin, Xing; Ye, Yongzheng; Yu, Jiawang; Wang, Lingfang; Yu, Ying; Zhao, Yanhui; Meng, Yun; Hu, Xiaolong; Wang, Da-Wei; Jin, Chaoyuan; Liu, Feng
    Nano Letters (2022), 22 (4), 1483-1490CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
    Single-photon sources play a key role in photonic quantum technologies. Semiconductor quantum dots can emit indistinguishable single photons under resonant excitation. However, the resonance fluorescence technique typically requires cross-polarization filtering, which causes a loss of the unpolarized quantum dot emission by 50%. To solve this problem, we demonstrate a method for generating indistinguishable single photons with optically controlled polarization by two laser pulses off-resonant with neutral exciton states. This scheme is realized by exciting the quantum dot to the biexciton state and subsequently driving the quantum dot to an exciton eigenstate. By combining with a magnetic field, we demonstrated the generation of photons with optically controlled polarization (the degree of polarization is 101(2)%), laser-neutral exciton detuning up to 0.81 meV, high single-photon purity (99.6(1)%), and indistinguishability (85(4)%). Laser pulses can be blocked using polarization and spectral filtering. Our work makes an important step toward indistinguishable single-photon sources with near-unity collection efficiency.
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Cited By

This article is cited by 2 publications.

  1. Thomas K. Bracht, Tim Seidelmann, Yusuf Karli, Florian Kappe, Vikas Remesh, Gregor Weihs, Vollrath Martin Axt, Doris E. Reiter. Dressed-state analysis of two-color excitation schemes. Physical Review B 2023, 107 (3) https://doi.org/10.1103/PhysRevB.107.035425
  2. Benedek Gaál, Martin Arentoft Jacobsen, Luca Vannucci, Julien Claudon, Jean-Michel Gérard, Niels Gregersen. Near-unity efficiency and photon indistinguishability for the “hourglass” single-photon source using suppression of the background emission. Applied Physics Letters 2022, 121 (17) , 170501. https://doi.org/10.1063/5.0107624
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  • Abstract

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    Figure 1

    Figure 1. Concept of SUPER scheme: (a) Spectrum of the broadband excitation pulse (red dashed curve) and an exemplary pulse pair (blue solid curve) after spectral shaping with transmissivities I1 = 0.5 and I2 = 0.96 at detunings Δ1 = −4.9 meV and Δ2 = −11.12 meV. Black arrow denotes the position of the targeted exciton state. (b) Calculated dynamics of the exciton population using the shaped spectrum. Inset shows the energy level scheme with detunings. |g⟩ , ground state, |x⟩, exciton state.

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    Figure 2

    Figure 2. Sketch of the experimental setup: The laser beam is guided to a folded 4f pulse shaper equipped with a spatial light modulator (SLM) for amplitude-shaping the broadband spectrum (gray shade, inset). Incoming and outgoing beams are shown as separate paths for clarity. The shaped pulse-pair is directed with a beam splitter (BS) to the cryostat that holds the quantum dot at 8 K. Emitted photons from the quantum dot are sent through a bandpass filter (BPF) and a notch filter (NF) to either the spectrometer or with an additional fiber beam splitter (FBS) to the superconducting nanowire single-photon detectors (SNSPD) to record the photon coincidences. On the basis of above-band excitation, the quantum dot exciton emission line (X, green) is identified. An exemplary pulse-pair with detunings Δ1 (orange) and Δ2 (red) is also shown.

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    Figure 3

    Figure 3. Exciton population achieved by the SUPER scheme: (a) Measured photon counts at exciton emission energy as a function of the detuning Δ2 and the transmissivity I2 of the second pulse. The first pulse is fixed to Δ1 = −4.9 meV and I1 = 0.5. The scale shows the integrated exciton counts after correcting for background. The red dot indicates the parameters used in the photon quality experiment (Figure 4). (b) Theoretically calculated exciton (X) population based on a two-level system. (c) Vertical line-cuts through the 2D map for Δ2 = −10.5 meV (blue), –10.6 meV (red), and −10.9 meV (green). The dashed red line indicates the parameters at which the photon quality measurements are performed.

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    Figure 4

    Figure 4. Scope of SUPER scheme: (a) Measured photon counts at the exciton-emission energy (red crosses) under SUPER excitation in contrast to resonant TPE (blue circles). The x-axes values show corresponding power measured with a 1% beam sampler near the cryostat window. (b) Quantum dot emission spectra under TPE (top panel) and SUPER excitation (bottom panel). The TPE emission spectrum shows residual laser scattering and the SUPER emission spectrum shows the first detuned pulse. (c) Single photon characteristics under SUPER excitation as shown by g(2)(0) = 0.06(1). The dark green dots show the measured data, while the orange curves denote the fit.

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  • References

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      Bright solid-state sources of indistinguishable single photons
      Gazzano O; Michaelis de Vasconcellos S; Arnold C; Nowak A; Galopin E; Sagnes I; Lanco L; Lemaitre A; Senellart P
      Nature communications (2013), 4 (), 1425 ISSN:.
      Bright sources of indistinguishable single photons are strongly needed for the scalability of quantum information processing. Semiconductor quantum dots are promising systems to build such sources. Several works demonstrated emission of indistinguishable photons while others proposed various approaches to efficiently collect them. Here we combine both properties and report on the fabrication of ultrabright sources of indistinguishable single photons, thanks to deterministic positioning of single quantum dots in well-designed pillar cavities. Brightness as high as 0.79±0.08 collected photon per pulse is demonstrated. The indistinguishability of the photons is investigated as a function of the source brightness and the excitation conditions. We show that a two-laser excitation scheme allows reducing the fluctuations of the quantum dot electrostatic environment under high pumping conditions. With this method, we obtain 82±10% indistinguishability for a brightness as large as 0.65±0.06 collected photon per pulse.
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    12. 12
      Ding, X.; He, Y.; Duan, Z. C.; Gregersen, N.; Chen, M. C.; Unsleber, S.; Maier, S.; Schneider, C.; Kamp, M.; Höfling, S.; Lu, C. Y.; Pan, J. W. On-Demand Single Photons with High Extraction Efficiency and Near-Unity Indistinguishability from a Resonantly Driven Quantum Dot in a Micropillar. Phys. Rev. Lett. 2016, 116, 20401,  DOI: 10.1103/PhysRevLett.116.020401
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      12
      On-Demand Single Photons with High Extraction Efficiency and Near-Unity Indistinguishability from a Resonantly Driven Quantum Dot in a Micropillar
      Ding Xing; He Yu; Duan Z-C; Chen M-C; Hofling Sven; Lu Chao-Yang; Pan Jian-Wei; Ding Xing; He Yu; Duan Z-C; Chen M-C; Lu Chao-Yang; Pan Jian-Wei; Ding Xing; He Yu; Duan Z-C; Chen M-C; Lu Chao-Yang; Pan Jian-Wei; Gregersen Niels; Unsleber S; Maier S; Schneider Christian; Kamp Martin; Hofling Sven; Hofling Sven
      Physical review letters (2016), 116 (2), 020401 ISSN:.
      Scalable photonic quantum technologies require on-demand single-photon sources with simultaneously high levels of purity, indistinguishability, and efficiency. These key features, however, have only been demonstrated separately in previous experiments. Here, by s-shell pulsed resonant excitation of a Purcell-enhanced quantum dot-micropillar system, we deterministically generate resonance fluorescence single photons which, at π pulse excitation, have an extraction efficiency of 66%, single-photon purity of 99.1%, and photon indistinguishability of 98.5%. Such a single-photon source for the first time combines the features of high efficiency and near-perfect levels of purity and indistinguishabilty, and thus opens the way to multiphoton experiments with semiconductor quantum dots.
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      Senellart, P.; Solomon, G.; White, A. High-performance semiconductor quantum-dot single-photon sources. Nat. Nanotechnol. 2017, 12, 1026– 1039,  DOI: 10.1038/nnano.2017.218
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      13
      High-performance semiconductor quantum-dot single-photon sources
      Senellart, Pascale; Solomon, Glenn; White, Andrew
      Nature Nanotechnology (2017), 12 (11), 1026-1039CODEN: NNAABX; ISSN:1748-3387. (Nature Research)
      A review. Single photons are a fundamental element of most quantum optical technologies. The ideal single-photon source is an on-demand, deterministic, single-photon source delivering light pulses in a well-defined polarization and spatiotemporal mode, and contg. exactly one photon. In addn., for many applications, there is a quantum advantage if the single photons are indistinguishable in all their degrees of freedom. Single-photon sources based on parametric down-conversion are currently used, and while excellent in many ways, scaling to large quantum optical systems remains challenging. In 2000, semiconductor quantum dots were shown to emit single photons, opening a path towards integrated single-photon sources. Here, we review the progress achieved in the past few years, and discuss remaining challenges. The latest quantum dot-based single-photon sources are edging closer to the ideal single-photon source, and have opened new possibilities for quantum technologies.
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    14. 14
      Schweickert, L.; Jöns, K. D.; Zeuner, K. D.; Covre Da Silva, S. F.; Huang, H.; Lettner, T.; Reindl, M.; Zichi, J.; Trotta, R.; Rastelli, A.; Zwiller, V. On-demand generation of background-free single photons from a solid-state source. Appl. Phys. Lett. 2018, 112, 093106,  DOI: 10.1063/1.5020038
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      On-demand generation of background-free single photons from a solid-state source
      Schweickert, Lucas; Joens, Klaus D.; Zeuner, Katharina D.; Covre da Silva, Saimon Filipe; Huang, Huiying; Lettner, Thomas; Reindl, Marcus; Zichi, Julien; Trotta, Rinaldo; Rastelli, Armando; Zwiller, Val
      Applied Physics Letters (2018), 112 (9), 093106/1-093106/4CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
      True on-demand high-repetition-rate single-photon sources are highly sought after for quantum information processing applications. Any coherently driven 2-level quantum system suffers from a finite reexcitation probability under pulsed excitation, causing undesirable multi-photon emission. A solid-state source of on-demand single photons yielding a raw 2nd-order coherence of g(2)(0) = (7.5 ± 1.6) × 10-5 without any background subtraction or data processing is presented. To this date, this is the lowest value of g(2)(0) reported for any single-photon source even compared to the previously reported best background subtracted values. This result was achieved on GaAs/AlGaAs quantum dots embedded in a low-Q planar cavity by using (i) a 2-photon excitation process and (ii) a filtering and detection setup featuring 2 superconducting single-photon detectors with ultralow dark-count rates of (0.0056 ± 0.0007) s-1 and (0.017 ± 0.001) s-1, resp. Reexcitation processes are dramatically suppressed by (i), while (ii) removes false coincidences resulting in a negligibly low noise floor. (c) 2018 American Institute of Physics.
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      Rodt, S.; Reitzenstein, S.; Heindel, T. Deterministically fabricated solid-state quantum-light sources. J. Phys.: Condens. Matter 2020, 32, 153003,  DOI: 10.1088/1361-648X/ab5e15
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      15
      Deterministically fabricated solid-state quantum-light sources
      Rodt, Sven; Reitzenstein, Stephan; Heindel, Tobias
      Journal of Physics: Condensed Matter (2020), 32 (15), 153003CODEN: JCOMEL; ISSN:0953-8984. (IOP Publishing Ltd.)
      A review. The controlled generation of non-classical states of light is a challenging task at the heart of quantum optics. Aside from the mere spirit of science, the related research is strongly driven by applications in photonic quantum technologies, including the fields of quantum communication, quantum computation, and quantum metrol. In this context, the realization of integrated solid-state-based quantum-light sources is of particular interest, due to the prospects for scalability and device integration. This topical review focuses on solid-state quantum-light sources which are fabricated in a deterministic fashion. In this framework we cover quantum emitters represented by semiconductor quantum dots, color centers in diamond, and defect-/strain-centers in two-dimensional materials. First, we introduce the topic of quantum-light sources and non-classical light generation for applications in photonic quantum technologies, motivating the need for the development of scalable device technologies to push the field towards real-world applications. In the second part, we summarize material systems hosting quantum emitters in the solid-state. The third part reviews deterministic fabrication techniques and comparatively discusses their advantages and disadvantages. The techniques are classified in bottom-up approaches, exploiting the site-controlled positioning of the quantum emitters themselves, and top-down approaches, allowing for the precise alignment of photonic microstructures to pre-selected quantum emitters. Special emphasis is put on the progress achieved in the development of in situ techniques, which significantly pushed the performance of quantum-light sources towards applications. Addnl., we discuss hybrid approaches, exploiting pick-and-place techniques or wafer-bonding. The fourth part presents state-of-the-art quantum-dot quantum-light sources based on the fabrication techniques presented in the previous sections, which feature engineered functionality and enhanced photon collection efficiency. The article closes by highlighting recent applications of deterministic solid-state-based quantum-light sources in the fields of quantum communication, quantum computing, and quantum metrol., and by discussing future perspectives in the field of solid-state quantum-light sources.
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    16. 16
      Srocka, N.; Mrowiński, P.; Große, J.; von Helversen, M.; Heindel, T.; Rodt, S.; Reitzenstein, S. Deterministically fabricated quantum dot single-photon source emitting indistinguishable photons in the telecom O-band. Appl. Phys. Lett. 2020, 116, 231104,  DOI: 10.1063/5.0010436
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      Deterministically fabricated quantum dot single-photon source emitting indistinguishable photons in the telecom O-band
      Srocka, N.; Mrowinski, P.; Grosse, J.; von Helversen, M.; Heindel, T.; Rodt, S.; Reitzenstein, S.
      Applied Physics Letters (2020), 116 (23), 231104CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
      The authors develop and study single-photon sources based on InGaAs quantum dots (QDs) emitting in the telecom O-band. Quantum devices are fabricated using in situ electron beam lithog. in combination with thermocompression bonding to realize a backside Au mirror. The structures are based on InGaAs/GaAs heterostructures, where the QD emission is red shifted toward the telecom O-band at 1.3μm via a strain-reducing layer. QDs pre-selected by cathodoluminescence mapping are embedded into mesa structures with a backside Au mirror for enhanced photon-extn. efficiency. Photon-autocorrelation measurements under pulsed nonresonant wetting-layer excitation are performed at temps. up to 40 K, showing pure single-photon emission, which makes the devices compatible with stand-alone operation using Stirling cryocoolers. Using pulsed p-shell excitation, the authors realize single-photon emission with a high multi-photon suppression of g(2)(0) = 0.027 ± 0.005, an as-measured 2-photon interference visibility of (12 ± 4)%, a post-selected visibility of (96 ± 10)%, and an assocd. coherence time of (212 ± 25) ps. Also, the structures show an extn. efficiency of ∼5%, which is comparable to values expected from numeric simulations of this photonic structure. Further improvements of the devices will enable implementations of quantum communication via optical fibers. (c) 2020 American Institute of Physics.
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      Wang, B. Y.; Denning, E. V.; Gür, U. M.; Lu, C. Y.; Gregersen, N. Micropillar single-photon source design for simultaneous near-unity efficiency and indistinguishability. Phys. Rev. B 2020, 102, 125301,  DOI: 10.1103/PhysRevB.102.125301
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      Micropillar single-photon source design for simultaneous near-unity efficiency and indistinguishability
      Wang, Bi-Ying; Denning, Emil V.; Gur, Ugur Meric; Lu, Chao-Yang; Gregersen, Niels
      Physical Review B (2020), 102 (12), 125301CODEN: PRBHB7; ISSN:2469-9969. (American Physical Society)
      We present a numerical investigation of the performance of the micropillar cavity single-photon source in terms of collection efficiency and indistinguishability of the emitted photons in the presence of non-Markovian phonon-induced decoherence. We analyze the physics governing the efficiency using a single-mode model, and we optimize efficiency ε and the indistinguishability η on an equal footing by computing εη as function of the micropillar design parameters. We show that εη is limited to ~ 0.96 for the ideal geometry due to an inherent tradeoff between efficiency and indistinguishability. Finally, we subsequently consider the influence of realistic fabrication imperfections and Markovian pure dephasing noise on the performance.
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      Tomm, N.; Javadi, A.; Antoniadis, N. O.; Najer, D.; Löbl, M. C.; Korsch, A. R.; Schott, R.; Valentin, S. R.; Wieck, A. D.; Ludwig, A.; Warburton, R. J. A bright and fast source of coherent single photons. Nat. Nanotechnol. 2021, 16, 399– 403,  DOI: 10.1038/s41565-020-00831-x
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      18
      A bright and fast source of coherent single photons
      Tomm, Natasha; Javadi, Alisa; Antoniadis, Nadia Olympia; Najer, Daniel; Lobl, Matthias Christian; Korsch, Alexander Rolf; Schott, Rudiger; Valentin, Sascha Rene; Wieck, Andreas Dirk; Ludwig, Arne; Warburton, Richard John
      Nature Nanotechnology (2021), 16 (4), 399-403CODEN: NNAABX; ISSN:1748-3387. (Nature Portfolio)
      A single-photon source is an enabling technol. in device-independent quantum communication, quantum simulation, and linear optics-based and measurement-based quantum computing. These applications employ many photons and place stringent requirements on the efficiency of single-photon creation. The scaling on efficiency is typically an exponential function of the no. of photons. Schemes taking full advantage of quantum superpositions also depend sensitively on the coherence of the photons, i.e., their indistinguishability. Here, we report a single-photon source with a high end-to-end efficiency. We employ gated quantum dots in an open, tunable microcavity. The gating provides control of the charge and elec. tuning of the emission frequency; the high-quality material ensures low noise; and the tunability of the microcavity compensates for the lack of control in quantum dot position and emission frequency. Transmission through the top mirror is the dominant escape route for photons from the microcavity, and this output is well matched to a single-mode fiber. With this design, we can create a single photon at the output of the final optical fiber on-demand with a probability of up to 57% and with an av. two-photon interference visibility of 97.5%. Coherence persists in trains of thousands of photons with single-photon creation at a repetition rate of 1 GHz.
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      Thomas, S. E. Bright Polarized Single-Photon Source Based on a Linear Dipole. Phys. Rev. Lett. 2021, 126, 233601,  DOI: 10.1103/PhysRevLett.126.233601
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      Bright Polarized Single-Photon Source Based on a Linear Dipole
      Thomas, S. E.; Billard, M.; Coste, N.; Wein, S. C.; Priya; Ollivier, H.; Krebs, O.; Tazairt, L.; Harouri, A.; Lemaitre, A.; Sagnes, I.; Anton, C.; Lanco, L.; Somaschi, N.; Loredo, J. C.; Senellart, P.
      Physical Review Letters (2021), 126 (23), 233601CODEN: PRLTAO; ISSN:1079-7114. (American Physical Society)
      Semiconductor quantum dots in cavities are promising single-photon sources. Here, we present a path to deterministic operation, by harnessing the intrinsic linear dipole in a neutral quantum dot via phonon-assisted excitation. This enables emission of fully polarized single photons, with a measured degree of linear polarization up to 0.994±0.007, and high population inversion-85% as high as resonant excitation. We demonstrate a single-photon source with a polarized first lens brightness of 0.50±0.01, a single-photon purity of 0.954±0.001, and single-photon indistinguishability of 0.909±0.004.
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      Lu, C.-Y.; Pan, J.-W. Quantum-dot single-photon sources for the quantum internet. Nat. Nanotechol. 2021, 16, 1294– 1296,  DOI: 10.1038/s41565-021-01033-9
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      Lodahl, P.; Mahmoodian, S.; Stobbe, S. Interfacing single photons and single quantum dots with photonic nanostructures. Rev. Mod. Phys. 2015, 87, 347– 400,  DOI: 10.1103/RevModPhys.87.347
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      Interfacing single photons and single quantum dots with photonic nanostructures
      Lodahl, Peter; Mahmoodian, Sahand; Stobbe, Soren
      Reviews of Modern Physics (2015), 87 (2), 347-400CODEN: RMPHAT; ISSN:0034-6861. (American Physical Society)
      Photonic nanostructures provide a means of tailoring the interaction between light and matter and the past decade has witnessed tremendous exptl. and theor. progress on this subject. In particular, the combination with semiconductor quantum dots has proven successful. This manuscript reviews quantum optics with excitons in single quantum dots embedded in photonic nanostructures. The ability to engineer the light-matter interaction strength in integrated photonic nanostructures enables a range of fundamental quantum-electrodynamics expts. on, e.g.. spontaneous- emission control, modified Lamb shifts, and enhanced dipole-dipole interaction. Furthermore, highly efficient single-photon sources and giant photon nonlinearities may be implemented with immediate applications for photonic quantum-information processing. This review summarizes the general theor. framework of photon emission including the role of dephasing processes and applies it to photonic nanostructures of current interest, such as photonic-crystal cavities and waveguides, dielec. nanowires, and plasmonic waveguides. The introduced concepts are generally applicable in quantum nanophotonics and apply to a large extent also to other quantum emitters, such as mols., nitrogen vacancy centers, or atoms. Finally, the progress and future prospects of applications in quantum-information processing are considered.
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      Dusanowski, Ł.; Köck, D.; Shin, E.; Kwon, S. H.; Schneider, C.; Höfling, S. Purcell-Enhanced and Indistinguishable Single-Photon Generation from Quantum Dots Coupled to On-Chip Integrated Ring Resonators. Nano Lett. 2020, 20, 6357– 6363,  DOI: 10.1021/acs.nanolett.0c01771
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      Purcell-Enhanced and Indistinguishable Single-Photon Generation from Quantum Dots Coupled to On-Chip Integrated Ring Resonators
      Dusanowski, Lukasz; Koeck, Dominik; Shin, Eunso; Kwon, Soon-Hong; Schneider, Christian; Hoefling, Sven
      Nano Letters (2020), 20 (9), 6357-6363CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
      Integrated photonic circuits provide a versatile toolbox of functionalities for advanced quantum optics applications. Here, we demonstrate an essential component of such a system in the form of a Purcell-enhanced single-photon source based on a quantum dot coupled to a robust on-chip integrated resonator. For that, we develop GaAs monolithic ring cavities based on distributed Bragg reflector ridge waveguides. Under resonant excitation conditions, we observe an over 2-fold spontaneous emission rate enhancement using Purcell effect and gain a full coherent optical control of a QD-two-level system via Rabi oscillations. Furthermore, we demonstrate an on-demand single-photon generation with strongly suppressed multiphoton emission probability as low as 1% and two-photon interference with visibility up to 95%. This integrated single-photon source can be readily scaled up, promising a realistic pathway for scalable on-chip linear optical quantum simulation, quantum computation, and quantum networks.
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      Uppu, R.; Pedersen, F. T.; Wang, Y.; Olesen, C. T.; Papon, C.; Zhou, X.; Midolo, L.; Scholz, S.; Wieck, A. D.; Ludwig, A.; Lodahl, P. Scalable integrated single-photon source. Sci. Adv. 2020, 6, eabc8268  DOI: 10.1126/sciadv.abc8268
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      Elshaari, A. W.; Pernice, W.; Srinivasan, K.; Benson, O.; Zwiller, V. Hybrid integrated quantum photonic circuits. Nat. Photonics 2020, 14, 285– 298,  DOI: 10.1038/s41566-020-0609-x
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      Hybrid integrated quantum photonic circuits
      Elshaari, Ali W.; Pernice, Wolfram; Srinivasan, Kartik; Benson, Oliver; Zwiller, Val
      Nature Photonics (2020), 14 (5), 285-298CODEN: NPAHBY; ISSN:1749-4885. (Nature Research)
      Abstr.: Recent developments in chip-based photonic quantum circuits have radically impacted quantum information processing. However, it is challenging for monolithic photonic platforms to meet the stringent demands of most quantum applications. Hybrid platforms combining different photonic technologies in a single functional unit have great potential to overcome the limitations of monolithic photonic circuits. Our Review summarizes the progress of hybrid quantum photonics integration, discusses important design considerations, including optical connectivity and operation conditions, and highlights several successful realizations of key phys. resources for building a quantum teleporter. We conclude by discussing the roadmap for realizing future advanced large-scale hybrid devices, beyond the solid-state platform, which hold great potential for quantum information applications.
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      Bounouar, S.; Davanco, M.; Reitzenstein, S. Semicond. Semimet.; Elsevier, 2020; Vol. 105; pp 153– 234.
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      Bracht, T. K.; Seidelmann, T.; Kuhn, T.; Axt, V. M.; Reiter, D. E. Phonon Wave Packet Emission during State Preparation of a Semiconductor Quantum Dot using Different Schemes. Phys. Status Solidi B 2022, 259, 2100649,  DOI: 10.1002/pssb.202100649
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      26
      Phonon Wave Packet Emission during State Preparation of a Semiconductor Quantum Dot using Different Schemes
      Bracht, Thomas K.; Seidelmann, Tim; Kuhn, Tilmann; Axt, Vollrath Martin; Reiter, Doris E.
      Physica Status Solidi B: Basic Solid State Physics (2022), 259 (6), 2100649CODEN: PSSBBD; ISSN:0370-1972. (Wiley-VCH Verlag GmbH & Co. KGaA)
      The carrier-phonon interaction in semiconductor quantum dots (QDs) can greatly affect the optical prepn. of the excited state. For resonant excitation used in the Rabi prepn. scheme, the polaron is formed accompanied by the emission of a phonon wave packet, leading to a degrdn. of prepn. fidelity. In this article, phonon wave packets for different coherent excitation schemes are analyzed. One example is the adiabatic rapid passage scheme relying on a chirped excitation. Herein, also a phonon wave packet is emitted, but the prepn. fidelity can still be approx. unity. A focus is on the phonon impact on a recently proposed swing-up scheme, induced by two detuned pulses. Similar to the Rabi scheme, a degrdn. and a phonon wave packet emission are found, despite the detuning. If the swing-up frequency coincides with the max. of the phonon spectral d., a series of wave packets is emitted yielding an even stronger degrdn. The insight gained from our results further helps in designing an optimal prepn. scheme for QDs.
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      Huber, D.; Reindl, M.; Huo, Y.; Huang, H.; Wildmann, J. S.; Schmidt, O. G.; Rastelli, A.; Trotta, R. Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots. Nat. Commun. 2017, 8, 15506,  DOI: 10.1038/ncomms15506
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      Highly indistinguishable and strongly entangled photons from symmetric GaAs quantum dots
      Huber, Daniel; Reindl, Marcus; Huo, Yongheng; Huang, Huiying; Wildmann, Johannes S.; Schmidt, Oliver G.; Rastelli, Armando; Trotta, Rinaldo
      Nature Communications (2017), 8 (), 15506CODEN: NCAOBW; ISSN:2041-1723. (Nature Publishing Group)
      The development of scalable sources of non-classical light is fundamental to unlocking the technol. potential of quantum photonics. Semiconductor quantum dots are emerging as near-optimal sources of indistinguishable single photons. However, their performance as sources of entangled-photon pairs are still modest compared to parametric down converters. Photons emitted from conventional Stranski-Krastanov InGaAs quantum dots have shown non-optimal levels of entanglement and indistinguishability. For quantum networks, both criteria must be met simultaneously. Here, we show that this is possible with a system that has received limited attention so far: GaAs quantum dots. They can emit triggered polarization-entangled photons with high purity (g(2)(0) = 0.002±0.002), high indistinguishability (0.93±0.07 for 2 ns pulse sepn.) and high entanglement fidelity (0.94±0.01). Our results show that GaAs might be the material of choice for quantum-dot entanglement sources in future quantum technologies.
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      da Silva, S. F. C.; Undeutsch, G.; Lehner, B.; Manna, S.; Krieger, T. M.; Reindl, M.; Schimpf, C.; Trotta, R.; Rastelli, A. GaAs quantum dots grown by droplet etching epitaxy as quantum light sources. Appl. Phys. Lett. 2021, 119, 120502,  DOI: 10.1063/5.0057070
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      GaAs quantum dots grown by droplet etching epitaxy as quantum light sources
      da Silva, Saimon Filipe Covre; Undeutsch, Gabriel; Lehner, Barbara; Manna, Santanu; Krieger, Tobias M.; Reindl, Marcus; Schimpf, Christian; Trotta, Rinaldo; Rastelli, Armando
      Applied Physics Letters (2021), 119 (12), 120502CODEN: APPLAB; ISSN:0003-6951. (American Institute of Physics)
      A review. This Perspective presents an overview on the epitaxial growth and optical properties of GaAs quantum dots obtained with the droplet etching method as high-quality sources of quantum light. We illustrate recent achievements regarding the generation of single photons and polarization entangled photon pairs and the use of these sources in applications of central importance in quantum communication such as entanglement swapping and quantum key distribution. (c) 2021 American Institute of Physics.
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      https://chemport.cas.org/services/resolver?origin=ACS&resolution=options&coi=1%3ACAS%3A528%3ADC%252BB3MXitFaqt7%252FN&md5=eb8808331be56ae65e290dec8765e391
    29. 29
      Jayakumar, H.; Predojević, A.; Huber, T.; Kauten, T.; Solomon, G. S.; Weihs, G. Deterministic photon pairs and coherent optical control of a single quantum dot. Phys. Rev. Lett. 2013, 110, 135505,  DOI: 10.1103/PhysRevLett.110.135505
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      Deterministic photon pairs and coherent optical control of a single quantum dot
      Jayakumar, Harishankar; Predojevic, Ana; Huber, Tobias; Kauten, Thomas; Solomon, Glenn S.; Weihs, Gregor
      Physical Review Letters (2013), 110 (13), 135505/1-135505/5CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
      The strong confinement of semiconductor excitons in a quantum dot gives rise to atomlike behavior. The full benefit of such a structure is best obsd. in resonant excitation where the excited state can be deterministically populated and coherently manipulated. Because of the large refractive index and device geometry it remains challenging to observe resonantly excited emission that is free from laser scattering in III/V self-assembled quantum dots. Here we exploit the biexciton binding energy to create an extremely clean single photon source via two-photon resonant excitation of an InAs/GaAs quantum dot. We observe complete suppression of the excitation laser and multiphoton emissions. Addnl., we perform full coherent control of the ground-biexciton state qubit and observe an extended coherence time using an all-optical echo technique. The deterministic coherent photon pair creation makes this system suitable for the generation of time-bin entanglement and expts. on the interaction of photons from dissimilar sources.
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    30. 30
      Münzberg, J.; Draxl, F.; da Silva, S. F. C.; Karli, Y.; Manna, S.; Rastelli, A.; Weihs, G.; Keil, R. Fast and efficient demultiplexing of single photons from a quantum dot with resonantly enhanced electro-optic modulators. APL Photonics 2022, 2203, 08682,  DOI: 10.1063/5.0091867
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      Ramsay, A. J.; Gopal, A. V.; Gauger, E. M.; Nazir, A.; Lovett, B. W.; Fox, A. M.; Skolnick, M. S. Damping of exciton Rabi rotations by acoustic phonons in optically excited InGaAs/GaAs quantum dots. Phys. Rev. Lett. 2010, 104, 17402,  DOI: 10.1103/PhysRevLett.104.017402
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      31
      Damping of exciton Rabi rotations by acoustic phonons in optically excited InGaAs/GaAs quantum dots
      Ramsay, A. J.; Gopal, Achanta Venu; Gauger, E. M.; Nazir, A.; Lovett, B. W.; Fox, A. M.; Skolnick, M. S.
      Physical Review Letters (2010), 104 (1), 017402/1-017402/4CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
      Exptl. evidence identifying acoustic phonons as the principal source of the excitation-induced-dephasing (EID) responsible for the intensity damping of quantum dot excitonic Rabi rotations is reported. The rate of EID is extd. from temp. dependent Rabi rotation measurements of the ground-state excitonic transition, and is in close quant. agreement with an acoustic-phonon model.
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    32. 32
      He, Y.-M.; He, Y.; Wei, Y.-J.; Wu, D.; Atatüre, M.; Schneider, C.; Höfling, S.; Kamp, M.; Lu, C.-Y.; Pan, J.-W. On-demand semiconductor single-photon source with near-unity indistinguishability. Nat. Nanotechnol. 2013, 8, 213,  DOI: 10.1038/nnano.2012.262
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      On-demand semiconductor single-photon source with near-unity indistinguishability
      He, Yu-Ming; He, Yu; Wei, Yu-Jia; Wu, Dian; Atatuere, Mete; Schneider, Christian; Hoefling, Sven; Kamp, Martin; Lu, Chao-Yang; Pan, Jian-Wei
      Nature Nanotechnology (2013), 8 (3), 213-217CODEN: NNAABX; ISSN:1748-3387. (Nature Publishing Group)
      Single-photon sources based on semiconductor quantum dots offer distinct advantages for quantum information, including a scalable solid-state platform, ultrabrightness and interconnectivity with matter qubits. A key prerequisite for their use in optical quantum computing and solid-state networks is a high level of efficiency and indistinguishability. Pulsed resonance fluorescence was anticipated as the optimum condition for the deterministic generation of high-quality photons with vanishing effects of dephasing. Here, the authors generate pulsed single photons on demand from a single, microcavity-embedded quantum dot under s-shell excitation with 3 ps laser pulses. The π pulse-excited resonance-fluorescence photons have <0.3% background contribution and a vanishing 2-photon emission probability. Nonpostselective Hong-Ou-Mandel interference between 2 successively emitted photons is obsd. with a visibility of 0.97(2), comparable to trapped atoms and ions. Two single photons are further used to implement a high-fidelity quantum controlled-NOT gate.
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    33. 33
      Mathew, R.; Dilcher, E.; Gamouras, A.; Ramachandran, A.; Yang, H. Y. S.; Freisem, S.; Deppe, D.; Hall, K. C. Subpicosecond adiabatic rapid passage on a single semiconductor quantum dot: Phonon-mediated dephasing in the strong-driving regime. Phys. Rev. B 2014, 90, 35316,  DOI: 10.1103/PhysRevB.90.035316
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      Subpicosecond adiabatic rapid passage on a single semiconductor quantum dot: phonon-mediated dephasing in the strong-driving regime
      Mathew, Reuble; Dilcher, Eric; Gamouras, Angela; Ramachandran, Ajan; Yang, Hong Yi Shi; Freisem, Sabine; Deppe, Dennis; Hall, Kimberley C.
      Physical Review B: Condensed Matter and Materials Physics (2014), 90 (3), 035316CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
      We demonstrate adiabatic rapid passage on a subpicosecond time scale in a single semiconductor quantum dot, enabling the exploration of a regime of strong (and rapidly varying) Rabi energies for optical control of excitons. An obsd. dependence of the exciton inversion efficiency on the sign of the pulse chirp demonstrates the dominance of phonon-mediated dephasing, which is suppressed for pos. chirp at low temp. Our findings will support the realization of dynamical decoupling strategies and suggest that multiphonon emission and/or non-Markovian effects should be taken into account.
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    34. 34
      Wei, Y. J.; He, Y. M.; Chen, M. C.; Hu, Y. N.; He, Y.; Wu, D.; Schneider, C.; Kamp, M.; Höfling, S.; Lu, C. Y.; Pan, J. W. Deterministic and robust generation of single photons from a single quantum dot with 99.5% indistinguishability using adiabatic rapid passage. Nano Lett. 2014, 14, 6515– 6519,  DOI: 10.1021/nl503081n
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      34
      Deterministic and Robust Generation of Single Photons from a Single Quantum Dot with 99.5% Indistinguishability Using Adiabatic Rapid Passage
      Wei, Yu-Jia; He, Yu-Ming; Chen, Ming-Cheng; Hu, Yi-Nan; He, Yu; Wu, Dian; Schneider, Christian; Kamp, Martin; Hofling, Sven; Lu, Chao-Yang; Pan, Jian-Wei
      Nano Letters (2014), 14 (11), 6515-6519CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
      Single photons are attractive candidates of quantum bits (qubits) for quantum computation and are the best messengers in quantum networks. Future scalable, fault-tolerant photonic quantum technologies demand both stringently high levels of photon indistinguishability and generation efficiency. Here, the authors demonstrate deterministic and robust generation of pulsed resonance fluorescence single photons from a single semiconductor quantum dot using adiabatic rapid passage, a method robust against fluctuation of driving pulse area and dipole moments of solid-state emitters. The emitted photons are background-free, have a vanishing 2-photon emission probability of 0.3% and a raw (cor.) 2-photon Hong-Ou-Mandel interference visibility of 97.9% (99.5%), reaching a precision that places single photons at the threshold for fault-tolerant surface-code quantum computing. This single-photon source can be readily scaled up to multiphoton entanglement and used for quantum metrol., boson sampling, and linear optical quantum computing.
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      Debnath, A.; Meier, C.; Chatel, B.; Amand, T. High-fidelity biexciton generation in quantum dots by chirped laser pulses. Phys. Rev. B 2013, 88, 201305,  DOI: 10.1103/PhysRevB.88.201305
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      High-fidelity biexciton generation in quantum dots by chirped laser pulses
      Debnath, A.; Meier, C.; Chatel, B.; Amand, T.
      Physical Review B: Condensed Matter and Materials Physics (2013), 88 (20), 201305/1-201305/5CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
      We present a detailed theor. anal. of biexciton state generation in InAs-GaAs quantum dots by strong, chirped laser pulses. Specifically, we derive an accurate anal. expression, which not only provides a clear phys. picture of the process, but also allows identifications of laser parameter regimes where efficient biexciton generation should be possible, even at temps. ≤80 K. The results are confirmed by numerical simulations, in very good agreement with the model proposed. A clear choice of parameters is proposed, which might pave the way towards the optimal design of high-fidelity sources of entangled photon pairs based on individual quantum dots.
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    36. 36
      Kaldewey, T.; Lüker, S.; Kuhlmann, A. V.; Valentin, S. R.; Ludwig, A.; Wieck, A. D.; Reiter, D. E.; Kuhn, T.; Warburton, R. J. Coherent and robust high-fidelity generation of a biexciton in a quantum dot by rapid adiabatic passage. Phys. Rev. B 2017, 95, 161302  DOI: 10.1103/PhysRevB.95.161302
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      36
      Coherent and robust high-fidelity generation of a biexciton in a quantum dot by rapid adiabatic passage
      Kaldewey, Timo; Lueker, Sebastian; Kuhlmann, Andreas V.; Valentin, Sascha R.; Ludwig, Arne; Wieck, Andreas D.; Reiter, Doris E.; Kuhn, Tilmann; Warburton, Richard J.
      Physical Review B (2017), 95 (16), 161302/1-161302/5CODEN: PRBHB7; ISSN:2469-9969. (American Physical Society)
      Abiexciton in a semiconductor quantum dot is a source of polarization-entangled photons with high potential for implementation in scalable systems. Several approaches for nonresonant, resonant, and quasiresonant biexciton prepn. exist, but all have their own disadvantages; for instance, low fidelity, timing jitter, incoherence, or sensitivity to exptl. parameters. We demonstrate a coherent and robust technique to generate a biexciton in an InGaAs quantum dot with a fidelity close to 1. The main concept is the application of rapid adiabatic passage to the ground-state-exciton-biexciton system. We reinforce our exptl. results with simulations which include a microscopic coupling to phonons.
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    37. 37
      Wilbur, G.; Binai-Motlagh, A.; Clarke, A.; Ramachandran, A.; Milson, N.; Healey, J.; O’Neal, S.; Deppe, D.; Hall, K. Spectrally-modified frequency-swept pulses for optically-driven quantum light sources. 2022, 2203.01385, arXiv(Quantum Physics), https://arxiv.org/abs/2203.01385, (accessed March 02, 2022).
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      Peiris, M.; Konthasinghe, K.; Yu, Y.; Niu, Z. C.; Muller, A. Bichromatic resonant light scattering from a quantum dot. Phys. Rev. B 2014, 89, 155305,  DOI: 10.1103/PhysRevB.89.155305
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      Bichromatic resonant light scattering from a quantum dot
      Peiris, M.; Konthasinghe, K.; Yu, Y.; Niu, Z. C.; Muller, A.
      Physical Review B: Condensed Matter and Materials Physics (2014), 89 (15), 155305/1-155305/6CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
      We report on resonant light scattering expts. in which a single InAs quantum dot is exposed to two independently tunable continuous-wave lasers while the scattered light is analyzed background free, with high spectral and temporal resoln. In contrast to the well-known monochromatic case exhibiting Rabi oscillations, in this bichromatic case the addnl. field introduces oscillations at half the difference of the laser frequencies and harmonics thereof, persisting beyond the natural lifetime. The familiar "dressed-states" ladder now contains an infinite no. of levels per manifold. With suitable averaging, the rich resulting spectra and second-order correlations can be reproduced accurately using the Bloch equations and the quantum regression theorem.
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    39. 39
      Sbresny, F.; Hanschke, L.; Schöll, E.; Rauhaus, W.; Scaparra, B.; Boos, K.; Casalengua, E. Z.; Riedl, H.; Del Valle, E.; Finley, J. J. Stimulated generation of indistinguishable single photons from a quantum ladder system. Phys. Rev. Lett. 2022, 128, 093603,  DOI: 10.1103/PhysRevLett.128.093603
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      Stimulated Generation of Indistinguishable Single Photons from a Quantum Ladder System
      Sbresny, Friedrich; Hanschke, Lukas; Schoell, Eva; Rauhaus, William; Scaparra, Bianca; Boos, Katarina; Zubizarreta Casalengua, Eduardo; Riedl, Hubert; del Valle, Elena; Finley, Jonathan J.; Joens, Klaus D.; Mueller, Kai
      Physical Review Letters (2022), 128 (9), 093603CODEN: PRLTAO; ISSN:1079-7114. (American Physical Society)
      We propose a scheme for the generation of highly indistinguishable single photons using semiconductor quantum dots and demonstrate its performance and potential. The scheme is based on the resonant two-photon excitation of the biexciton followed by stimulation of the biexciton to selectively prep. an exciton. Quantum-optical simulations and expts. are in good agreement and show that the scheme provides significant advantages over previously demonstrated excitation methods. The two-photon excitation of the biexciton suppresses re-excitation and enables ultralow multiphoton errors, while the precisely timed stimulation pulse results in very low timing jitter of the photons, and consequently, high indistinguishability. In addn., the polarization of the stimulation pulse allows us to deterministically program the polarization of the emitted photon (H or V). This ensures that all emission of interest occurs in the polarization of the detection channel, resulting in higher brightness than cross-polarized resonant excitation.
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    40. 40
      Wei, Y.; Liu, S.; Li, X.; Yu, Y.; Su, X.; Li, S.; Shang, X.; Liu, H.; Hao, H.; Ni, H.; Yu, S.; Niu, Z.; Iles-Smith, J.; Liu, J.; Wang, X. Tailoring solid-state single-photon sources with stimulated emissions. Nat. Nanotechnol. 2022, 17, 470– 476,  DOI: 10.1038/s41565-022-01092-6
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      40
      Tailoring solid-state single-photon sources with stimulated emissions
      Wei, Yuming; Liu, Shunfa; Li, Xueshi; Yu, Ying; Su, Xiangbin; Li, Shulun; Shang, Xiangjun; Liu, Hanqing; Hao, Huiming; Ni, Haiqiao; Yu, Siyuan; Niu, Zhichuan; Iles-Smith, Jake; Liu, Jin; Wang, Xuehua
      Nature Nanotechnology (2022), 17 (5), 470-476CODEN: NNAABX; ISSN:1748-3387. (Nature Portfolio)
      The coherent interaction of electromagnetic fields with solid-state two-level systems can yield deterministic quantum light sources for photonic quantum technologies. To date, the performance of semiconductor single-photon sources based on three-level systems is limited mainly due to a lack of high photon indistinguishability. Here we tailor the cavity-enhanced spontaneous emission from a ladder-type three-level system in a single epitaxial quantum dot through stimulated emission. After populating the biexciton (XX) of the quantum dot through two-photon resonant excitation, we use another laser pulse to selectively depopulate the XX state into an exciton (X) state with a predefined polarization. The stimulated XX-X emission modifies the X decay dynamics and improves the characteristics of a polarized single-photon source, such as a source brightness of 0.030(2), a single-photon purity of 0.998(1) and an indistinguishability of 0.926(4). Our method can be readily applied to existing quantum dot single-photon sources and expands the capabilities of three-level systems for advanced quantum photonic functionalities.
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      Yan, J.; Liu, S.; Lin, X.; Ye, Y.; Yu, J.; Wang, L.; Yu, Y.; Zhao, Y.; Meng, Y.; Hu, X. Double-pulse generation of indistinguishable single photons with optically controlled polarization. Nano Lett. 2022, 22, 1483– 1490,  DOI: 10.1021/acs.nanolett.1c03543
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      41
      Double-Pulse Generation of Indistinguishable Single Photons with Optically Controlled Polarization
      Yan, Junyong; Liu, Shunfa; Lin, Xing; Ye, Yongzheng; Yu, Jiawang; Wang, Lingfang; Yu, Ying; Zhao, Yanhui; Meng, Yun; Hu, Xiaolong; Wang, Da-Wei; Jin, Chaoyuan; Liu, Feng
      Nano Letters (2022), 22 (4), 1483-1490CODEN: NALEFD; ISSN:1530-6984. (American Chemical Society)
      Single-photon sources play a key role in photonic quantum technologies. Semiconductor quantum dots can emit indistinguishable single photons under resonant excitation. However, the resonance fluorescence technique typically requires cross-polarization filtering, which causes a loss of the unpolarized quantum dot emission by 50%. To solve this problem, we demonstrate a method for generating indistinguishable single photons with optically controlled polarization by two laser pulses off-resonant with neutral exciton states. This scheme is realized by exciting the quantum dot to the biexciton state and subsequently driving the quantum dot to an exciton eigenstate. By combining with a magnetic field, we demonstrated the generation of photons with optically controlled polarization (the degree of polarization is 101(2)%), laser-neutral exciton detuning up to 0.81 meV, high single-photon purity (99.6(1)%), and indistinguishability (85(4)%). Laser pulses can be blocked using polarization and spectral filtering. Our work makes an important step toward indistinguishable single-photon sources with near-unity collection efficiency.
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    42. 42
      Ardelt, P. L.; Hanschke, L.; Fischer, K. A.; Müller, K.; Kleinkauf, A.; Koller, M.; Bechtold, A.; Simmet, T.; Wierzbowski, J.; Riedl, H.; Abstreiter, G.; Finley, J. J. Dissipative preparation of the exciton and biexciton in self-assembled quantum dots on picosecond time scales. Phys. Rev. B 2014, 90, 241404  DOI: 10.1103/PhysRevB.90.241404
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      42
      Dissipative preparation of the exciton and biexciton in self-assembled quantum dots on picosecond time scales
      Ardelt, Per-Lennart; Hanschke, Lukas; Fischer, Kevin A.; Mueller, Kai; Kleinkauf, Alexander; Koller, Manuel; Bechtold, Alexander; Simmet, Tobias; Wierzbowski, Jakob; Riedl, Hubert; Abstreiter, Gerhard; Finley, Jonathan J.
      Physical Review B: Condensed Matter and Materials Physics (2014), 90 (24), 241404CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
      Pulsed resonant fluorescence is used to probe ultrafast phonon-assisted exciton and biexciton prepn. in individual self-assembled InGaAs quantum dots. By driving the system using large area (≥10π) near resonant optical pulses, we exptl. demonstrate how phonon-mediated dissipation within the manifold of dressed excitonic states can be used to prep. the neutral exciton with a fidelity ≥70%. By comparing the phonon-assisted prepn. with resonant Rabi oscillations we show that the phonon-mediated process provides the higher-fidelity prepn. for large pulse areas and is less sensitive to pulse area variations. Moreover, by detuning the laser with respect to the exciton transition, we map out the spectral d. for exciton coupling to the bulk LA-phonon continuum. Similar phonon-mediated processes are shown to facilitate direct biexciton prepn. via two-photon biexciton absorption, with fidelities >80%. Our results are found to be in very good quant. agreement with simulations that model the quantum dot-phonon bath interactions with Bloch-Redfield theory.
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      Bounouar, S.; Müller, M.; Barth, A. M.; Glässl, M.; Axt, V. M.; Michler, P. Phonon-assisted robust and deterministic two-photon biexciton preparation in a quantum dot. Phys. Rev. B 2015, 91, 161302  DOI: 10.1103/PhysRevB.91.161302
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      43
      Phonon-assisted robust and deterministic two-photon biexciton preparation in a quantum dot
      Bounouar, S.; Mueller, M.; Barth, A. M.; Glaessl, M.; Axt, V. M.; Michler, P.
      Physical Review B: Condensed Matter and Materials Physics (2015), 91 (16), 161302/1-161302/5CODEN: PRBMDO; ISSN:1098-0121. (American Physical Society)
      We investigate both exptl. and theor. a simple yet more robust and flexible alternative to Rabi oscillation-type biexciton prepn. protocols traditionally used for semiconductor quantum dots. The quantum dot is excited by a strong laser pulse pos. detuned from the two-photon resonance yielding an on demand initialization of the biexciton state by making use of the phonon-induced thermalization of the photon dressed states. It is shown that for excitation pulses in the picosecond range, a stable and high occupation of up to CXX = 0.95 ± 0.02 is reached. Notably, the generated photons show similar coherence properties as measured in the resonant two-photon scheme. This protocol is a powerful tool for the control of complex solid state systems combining radiative cascades, entanglement, and resonant cavity modes.
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    44. 44
      Quilter, J. H.; Brash, A. J.; Liu, F.; Glässl, M.; Barth, A. M.; Axt, V. M.; Ramsay, A. J.; Skolnick, M. S.; Fox, A. M. Phonon-Assisted Population Inversion of a Single InGaAs/GaAs Quantum Dot by Pulsed Laser Excitation. Phys. Rev. Lett. 2015, 114, 137401,  DOI: 10.1103/PhysRevLett.114.137401
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      44
      Phonon-assisted population inversion of a single InGaAs/GaAs quantum dot by pulsed laser excitation
      Quilter, J. H.; Brash, A. J.; Liu, F.; Glassl, M.; Barth, A. M.; Axt, V. M.; Ramsay, A. J.; Skolnick, M. S.; Fox, A. M.
      Physical Review Letters (2015), 114 (13), 137401/1-137401/5CODEN: PRLTAO; ISSN:0031-9007. (American Physical Society)
      We demonstrate a new method to realize the population inversion of a single InGaAs/GaAsquantum dot excited by a laser pulse tuned within the neutral exciton phonon sideband. In contrast to the conventional method of inverting a two-level system by performing coherent Rabi oscillation, the inversion is achieved by rapid thermalization of the optically dressed states via incoherent phonon-assisted relaxation. A max. exciton population of 0.67 ± 0.06 is measured for a laser tuned 0.83 meV to higher energy. Furthermore, the phonon sideband is mapped using a two-color pump-probe technique, with its spectral form and magnitude in very good agreement with the result of path-integral calcns.
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      Barth, A. M.; Lüker, S.; Vagov, A.; Reiter, D. E.; Kuhn, T.; Axt, V. M. Fast and selective phonon-assisted state preparation of a quantum dot by adiabatic undressing. Phys. Rev. B 2016, 94, 45306,  DOI: 10.1103/PhysRevB.94.045306
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      Fast and selective phonon-assisted state preparation of a quantum dot by adiabatic undressing
      Barth, A. M.; Lueker, S.; Vagov, A.; Reiter, D. E.; Kuhn, T.; Axt, V. M.
      Physical Review B (2016), 94 (4), 045306/1-045306/10CODEN: PRBHB7; ISSN:2469-9950. (American Physical Society)
      We investigate theor. the temporal behavior of a quantum dot under off-resonant optical excitation targeted at fast acoustic phonon-assisted state prepn. We demonstrate that in a prepn. process driven by short laser pulses, three processes can be identified: a dressing of the states during the switch-on of the laser pulse, a subsequent phonon-induced relaxation, and an undressing at the end of the pulse. By analyzing excitation scenarios with different pulse shapes we highlight the decisive impact of an adiabatic undressing on the final state in short-pulse protocols. Furthermore, we show that in exciton-biexciton systems the laser characteristics such as the pulse detuning and the pulse length as well as the biexciton binding energy can be used to select the targeted quantum dot state.
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      Cosacchi, M.; Ungar, F.; Cygorek, M.; Vagov, A.; Axt, V. M. Emission-Frequency Separated High Quality Single-Photon Sources Enabled by Phonons. Phys. Rev. Lett. 2019, 123, 17403,  DOI: 10.1103/PhysRevLett.123.017403
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      46
      Emission-Frequency Separated High Quality Single-Photon Sources Enabled by Phonons
      Cosacchi, M.; Ungar, F.; Cygorek, M.; Vagov, A.; Axt, V. M.
      Physical Review Letters (2019), 123 (1), 017403CODEN: PRLTAO; ISSN:1079-7114. (American Physical Society)
      We demonstrate theor. that the single-photon purity of photons emitted from a quantum dot exciton prepd. by phonon-assisted off-resonant excitation can be significantly higher in a wide range of parameters than that obtained by resonant prepn. for otherwise identical conditions. Despite the off-resonant excitation, the brightness stays on a high level. These surprising findings exploit the fact that the phonon-assisted prepn. is a two-step process where phonons first lead to a relaxation between laser-dressed states while high exciton occupations are reached only with a delay to the laser pulse max. by adiabatically undressing the dot states. Due to this delay, possible subsequent processes, in particular multiphoton excitations, appear at a time when the laser pulse is almost gone. The resulting suppression of reexcitation processes increases the single-photon purity. Due to the spectral sepn. of the signal photons from the laser frequencies this enables the emission of high quality single photons not disturbed by a laser background while taking advantage of the robustness of the phonon assisted scheme.
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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.nanolett.2c01783.

    • Experimental details; background estimation; normalization of the pulse intensities; verification of the two-pulse effect; optimizing the first pulse intensity; lifetime and intrinsic line width; radiative efficiency (PDF)


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