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arXiv:2301.13806 · New Journal of Physics

Cavity-enhanced excitation of a quantum dot in the picosecond regime

Alisa Javadi, Natasha Tomm, Nadia O. Antoniadis, Alistair J. Brash, Rüdiger Schott, Sascha R. Valentin, Andreas Dirk Wieck, Arne Ludwig, Richard John Warburton

Published Aug 23, 2023• 7 citations
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Abstract

Abstract A major challenge in generating single photons with a single emitter is to excite the emitter while avoiding laser leakage into the collection path. Ideally, any scheme to suppress this leakage should not result in a loss in the efficiency of the single-photon source. Here, we investigate a scheme in which a single emitter, a semiconductor quantum dot, is embedded in a microcavity. The scheme exploits the splitting of the cavity mode into two orthogonally-polarised modes: one mode is used for excitation, the other for collection. By linking the experiment to theory, we show that the best population inversion is achieved with a laser pulse detuned from the quantum emitter. The Rabi oscillations exhibit an unusual dependence on pulse power. Our theory describes them quantitatively, enabling us to determine the absolute population inversion. By comparing the experimental results with our theoretical model, we determine a population inversion of 98 % − 5 % + 1 % for optimal laser detuning. The Rabi oscillations depend on the sign of the laser-pulse detuning, a phenomenon arising from the non-trivial effect of phonons on the exciton dynamics. The exciton–phonon interaction is included in the theory and gives excellent agreement with all the experimental results.

DOI
10.1088/1367-2630/acf33b

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Abstract A major challenge in generating single photons with a single emitter is to excite the emitter while avoiding laser leakage into the collection path. Ideally, any scheme to suppress this leakage should not result in a loss in the efficiency of the single-photon source. Here, we investigate a scheme in which a single emitter, a semiconductor quantum dot, is embedded in a microcavity. The scheme exploits the splitting of the cavity mode into two orthogonally-polarised modes: one mode is used for excitation, the other for collection. By linking the experiment to theory, we show that the best population inversion is achieved with a laser pulse detuned from the quantum emitter. The Rabi oscillations exhibit an unusual dependence on pulse power. Our theory describes them quantitatively, enabling us to determine the absolute population inversion. By comparing the experimental results with our theoretical model, we determine a population inversion of 98 % − 5 % + 1 % for optimal laser detuning. The Rabi oscillations depend on the sign of the laser-pulse detuning, a phenomenon arising from the non-trivial effect of phonons on the exciton dynamics. The exciton–phonon interaction is included in the theory and gives excellent agreement with all the experimental results.
We introduce an intuitive and semianalytical polaron master equation approach to model pulse-driven population inversion and emitted single photons from a quantum dot exciton. The master equation theory allows one to identify important phonon-induced scattering rates analytically and fully includes the role of the time-dependent pump field. As an application of the theory, we first study a quantum dot driven by a time-varying laser pulse on and off resonance, showing the population inversion caused by acoustic phonon emission in direct agreement with recent experiments of Quilter et al. [Phys. Rev. Lett. 114, 137401 (2015)]. We then model quantum dots in weakly coupled cavities and show the difference in population response between exciton-driven and cavity-driven systems. Finally, we assess the nonresonant phonon-assisted loading scheme with a quantum dot resonantly coupled to a cavity as a deterministic single-photon source. We also compare and contrast the important single photon figures of merit with direct Rabi oscillation of the population using a resonant $\ensuremath{\pi}$ pulse, and show that the resonant scheme is much more efficient.
Semiconductor quantum dots (QDs) coupled with optical microcavities provide an excellent platform for generating high-performance single-photon sources. However, the current microcavity structures are difficult to solve the tradeoff between single-photon purity and indistinguishability without additional filtering, due to challenges in suppressing broad phonon sideband spectrum and two-photon emission in the practical experiments. To address these issues, we have developed a novel asymmetric microcavity that supports two nondegenerate polarized modes, both resonant with a single quantum dot. One cavity mode is broadband and is used for excitation to reduce two-photon emission intensity, while the other is narrowband and is used for collection to enhance the indistinguishability of single-photon sources. This asymmetric microcavity also has the ability to overcome at least half of the photon efficiency loss under polarization filtering. Moreover, our model has employed an excitation pulse that resonates with cavity modes eliminating spectral distortion of intracavity fields, and efficiently achieving deterministic population inversion of QDs compared to an elliptical cavity. Our scheme paves the way to develop the excellent performance single-photon sources with higher brightness, near-unity purity, and indistinguishability without any additional filtering in practical experiments.
Coherent control of quantum emitters is essential for scalable quantum photonic technologies. The recently proposed swing up of the quantum emitter population (SUPER) scheme allows efficient and coherent state preparation via off-resonant, red-detuned laser pulses, simplifying laser suppression and enhancing photon collection. We present a systematic study of SUPER excitation applied to a single GaAs quantum dot in a low- Q micropillar cavity. We first identify the optimal excitation conditions for SUPER, and then compare the key figures of merit against the well-established two-photon excitation (TPE). Despite requiring higher excitation powers, SUPER achieves near-unity population inversion of the exciton state ( ∼ 95 % ) and high single-photon purity ( g ( 2 ) = 0.03 ) comparable to that under TPE, while also exhibiting a shortened decay time ( ∼ 200 ps) reducing the time jitter in the exciton population. A polarization-resolved analysis reveals that when both excitation and collection are aligned with one of the exciton dipoles, SUPER results in highly polarized single-photon emission, exceeding the resonant TPE saturation by a factor of 1.45. Under optimized excitation conditions, we also observe biexciton preparation via a distinct SUPER resonance, constituting an experimental demonstration of biexciton preparation using SUPER. These findings are in good agreement with a proposed four-level theoretical model that incorporates the biexciton state. Furthermore, we report that, strikingly, a slight misalignment of laser polarization induces an additional SUPER resonance that selectively populates the orthogonal exciton dipole, without altering the nominal excitation polarization. This unexpected behavior reveals a new degree of freedom for coherent state preparation. Our findings establish the SUPER scheme as a versatile tool for state-selective exciton and biexciton control, with strong potential for quantum photonic applications.
We demonstrate a new method to realize the population inversion of a single InGaAs/GaAs quantum 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 maximum 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 calculations.
Single-photon sources with near-unity efficiency and indistinguishability play a major role in the development of quantum technologies. However, on-demand excitation of the emitter imposes substantial limitations to the source performance. Here, we show that coherent two-color pumping allows for population inversion arbitrarily close to unity in bulk quantum dots thanks to a decoupling effect between the emitter and its phonon bath. Driving a micropillar single-photon source with this scheme, we calculate very high photon emission into the cavity mode (0.95 photons per pulse) together with excellent indistinguishability (0.975) in a realistic configuration, thereby removing the limitations imposed by the excitation scheme on single-photon source engineering.
We demonstrate the simultaneous dressing of both vacuum-to-exciton and exciton-to-biexciton transitions of a single semiconductor quantum dot in a high-Q micropillar cavity, using photoluminescence spectroscopy. Resonant two-photon excitation of the biexciton is achieved by spectrally tuning the quantum dot emission with respect to the cavity mode. The cavity couples to both transitions and amplifies the Rabi frequency of the likewise resonant continuous wave laser, driving the transitions. We observe strong-field splitting of the emission lines, which depend on the driving Rabi field amplitude and the cavity-laser detuning. A dressed state theory of a driven 4-level atom correctly predicts the distinct spectral transitions observed in the emission spectrum, and a detailed description of the emission spectra is further provided through a polaron master equation approach which accounts for cavity coupling and acoustic phonon interactions of the semiconductor medium.