Asymmetric two-photon response of an incoherently driven quantum emitter
Lennart Jehle, L. M. Hansen, Patrik Isene Sund, Thomas Wilkens Sandø, Raphael Joos, Michael Jetter, Simone Luca Portalupi, Mathieu Bozzio, Peter Michler, Philip John Walther
Quantum emitters promise to emit exactly one photon when pumped by a laser pulse. However, even in ideal systems, re-excitation during the laser pulse duration causes the consecutive emission of two photons, thus limiting the single-photon purity. Although the probability and characteristics of re-excitation are largely determined by the excitation scheme, until now, only resonant driving has been studied. Here, we demonstrate qualitative differences for phonon-assisted excitation and resolve the distinct temporal and spectral profile of each of the photons. These uncover correlations between the emission time and wavelength, resulting in an asymmetric two-photon spectrum. On a fundamental level, we show that this spectrum provides direct access to the Rabi frequency of an incoherently driven quantum dot. On the application side, we leverage the asymmetry to selectively suppress multiphoton noise, ensuring high single-photon purity regardless of the laser pulse length and thus enhancing implementations across quantum cryptography and quantum computing.
Quantum emitters promise to emit exactly one photon when pumped by a laser pulse. However, even in ideal systems, re-excitation during the laser pulse duration causes the consecutive emission of two photons, thus limiting the single-photon purity. Although the probability and characteristics of re-excitation are largely determined by the excitation scheme, until now, only resonant driving has been studied. Here, we demonstrate qualitative differences for phonon-assisted excitation and resolve the distinct temporal and spectral profile of each of the photons. These uncover correlations between the emission time and wavelength, resulting in an asymmetric two-photon spectrum. On a fundamental level, we show that this spectrum provides direct access to the Rabi frequency of an incoherently driven quantum dot. On the application side, we leverage the asymmetry to selectively suppress multiphoton noise, ensuring high single-photon purity regardless of the laser pulse length and thus enhancing implementations across quantum cryptography and quantum computing.
We demonstrate theoretically that the single-photon purity of photons emitted from a quantum dot exciton prepared by phonon-assisted off-resonant excitation can be significantly higher in a wide range of parameters than that obtained by resonant preparation 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 preparation 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 maximum 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 separation 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.
Due to their excellent optical properties, quantum dots are promising for applications in photonic quantum technologies. For on-demand single-photon generation, a two-level system given by an excitonic transition is typically excited with a resonant laser pulse of area π. This prepares the two-level system in its excited state from where it spontaneously emits a single photon. However, emission that occurs already during the presence of the laser pulse allows for re-excitation and, thus, multi-photon emission which limits the single-photon purity [1]. In contrast, when exciting the system with a pulse of area 2π, the system is expected to be returned to the ground state. However, in this case emission during the presence of the pulse is most likely to occur when the system is in its excited state – exactly after an area of π has been absorbed. This restarts the Rabi oscillation with a pulse area of π remaining in the pulse which leads to re-excitation with near-unity probability and the emission of a second photon within the excited state lifetime [2,3]. Finally, we present the generation of single photons with ultra-low multi-photon probability [4]. Using two-photon excitation of the bi-exciton suppresses re-excitation and improves the single photon purity by several orders of magnitude for short pulses. [1] K. A. Fischer, et al., New J. Phys. 18, 113053 (2016) [2] K. A. Fischer, et al., Nature Physics 13, 649-654 (2017) [3] K. A. Fischer, et al., Quantum Sci. Technol. 3, 014006 (2017) [4] L. Hanschke et al., arxiv: 1801.01672 (2018)
Semiconductor quantum dots (QDs) are commonly considered as artificial atoms due to the 3D confinement of the electrons. These nanostructures are very promising for the realization of integrated devices such as single photon sources for quantum cryptography applications [1,2]. However, contrarily to genuine atoms, QDs are condensed matter systems and they consequently suffer from the coupling to their environment [3] which degrades the quality of the emitted photons in view of quantum cryptography applications. One way to circumvent this coupling is to excite strictly resonantly the QD at low temperature [4-10]. This difficult task has been achieved by designing an original excitation scheme to spatially decouple the excitation and detection paths. We first report that experimental studies of the resonant emission (RE) of single QDs can be strongly limited, even impossible, since most of the QDs show a very strong quenching of the RE of the fundamental transition. This issue is a broadly met experimental situation which is highly problematic for cavity quantum electrodynamics experiments in single QDs. We propose an efficient way to overcome this issue based on the use of an ultra-weak non-resonant laser that optically gates the QD RE [8] which controls the residual doping inherent to the QDs fabrication. It induces a complete recovery of the properties of an artificial atom, and the single QDs behave as quasi-ideal two-level systems. Up to now [7,9], the measurements on the QDs RE reported in the literature mainly focus on the incoherent fluorescence signal for achieving efficient single photon emission. In this regime, the spectrum linewidth is always limited to the radiative limit. We present experimental studies on the coherent laser light scattering by a single QD [7]. Besides the antibunching effect showing the non-classical nature of the emitted light, we observe that the QD emission spectrum is determined by the spectrum of the resonant excitation laser. By reducing the resonant excitation power, the so-called Mollow triplet shrinks to a single narrow Lorentzian line, while the relative intensity of this narrow peak increases and tends to overwhelm the RE spectrum. This implies that single QDs can produce single photons with a coherence time that is not limited anymore by the QD electronic properties, resulting in what we name an " ultra-coherent " character [7]. In conclusion, the resulting ultra-coherent single photon source promises high degrees of indistinguishability of the emitted photons which is a crucial requirement for quantum information applications. References [1] P. Michler et al., Science 290 (2000). [6] S. Ates et al., PRL 103 (2009). [2] C. Santori et al., Nature 419 (2002). [7] H. S. Nguyen et al., APL 99 (2011). [3] A. Berthelot et al., Nat. Phys. 2 (2006). [8] H. S. Nguyen et al., PRL 108 (2012). [4] A. Muller et al., PRL 99 (2007). [9] C. Matthiesen et al., PRL 1082 (2012). [5] R. Melet et al., PRB 78 (2008). [10] A. Reinhard et al., Nat. Phot. 6 (2012).
Two experiments observe the so-called Mollow triplet in the emission spectrum of a quantum dot—originating from resonantly driving a dot transition—and demonstrate the potential of these systems to act as single-photon sources, and as a readout modality for electron-spin states. Single-quantum emitters emit only one photon at a time1,2, but the properties of the photon depend on how the emitter is excited3. Incoherent excitation is simple and broadly used with solid-state emitters such as quantum dots, but does not allow direct manipulation of the quantum state. Coherent, resonant excitation on the other hand is used in pump–probe techniques to examine the quantum state of the emitter4, but does not permit collection of the single-photon emission. Coherent control with simultaneous generation of photons has been an elusive goal in solid-state approaches, where, because of strong laser scattering at the detection wavelength, measurement of resonant emission has been limited to cross-polarized detection5 or Stokes-shift techniques6,7. Here we demonstrate that a semiconductor quantum dot in a microcavity can be resonantly driven and its single-photon emission extracted background free. Under strong continuous-wave excitation, the dot undergoes several Rabi oscillations before emitting, which are visible as oscillations in the second-order correlation function. The quantum-dot states are therefore ‘dressed’, resulting in a Mollow-triplet emission spectrum. Such coherent control will be necessary for future high-efficiency sources of indistinguishable single photons3,8, which can be used for quantum key distribution9 or through post-selection10 to generate entangled photon pairs11,12.
Resonant laser excitation of a two-level system with subsequent single-photon emission can be used to generate single photons with high indistinguishability or Hong-Ou-Mandel (HOM) visibility. However, spectral overlap between excitation laser and emitted photons generally poses significant challenges. Furthermore, emitter re-excitation intrinsically limits achievable single-photon purity. Established solutions mitigate these issues at significant cost to source efficiency and with increased source complexity. This motivates the use of few-level systems with spectral separation of excitation and emission pathways. One option is a three-level cascade. However, without targeted lifetime engineering of emitting states, the cascade naturally limits achievable photon indistinguishability. Here we study a semiconductor quantum dot with resonant and selective cavity-enhancement of biexciton-to-exciton transition. Following resonant two-photon excitation of the biexciton state, we collect the emitted single photon with the cavity. This approach circumvents emitter re-excitation and naturally introduces spectral separation of excitation laser and emitted single photon. Supported by first experimental results, we demonstrate theoretically that with selective Purcell enhancement, the observed quality quantifiers of single-photon emission (purity, equivalently g(2)(0), and HOM visibility V, equivalently indistinguishability) are competitive with respect to high-quality deterministic quantum-dot single-photon sources. This is already achieved without systematic optimization or targeted system engineering, which firmly places the reported approach as a viable route to the next generation of highest-quality quantum-dot based deterministic single-photon sources.
Single-photon purity is one of the most important key metrics of many quantum states of light. For applications in photonic quantum technologies, e.g. quantum communication and linear optical quantum computing, a minimization of the multi-photon error rate is required because of its error-introducing nature. Ultimately, the purity of state-of-the-art single-photon sources was found to be limited by spontaneous emission and subsequent reexcitation during the interaction with the driving field. Here, we demonstrate that even this fundamental limit to the single-photon purity can be overcome due to the distinct spectro-temporal properties of the individual photons forming multi-photon errors. For driving pulses shorter than the emitter lifetime, we find that photons emitted during the pulse exhibit a significantly broader spectral shape than the emitter's natural linewidth. Thus, we can selectively filter out the majority of this instantaneously emitted photon by employing narrowband spectral filters, which reduces the measured degree of second-order coherence at zero time delay by almost one order of magnitude. This enables a significant suppression of the multi-photon error rate without detrimental effects on the desired single-photon emission.