Emission coherence is crucial for quantum photonic technologies like single-photon emitters. However, emission from most bulk semiconductors suffers from severely limited coherence times under non-resonant excitation, typically in the femtosecond to picosecond range. In this study, we investigate the temporal coherence properties of excitons in cuprous oxide (Cu2O) using interferometric Fourier spectroscopy. We reveal a coherence time of approximately 24 ps and a homogeneous linewidth of 0.017 nm (55 μeV) at 4.7 K under non-resonant two-photon excitation. We also analyze the impact of relaxation, scattering, and the experimental setup on the decrease in coherence time. The 1S orthoexciton shows robust photoluminescence intensity and negligible spectral diffusion over 120 min. These results suggest that Cu2O presents itself as an exceptional material for generating indistinguishable single photons, demonstrating considerable potential for advanced applications in quantum photonics.
Emission coherence is crucial for quantum photonic technologies like single-photon emitters. However, emission from most bulk semiconductors suffers from severely limited coherence times under non-resonant excitation, typically in the femtosecond to picosecond range. In this study, we investigate the temporal coherence properties of excitons in cuprous oxide (Cu2O) using interferometric Fourier spectroscopy. We reveal a coherence time of approximately 24 ps and a homogeneous linewidth of 0.017 nm (55 μeV) at 4.7 K under non-resonant two-photon excitation. We also analyze the impact of relaxation, scattering, and the experimental setup on the decrease in coherence time. The 1S orthoexciton shows robust photoluminescence intensity and negligible spectral diffusion over 120 min. These results suggest that Cu2O presents itself as an exceptional material for generating indistinguishable single photons, demonstrating considerable potential for advanced applications in quantum photonics.
The intensity of the resonant emission of the 1s orthoexcitons in Cu2O is observed in a weak magnetic field under two-photon resonant excitation at 1.6K to investigate the quantum interference within the Zeeman sublevels in the Faraday configuration. A specific decrease of $\ensuremath{\sim}15%$ in the emission intensity is observed in the region of $\ifmmode\pm\else\textpm\fi{}0.2\phantom{\rule{0.3em}{0ex}}\mathrm{T}$. This structure is interpreted as a manifestation of the quantum interference effect between the Zeeman sublevels of the 1s orthoexcitons, known as the Hanle effect in atomic spectroscopy. The homogeneous width of the exciton level is estimated to be $5.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{eV}$. The contribution of the quadrupole exciton polariton is discussed by taking into account the geometry-dependent characteristics of the exciton-polariton on the direction of the magnetic field. The Hanle structure observed is attributed to the interference of the polariton wave packets of the longitudinal excitons, where the phase coherence is transferred via transverse excitons driven by resonant two-photon coupling with the radiation field.
Light emission from solid-state quantum emitters is inherently prone to environmental decoherence, which results in a line broadening and in the deterioration of photon indistinguishability. Here we employ photon correlation Fourier spectroscopy (PCFS) to study the temporal evolution of such a broadening in two prominent systems: GaAs and In(Ga)As quantum dots. Differently from previous experiments, the emitters are driven with short laser pulses as required for the generation of high-purity single photons, the time scales we probe range from a few nanoseconds to milliseconds and, simultaneously, the spectral resolution we achieve can be as small as ∼ 2µeV. We find pronounced differences in the temporal evolution of different optical transition lines, which we attribute to differences in their homogeneous linewidth and sensitivity to charge noise. We analyze the effect of irradiation with additional white light, which reduces blinking at the cost of enhanced charge noise. Due to its robustness against experimental imperfections and its high temporal resolution and bandwidth, PCFS outperforms established spectroscopy techniques, such as Michelson interferometry. We discuss its practical implementation and the possibility to use it to estimate the indistinguishability of consecutively emitted single photons for applications in quantum communication and photonic-based quantum information processing.
Single photon emission is one of the most striking optical properties of semiconductor quantum dots (QDs), and the corresponding photon anti-bunching effect was observed by non-resonant and resonant photoluminescence experiments in single QDs [1,2,3,4]. Other experiments demonstrated the possibility to use single QDs for the generation of indistinguishable single photons [3]. An important general issue is to reach the so-called fundamental radiative limit. Several strategies have been followed in that sense such as the shortening of population lifetime induced by the Purcell effect [5] or the reduction of pure dephasing by resonant excitation [2,3,4]. Up to now, all the measurements reported in the literature focus on the incoherent photoluminescence signal for achieving single photon emission. In this regime, the linewidth of the photoluminescence spectrum is always limited to the radiative limit. In this paper, we report on the resonant emission (RE) of the exciton in single InAs/GaAs QDs embedded in a planar microcavity, in an orthogonal excitation-detection geometry [4]. We present an original type of single photon source based on the coherent laser light scattering by a single QD [6]. 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. We present high-resolution measurements by Fourier transform spectroscopy of the RE where the data are fitted to the first-order correlation function g(1)(τ) of the RE of a two-level system. The inverse Fourier transform of the g(1)(τ) function allows a direct comparison of the different RE emission profiles. We show that, 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 an ultra-coherent character [6]. 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. [1] P. Michler et al., Science 290, 2282 (2000). [2] A. Muller et al., Phys. Rev. Lett. 99, 187402 (2007). [3] S. Ates et al., Phys. Rev. Lett. 103, 167402 (2009). [4] H. S. Nguyen et al., Phys. Rev. Lett. 108, 057401 (2012). [5] C. Santori et al., Nature 419, 594 (2002). [6] H. S. Nguyen et al., Appl. Phys. Lett. 99, 261904 (2011).
Single photon emission is one of the most striking optical properties of semiconductor quantum dots (QDs), and the corresponding photon anti-bunching effect was observed by non-resonant and resonant photoluminescence experiments in single QDs [1,2]. Up to now, all the measurements reported in the literature focus on the incoherent photoluminescence signal for achieving single photon emission. In this regime, the linewidth of the photoluminescence spectrum is limited to the so-called radiative limit. In this paper, we report on the resonant emission (RE) of the exciton in single InAs/GaAs QDs embedded in a planar microcavity [2]. We present an original type of single photon source based on the coherent laser light scattering by a single QD [3]. Besides the antibunching effect showing the nonclassical nature of the emitted light, we observe that the QD emission spectrum is determined by the spectrum of the resonant excitation laser. Figure (a,b,c) shows high-resolution measurements by Fourier transform spectroscopy of the RE where the data are fitted to the first-order correlation function g(1)(τ) of the RE of a two-level system. The inverse Fourier transform of the g(1)(τ) function allows a direct comparison of the different RE emission profiles in figure (d,e,f). By reducing the resonant excitation power, the 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 an ultra-coherent character [3]. References [1] P. Michler et al, Science 290, 2282 (2000). [2] H. S. Nguyen et al, Phys. Rev. Lett. (accepted, in press). See arXiv 1109.4304. [3] H. S. Nguyen et al, Appl. Phys. Lett. 99, 261904 (2011).
Rydberg excitons are, with their ultrastrong mutual interactions, giant optical nonlinearities, and very high sensitivity to external fields, promising for applications in quantum sensing and nonlinear optics at the single-photon level. To design quantum applications it is necessary to know how Rydberg excitons and other excited states relax to lower-lying exciton states. Here, we present photoluminescence excitation spectroscopy as a method to probe transition probabilities from various excitonic states in cuprous oxide. We show giant Rydberg excitons at T=38 mK with principal quantum numbers up to n=30, corresponding to a calculated diameter of $3\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{m}$.
The ability of individual photonic qubits to interact via interference lies at the heart of many quantum networking applications. For their development, sources of highly coherent, indistinguishable photons are therefore crucial. Here, we investigate the noise sources that affect InAs/InP quantum dots and limit their coherence. We show that the droplet epitaxy growth mode leads to a quiet environment with 96% of exciton transitions having a coherence time above 100 ps, even under non-resonant excitation. Further, Hong–Ou–Mandel interference reveal a corrected two-photon interference visibility of 98.6±1.6% for these quantum dots, showing their potential for quantum networking applications.