Introduction Quantum optics provides a complete description of the resonant interaction of light and a material system. The light scattered as a result of this interaction – the resonance fluorescence – provides a means to monitor and affect the material system's dynamics and also allows for the generation of nonclassical states of the electromagnetic field. Initial theoretical studies characterizing resonance fluorescence addressed fundamental questions regarding the necessity of quantizing the electromagnetic field. This is a particularly illustrative period in optical physics where multiple theories existed that might describe resonance fluorescence – semi-classical optical Bloch equations [1, 2] or quantum electrodynamics [4, 3] – and experimental evidence was necessary to identify the appropriate theoretical framework. Indeed, experiments in 1974 and 1977 investigating the resonance fluorescence lineshape [5, 6] and the photon statistics of the scattered light [7] vindicated the full quantum electrodynamical description of light-matter interaction over other models. In the subsequent 30 years, resonance fluorescence has been used as a high-resolution spectroscopic probe of a variety of physical systems, as a means to investigate quantum coherence in atomic gases and, with the current interest in quantum information science (QIS), as a tool for quantum-state preparation, measurement and control in trapped ions [8]. During this same time period, advances in material science have ushered in an era where it is possible to grow and fabricate solid-state devices at length scales commensurate with the quantum confinement of electrons and holes. It is only recently that resonance fluorescence has been observed from the prototypical artificial nanostructure exhibiting three-dimensional quantum confinement – a single semiconductor quantum dot (QD) [9].
Introduction Quantum optics provides a complete description of the resonant interaction of light and a material system. The light scattered as a result of this interaction – the resonance fluorescence – provides a means to monitor and affect the material system's dynamics and also allows for the generation of nonclassical states of the electromagnetic field. Initial theoretical studies characterizing resonance fluorescence addressed fundamental questions regarding the necessity of quantizing the electromagnetic field. This is a particularly illustrative period in optical physics where multiple theories existed that might describe resonance fluorescence – semi-classical optical Bloch equations [1, 2] or quantum electrodynamics [4, 3] – and experimental evidence was necessary to identify the appropriate theoretical framework. Indeed, experiments in 1974 and 1977 investigating the resonance fluorescence lineshape [5, 6] and the photon statistics of the scattered light [7] vindicated the full quantum electrodynamical description of light-matter interaction over other models. In the subsequent 30 years, resonance fluorescence has been used as a high-resolution spectroscopic probe of a variety of physical systems, as a means to investigate quantum coherence in atomic gases and, with the current interest in quantum information science (QIS), as a tool for quantum-state preparation, measurement and control in trapped ions [8]. During this same time period, advances in material science have ushered in an era where it is possible to grow and fabricate solid-state devices at length scales commensurate with the quantum confinement of electrons and holes. It is only recently that resonance fluorescence has been observed from the prototypical artificial nanostructure exhibiting three-dimensional quantum confinement – a single semiconductor quantum dot (QD) [9].
Single semiconductor quantum dots, which are considered as two-level systems in the artificial atom model, are promising structures for the realization of integrated devices such as single photon sources for quantum information applications. However, contrary to genuine atoms, they are condensed matter systems which suffer from the coupling to their solid environment, leading to a degradation of the coherence of the emitted photons. One possibility to avoid this coupling, thereby improving the coherence of the photons until the one imposed by the radiative limit T2 = 2T1, is to perform strictly resonant excitation of a quantum dot at low temperature. Using an experimental setup that spatially decouples the excitation and detection paths, we showed that a fine control of the electrostatic environment related to the nanostructures residual doping remains a major challenge to answer the widely encountered problem of the inhibition of the resonance fluorescence of a quantum dot. Meanwhile, thanks to quantum optics experiments and high resolution optical spectroscopy, we demonstrated that the resonant Rayleigh scattering regime where quantum dots emit single photons with the laser coherence time, paves the way to the development of "ultra-coherent" sources of single photons with high degrees of indistinguishability. In this regime where the laser tailors the coherence of the photons and where the radiative limit becomes a secondary requirement, two photons emitted successively by the same quantum dot are indistinguishable on time scales never obtained before for a solid nano-emitter (up to ten nanoseconds, comparing to the carriers lifetime and decoherence time of about a hundred of picoseconds).
Next-generation information technology is expected to rely on discrete two-state quantum systems that can deterministically emit single photons. Quantum dots are mesoscopic (~10,000 atoms large) semiconductor islands grown in a host crystal of larger band-gap that make well-defined two-level quantum systems and are very attractive due to stability, record coherence times, and the possibility of integrating them into larger structures, such as optical microcavities. This work presents experimental progress towards understanding the coherent optical processes that occur in single quantum dots, particularly such phenomena that might be one day utilized for quantum communication applications. High resolution low temperature optical spectroscopy is used in conjunction with first order (amplitude) and second-order (intensity) correlation measurements of the emitted field. A novel technique is introduced that is capable of harvesting the fluorescence of single dots at the same frequency as the laser, previously impossible due to insurmountable scattering. This technique enables the observation, for the first time, of single quantum dot resonance fluorescence, in both the weak and strong excitation regimes, which forms the basis for deterministic generation of single photons. Guided by the rich theoretical description available from quantum optics with atoms we obtain insight into the complex dynamics of this driven system. Quantum dots confined to novel optical microcavities were further investigated using micro photoluminescence. An optical microcavity properly coupled to a two-level system can profoundly modify its emission characteristics via quantum electrodynamical effects, which are highly attractive for single photon sources. The all-epitaxial structures we probe are distinguished by a bulk morphology that overcomes the fragility problems of existing approaches, and provides high quality factors as well as small mode volumes. Lasing is obtained with larger strucutres. Additionally, isolation of individual dots is further realized in smaller cavities and the Purcell effect observed in time-resolved photon counting experiments.
Quantum optics provides a fundamental framework for understanding the interaction between light and matter at the quantum level. Recently, it has been shown that under incoherent pumping, the resonance fluorescence spectrum dramatically changes. Engineering the resonance fluorescence spectrum paves the way towards solid-state-based single-photon sources. In this paper, we start by reviewing and reproducing some of the results concerning the resonance fluorescence spectrum, single-photon sources, dressed-state lasers, and luminescence spectrum of a quantum dot in a microcavity. Photon correlations in quantum optical systems and spectral properties of radiation emitted by atomic and semiconductor systems interacting with external fields are investigated. The well known Mollow triplet structure of the emission spectrum is discussed, together with the role of dressed states in explaining the origin of the three spectral peaks. Furthermore, the luminescence spectra of quantum emitters coupled to microcavities are reviewed. The numerical results presented here contribute to the theoretical understanding of resonance fluorescence, photon correlations, and engineered emission in quantum optical systems. These studies highlight the rich physical properties arising from light matter interaction at the quantum level and demonstrate their relevance for emerging quantum technologies.
In this work, resonant laser spectroscopy has been utilized in two major projects --resonance fluorescence measurements in solid-state quantum-confined nanostructures and laser-induced fluorescence measurements in gases. The first project focuses on studying resonant light-matter interactions in semiconductor quantum dots "artificial atoms" with potential applications in quantum information science. Of primary interest is the understanding of fundamental processes and how they are affected by the solid-state matrix. Unlike atoms, quantum dots are susceptible to a variety of environmental influences such as phonon scattering and spectral diffusion. These interactions alter the desired properties of the scattered light and hinder uses in certain single photon source applications. One application of current interest is the use of quantum dots in “quantum repeaters” for which two-photon interference is key. Motivated by such an application we have explored the limits imposed by environmental effects on two quantum dots in the same sample, the scattered light from which is being interfered. We find that both one-photon and two-photon interference, although substantial, are affected in a variety of ways, in particular by spectral diffusion. These observations are discussed and compared with a theoretical model. We further investigated correlations in pulsed resonance fluorescence, and found significant unexpected spectral and temporal deviations from those studied under continuous wave excitation. Under these conditions, the scattered light exhibits Rabi oscillations and photon anti-bunching, while maintaining a rich spectrum containing many spectral features. These observations are discussed and compared with a theoretical model. In the second project, the focus is on the investigation of the possibility of detecting N2+ ions in air using laser induced fluorescence, with potential applications in detection of fissile materials at a distance. A photon-counting analysis reveals that the fluorescence decay rate rapidly increases with increasing N2 pressure and thus limits the detection at elevated pressures, in particular at atmospheric pressure. We show that time-gated detection can be used to isolate N2+ fluorescence from delayed N2 emission. Based on the spontaneous Raman signal from N2 simultaneously observed with N2+ fluorescence, we could estimate a limit of detection in air of order 108-1010 cm3.
Resonance fluorescence, the process in which a single two-level quantum emitter interacts with a near-resonant coherent light, is a cornerstone of quantum optics as a paradigmatic light-matter interaction. Quantum phenomena in resonance fluorescence have been accounted for in terms of one- and two-photon processes; however, the physical processes arising from the interaction of a single two-level atom with higher photon numbers remain unexplored experimentally. Here we experimentally reveal the multiphoton scattering nature of resonance fluorescence, which intrinsically gives rise to multiphoton entanglement. By accessing quantum fluctuations in the field emitted from a cavity-quantum electrodynamics system, we resolve third- and fourth-order photon scattering events from a single two-level atom. In the three-photon component, the scattered photons are shown to be genuinely energy-time entangled, as verified by a violation of Svetlichny's inequality. As a demonstration of an application, a quantum secret sharing protocol (QSS) is implemented using this entangled photon source. Our study refines the descriptive framework of resonance fluorescence and broadens the scope of its investigation. It also establishes a fundamentally simple route for generating multiphoton entangled states for quantum information processing and quantum metrology.
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).