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.
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.
Self-assembled semiconductor quantum dots have attracted considerable interest recently, ranging from fundamental studies of quantum optics to advanced applications in the field of quantum information science. With their atom-like properties, quantum dot based nanophotonic devices may also substantially contribute to the development of quantum computers. This work presents experimental progress towards the understanding of light-matter interactions that occur beyond well-understood monochromatic resonant light scattering processes in semiconductor quantum dots. First, we report measurements of resonance fluorescence under bichromatic laser excitation. With the inclusion of a second laser, both first-order and second-order correlation functions are substantially altered. Under these conditions, the scattered light exhibits a rich spectrum containing many spectral features that lead to a range of nonlinear multiphoton dynamics. These observations are discussed and compared with a theoretical model. Second, we investigated the light scattered by a quantum dot in the presence of spectral filtering. By scanning the tunable filters placed in front of each detector of a Hanbury-Brown and Twiss setup and recording coincidence measurements, a \\two-photon spectrum" has been experimentally reconstructed for the first time. The two-photon spectrum contains a wealth of information about the cascaded emission involved in the scattering process, such as transitions occurring via virtual intermediate states. Our measurements also reveal that the scattered frequency-filtered light from a quantum dot violates the Cauchy-Schwarz inequality. Finally, Franson-interferometry has been performed using spectrally filtered light from quantum dot resonance fluorescence. Visibilities exceeding the classical limit were demonstrated by using a pair of folded Mach-Zehnder interferometers, paving the way for producing single time-energy entangled photon pairs that could violate Bell's inequalities.
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).
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].
Semiconductor nanostructures such as quantum dots (QDs) have offered unique opportunities to investigate quantum optical effects in solid-state systems. These include quantum interference, Rabi oscillations, as well as photon antibunching, and were previously observable only in isolated atoms or ions. In addition, QDs can be integrated into optical microcavities, making them attractive for applications in quantum information processing and high efficiency quantum light sources. Despite much progress towards these goals, one area that was little explored is coherent control of such solid-state quantum emitters in cavities. The main technical hurdle lies in overcoming the laser background scattering. By using a sample structure in which QDs are embedded in a planar Fabry-Perot cavity and by using an orthogonal excitation geometry, we have achieved a nearly complete elimination of laser background scattering. This in turn allows us to show resonantly controlled light emission of quantum dots in the cavity including (a) Rabi flopping using pulse control, (b) direct observation of Mollow triplets in the frequency domain, and (c) simultaneously measured first-order and second order photon-photon correlations.
Excitons in quantum dots represent a remarkably good two-level system with a large optical dipole transition moment. Although most research currently focuses on enhancing their already outstanding properties as single photon emitters they become also increasingly interesting for experimental fundamental research due to their large dipole transition moment. This thesis presents studies which explore fundamental phenomena in quantum dots using coherent spectrocopy methods. First, we will first examine the optical properties of site-controlled quantum dots which were grown using a buried stressor via resonance fluorescence. Subsequently, we will show results that were obtained using photocurrent spectroscopy to study single quantum dots that are embedded in micropillar resonators. This is followed by a study of the Wigner time delay induced by a single quantum dot and which shows that the maximum delay is larger than its dephasing time T2 which is the theoretical limit for coherently scattered fraction. The next section demonstrates that the response of a resonantly driven two-level system which in our case is represented by an exciton in a seminconductor quantum dot depends significantly on the photon statistics of the exciting light field. Most strikingly, the Mollow triplet which we observe under coherent excitation vanishes under thermal excitation. The second part presents results concerned with the resonantly driven biexciton cascade via two- photon excitation. The coherent interaction between light field and excitons gives rise to a complex five-level system. Here, we show for the first time two-photon Rabi oscillations in the temporal domain. Furthermore, we examine the correlations between the different transitions. The measurements show that we can manipulate the time-ordering of the emitted photons by changing for example the laser power. All these studies share the resonant excitation scheme which allows for a coherent manipulation of the states of the quantum dot and grants access to phenomena typical for resonance fluorescence such as the Mollow triplet and Rabi oscillations. In particular the experiments on photon excitation spectroscopy and the studies on the dressed biexciton cascade show that fundamental effects of quantum optics can be explored in a scalable and application oriented setting using quantum dots.
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).