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Towards Violation of Classical Inequalities using Quantum Dot Resonance Fluorescence

M. Peiris

Published Jan 1, 2017• 0 citations
OpenAlex

Abstract

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.

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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.
Two-color second-order correlations of the light scattered near-resonantly by a quantum dot were measured by means of spectrally filtered coincidence detection. The effects of filter frequency and bandwidth were studied under monochromatic laser excitation, and a complete two-photon spectrum was reconstructed. The two-photon spectrum exhibits a rich structure associated with both real and virtual two-photon transitions down the ``dressed states'' ladder. Photon pairs generated via virtual transitions are found to violate the Cauchy-Schwarz inequality by a factor of 60. Our experiments are well described by the theoretical expressions obtained by del Valle et al. [Phys. Rev. Lett. 109, 183601 (2012)] via time- and normally-ordered correlation functions.
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.
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.
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.
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.
Recently, the concept of an ''NNN-photon spectrum'' -- a spectrally resolved NNN-photon correlation function -- has been introduced as an innovative quantum optics characterization tool that uniquely reveals information about pathways underlying the generation of light in a given source. Here, the authors investigate experimentally the three-photon spectrum of resonance fluorescence from a single semiconductor quantum dot. The observations agree with previous theoretical work, revealing significantly more pronounced photon antibunching at the Mollow triplet sidebands and more strongly correlated emission through virtual states compared to the two-photon counterpart.