Quantum spectroscopy in solids directly detects nonlinear changes created exclusively by quantum fluctuations of light. So far, it has been realized only by projecting a large set of measurements with a coherent-state laser to a specific quantum-light response. We present two complementary experimental approaches to realize intense and ultrafast thermal-state sources. We investigate the effects of continuous excitation from a superluminescent diode (SLD) as well as an ensemble-averaging technique using phase-modulated pulses. By measuring excitonic nonlinearities in gallium arsenide, we demonstrate that the experimentally realized thermal-state source produces significantly reduced many-body nonlinearities compared to a coherent-state excitation. We also review experimental approaches toward future realization of quantum spectroscopy with thermal states.
Quantum spectroscopy in solids directly detects nonlinear changes created exclusively by quantum fluctuations of light. So far, it has been realized only by projecting a large set of measurements with a coherent-state laser to a specific quantum-light response. We present two complementary experimental approaches to realize intense and ultrafast thermal-state sources. We investigate the effects of continuous excitation from a superluminescent diode (SLD) as well as an ensemble-averaging technique using phase-modulated pulses. By measuring excitonic nonlinearities in gallium arsenide, we demonstrate that the experimentally realized thermal-state source produces significantly reduced many-body nonlinearities compared to a coherent-state excitation. We also review experimental approaches toward future realization of quantum spectroscopy with thermal states.
Quantum spectroscopy utilizes the quantum fluctuations of the light source to characterize and control matter. More specifically, desired many-body states can be directly excited to the semiconductor by adjusting light source's quantum fluctuations. The method is experimentally realizable by projecting an extensive set of classical measurements into a quantum-optical response resulting from any possible quantum source. In this work, quantum spectroscopy is used to identify new classes of many-body states and quantum processes in semiconductor nanostructures. In the first part of this Thesis, the optical properties of semiconductor quantum wells are analyzed with quantum spectroscopy by projecting high-precision optical measurements into quantum-optical responses. It is shown that quantum spectroscopy can characterize the properties of specific stable electron-hole cluster – called quasiparticles – much more sensitively than traditional ultrafast laser spectroscopy. In particular, unambiguous evidence is demonstrated for the identification of a new highly correlated quasiparticle in direct-gap Galliumarsenide quantum wells, the dropleton, that is a quantum droplet consisting of four-to-seven electron-hole pairs. To determine the detectable excitation energetics of such correlated quasiparticles in optically excited semiconductor quantum wells, a new theoretical framework is presented which allows for the computation of the excitation spectrum based on a pair-correlation function formulation of the quasiparticle state. Another study in this Thesis deals with the emission properties of optically pumped quantum-dot microcavities. Experimental and theoretical evidence is shown for a new intriguing quantum-memory effect that is controllable by adjusting pump source's quantum fluctuations. The last part of this Thesis presents a fundamental study about the general applicability of quantum spectroscopy in dissipative systems.
The three-dimensional confinement created by the ultrasmall semiconductor structures known as quantum dots greatly modifies the optical properties of the spatially localized carriers. These systems are presently of great interest to the research community, both for the improved understanding of the physics of confined structures, and for the potential applications of these systems to areas such as optoelectronics and quantum computing. Here, the techniques of transient coherent nonlinear optical spectroscopy are applied to the investigation of excitons confined within InAs/GaAs self-assembled quantum dots. These methods provide a powerful tool for the study of dynamic processes in these novel materials. The nonlinear measurements are based on the differential transmission experimental geometry, and utilize ultrafast pulsed lasers in order to temporally resolve the carrier dynamics after excitation. The experiments performed here are resonant with the ground state absorption of the quantum dots, as evidenced by comparison with the photoluminescence measurements which are used to characterize the sample. The incoherent relaxation dynamics of the population of photoexcited excitons are examined, allowing for a determination of both the lifetime of the excitons and the time scale for relaxation between the two polarization eigenstates of the system. The three-dimensional quantum confinement results in the suppression of these relaxation processes, as predicted. The use of coherent spectroscopic techniques allows for the first unambiguous demonstration of an optically-induced nonradiative Raman coherence in these quantum dots. Simultaneous excitation of both polarization states of the exciton results in a coherent superposition state, whose temporal evolution is observed through the homodyne-detection scheme. In these transient experiments, this is manifested as a beating in the nonlinear response, which allows us to directly measure the fine-structure splitting between the polarization states. Utilizing optical pulse shaping techniques, transient spectral hole burning is performed, which allows for the nonlinear response to be spectrally resolved. As expected for the strongly confined quantum dot excitons, the results show that diffusion among the localized states is not a significant effect. Temperature dependent measurements show that at elevated temperatures, extra dephasing processes, potentially related to acoustic phonon scattering, become important. Finally, this technique allows for the first direct observation of the induced absorption from the exciton to biexciton transition in these InAs quantum dots, and a measurement of the associated binding energy. These results lay the foundation for future studies in this material system, and for the possible development of quantum logic devices utilizing quantum dots.
This thesis presents experiments carried out into the coherent properties of charge carriers confined within a single InGaAs/GaAs quantum dot. Specifically the ground state - single exciton qubit system is controlled with ultrafast optical pulses and then the population of the dot is measured by a high-sensitivity photocurrent detection technique. There are two principal results of these experiments, firstly by modulating the bias applied to the quantum dot diode, the detection efficiency of the photocurrent measurement technique is enhanced. The enhancement is possible as the modulated bias allows fast switching of the voltage-dependent carrier tunneling rates. Secondly, when the transition is addressed by an intense, positively detuned laser, the qubit system can be driven to a population inversion. This occurs due to phonon-assisted relaxation of the optical dressed states of the system. Here, the rapid thermalization due to the exciton-phonon interaction actually enables the population inversion, instead of simply being a source of decoherence.
Multi-dimensional coherent spectroscopy (MDCS) has become an extremely versatile and sensitive technique for elucidating the structure, composition, and dynamics of condensed matter, atomic, and molecular systems. The appeal of MDCS lies in its ability to resolve both individual-emitter and ensemble-averaged dynamics of optically created excitations in disordered systems. When applied to semiconductors, MDCS enables unambiguous separation of homogeneous and inhomogeneous contributions to the optical linewidth, pinpoints the nature of coupling between resonances, and reveals signatures of many-body interactions. In this review, we discuss the implementation of MDCS to measure the nonlinear optical response of excitonic transitions in semiconductor nanostructures. Capabilities of the technique are illustrated with recent experimental studies that advance our understanding of optical decoherence and dissipation, energy transfer, and many-body phenomena in quantum dots and quantum wells, semiconductor microcavities, layered semiconductors, and photovoltaic materials.
We review the nonlinear-optical effects observed at room temperature in semiconductor quantum-well structures photoexcited near the band gap. A comprehensive discussion of optical transitions in these microstructures is given, including excitonic effects and the specific features of room-temperature exciton resonances. Experimental investigations using continuous-wave, picosecond-, and femtosecond-laser sources are presented. They show extremely efficient nonlinear processes. In the case of excitations that are long compared with the exciton-ionization time, the induced changes in absorption and refraction do not depend on the wavelength or on the duration of excitation. These changes depend only on the density of absorbed photons and are interpreted in terms of electron–hole plasma screening and band filling. In contrast, for ultrashort excitation, nonlinear processes depend critically on the excitation wavelength. The selective generation of excitons is found to produce effects larger than a plasma of the same density. This unexpected result is shown to arise from the low temperature of the exciton gas before it interacts with the lattice and from the decrease of screening that is the reduced dimensionality of quantum-well structures.
In the previous chapters, we have seen that quantum-optical correlations can produce effects that have no classical explanation. In particular, the matter excitations can depend strongly on the specific form of the quantum fluctuations, i.e., the quantum statistics of the light source. For example, Fock-state sources can produce quantum Rabi flopping with discrete frequencies while coherent-state sources generate a sequence of collapses and revivals in atomic excitations. Hence, not only the intensity or the classical amplitude of the field is relevant but also the quantum statistics of the exciting light influences the matter response. Even if we take sources with identical intensities, the resulting atomic excitations are fully periodic for a Fock-state excitation while a coherentstate excitation produces a chaotic Bloch-vector trajectory with multiple collapses and revivals. In this chapter, we use this fundamental observation as the basis to develop the concept of quantum-optical spectroscopy. We show in Chapter 30 that this method yields a particularly intriguing scheme to characterize and control the quantum dynamics in solids. Since one cannot imagine how to exactly compute the many-body wave function or the density matrix, we also study how principal quantum-optical effects can be described with the help of the cluster-expansion scheme. Quantum-optical spectroscopy Historically, the continued refinement of optical spectroscopy and its use to manipulate the states of matter has followed a very distinct path where one simultaneously tries to control and characterize light with increased accuracy.