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.
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.
Nanotechnologically fabricated structures out of compound semiconductor materials make up the functional parts in LEDs, in semiconductor lasers and in electronics components. The small size of the structures evidently leads to requiring the modeling to look at phenomena at the quantum level. Especially for optoelectronical devices, one needs to treat the interaction between light and semiconductor material. This research adds to the understanding of inter-pretations of light-matter interaction phenomena and makes it possible to find totally new and undiscovered functionalities in semiconductor nanostructures. \nThis thesis presents work on modeling and creates new theoretical foundations for phenom-ena appearing in semiconductor quantum structures. Of special interest has been to generate a theoretical description to such phenomena that have been caused by an optical field and in which one sees changes, e.g., in angular momentum or spatial distribution of excited states. Basically, two kinds of structures are examined, quantum rings and wells. A quantum ring is a toroidal object of which volume is very small, but its diameter can be significant when com-pared to the wavelength of light. Another class of systems under study is a double quantum well structure, where there are two quantum wells on both sides of a tunnel barrier. In this system, the type-I and type-II semiconductor band-structure properties become combined in spatial coordinates, since the electrons and holes can occupy either the same or the separate quantum wells. \nThe two most interesting results are the angle-of-emission dependent photoluminescence from the quantum rings and the coherent control of vertical transport of desired quasiparticles through material interfaces in the quantum-well system in a selective manner. Since the ob-tained results on quantum rings are closely connected to the orbital-angular-momentum coupling between light and matter, they can prove to be important in different quantum infor-mation schemes where this angular-momentum aspect of light has been found to be highly beneficial. In quantum optics, there already are visible trends towards this direction. The predicted coherent control in a double-quantum-well system may mean a large technological progress, since by utilizing this effect one can study transport properties between materials over an interface, one of the most interesting examples of such phenomena being the transfer of quantum correlations through the interface without changing the local densities of electrons.
Excitation-induced many-body effects play an important role in semiconductor quantum materials, where ultrafast processes determine the system properties. These effects occur when light excitations dynamically alter light absorption and emission, leading to nonlinear, excitation-induced changes in a semiconductor's optical response. This thesis theoretically investigates ultrafast excitation-induced effects in semiconductor nanostructures. Specifically, using a first-principles analysis based on quantum dynamic cluster expansion, we implement a systematic approach to describe the dynamics of microscopic polarizations and carrier occupations in semiconductor quantum materials precisely, with Coulomb-induced scattering fully included. We explore the dynamic buildup of excitation-induced effects, and develop a quantum memory model to precisely describe it. We also do a perturbative study on the third-order nonlinearities and propose a method based on it to measure the build-up time of excitation-induced effects via ultrafast experiments. Utilizing these theoretical tools, we successfully guided experiments to detect ultrafast processes. We successfully observed the time-delayed buildup of dephasing from the experiments and demonstrated a reversible ultrafast switching that can be switched within femtosecond time scale and is capable for hundreds of switching operations. We also identified nonperturbative ultrafast nonlinearities in the carbon nanotube, with the nonlinear refractive indices orders of magnitude higher than those found from other materials, explained by the strong excitation-induced effects. Our findings are crucial for quantum photonic applications. They offer significant insights into the fundamental quantum processes relevant to ultrafast photonics and open up new possibilities for quantum information and quantum optoelectronics technologies.
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.
The biexciton resonance in the absorption spectra of semiconductor quantum wells is analyzed with quantum-optical spectroscopy by projecting experimental pump-probe measurements into quantum-optical absorption spectra. More specifically, the measurements are converted into phase-space distributions using the cluster-expansion transformation. The quantum-optical responses can then be projected with full convergence, despite the unavoidable experimental noise. The calculations show that classical and quantum excitations produce significantly different results for the biexciton resonance. In particular, quantum-optical spectroscopy monitors the excitation-induced broadening of the biexciton resonance as a function of pump intensity much more sensitively than classical spectroscopy does.
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.