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Physical Review B

Characterizing biexciton coherences with quantum spectroscopy

Martin Mootz, M. Kira, S. W. Koch, Andrew E. Almand-Hunter, Steven T. Cundiff

Published Apr 2, 2014• 15 citations
Publisher

Abstract

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.

DOI
10.1103/physrevb.89.155301

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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.
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.
We report on large optical nonlinear effects induced by coherent interactions between excitons and biexcitons in quantum dots. The absorption spectra in an exciton–biexciton system are measured in InGaAs quantum dots by using single dot spectroscopy. The spectra exhibit unusual shapes that have a transparent region under a strong excitation condition. A pump–probe measurement ensures that the exciton state is erased by a quantum interference effect with exciton and biexciton photoabsorption processes. These results suggest that optical functions such as electromagnetically induced transparency are feasible with excitons and biexcitons in quantum dots.
Exciton-biexciton coherent coupling effects are examined in semiconductor quantum dots. The exciton absorption spectrum is measured with the microphotoluminescence excitation technique in a single InGaAs quantum dot. The spectrum changes from a Lorenztian-type line shape to an unusual dip-shaped line shape with increasing excitation intensities in a higher exciton state where there is a large oscillator strength between the exciton and biexciton states. The intensity dependence of the dip energy width clearly indicates that coherent Rabi oscillation occurs between the exciton and biexciton states. The absorption properties with excitation light of different polarizations show that the dip-shaped spectra only appear when there is a large biexciton state population with linear polarization. A theoretical analysis undertaken with the density matrix method agrees well with experimental results. This agreement reveals that exciton-biexciton coherent interactions lead to unusual absorption spectra and contribute crucially to the optical properties of quantum dots. The exciton-biexciton coherent effects provide a scheme for controlling four distinguishable states, which can be applied to a demonstration of quantum gate operations.
Abstract Signatures of exciton and two‐exciton states in semiconductor systems are investigated experimentally and theoretically. A set of quantum well samples with different well widths is studied using coherent excitation spectroscopy. The experimental results are analyzed using a microscopic model demonstrating the importance of biexciton correlations and disorder effects. Additional numerical investigations of absorption changes in small nanorings are employed to analyze optical transitions from two‐exciton to three‐exciton resonances.
Fourier transform spectroscopy with classical interferometry corresponds to the measurement of a single-photon intensity spectrum from the viewpoint of the particle nature of light. In contrast, the Fourier transform of two-photon quantum interference patterns provides the intensity spectrum of the two photons as a function of the sum or difference frequency of the constituent photons. This unique feature of quantum interferometric spectroscopy offers a different type of spectral information from the classical measurement and may prove useful for nonlinear spectroscopy with two-photon emission. Here, we report the first experimental demonstration of two-photon quantum interference of photon pairs emitted via biexcitons in the semiconductor CuCl. Besides applying Fourier transform to quantum interference patterns, we reconstruct the intensity spectrum of the biexciton luminescence in the two-photon sum or difference frequency. We discuss the connection between the reconstructed spectra and exciton states in CuCl as well as the capability of quantum interferometry in solid-state spectroscopy.