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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Optical two-dimensional coherent spectroscopy of semiconductor nanostructures

Gaël Nardin, Travis M. Autry, Galan Moody, Rohan Singh, Hebin Li, Steven T. Cundiff

Published Sep 5, 2014• 0 citations
Publisher

Abstract

Our recent work on optical two-dimensional coherent spectroscopy (2DCS) of semiconductor materials is reviewed. We present and compare two approaches that are appropriate for the study of semiconductor nanostructures. The first one is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs), or large and dense ensembles of Quantum Dots (QDs). The second method is based on a collinear geometry, where the FWM is detected in the form of a photocurrent. This second approach enables 2DCS of samples where translational symmetry is broken, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. For each method, we provide an example of experimental results obtained on semiconductor QWs. In particular, it is shown how 2DCS can reveal coherent excitonic coupling between adjacent QWs.

DOI
10.1117/12.2062608

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Our recent work on optical two-dimensional coherent spectroscopy (2DCS) of semiconductor materials is reviewed. We present and compare two approaches that are appropriate for the study of semiconductor nanostructures. The first one is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs), or large and dense ensembles of Quantum Dots (QDs). The second method is based on a collinear geometry, where the FWM is detected in the form of a photocurrent. This second approach enables 2DCS of samples where translational symmetry is broken, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. For each method, we provide an example of experimental results obtained on semiconductor QWs. In particular, it is shown how 2DCS can reveal coherent excitonic coupling between adjacent QWs.
We review our recent work on multi-dimensional coherent optical spectroscopy (MDCS) of semiconductor nanostructures. Two approaches, appropriate for the study of semiconductor materials, are presented and compared. A first method is based on a non-collinear geometry, where the Four-Wave-Mixing (FWM) signal is detected in the form of a radiated optical field. This approach works for samples with translational symmetry, such as Quantum Wells (QWs) or large and dense ensembles of Quantum Dots (QDs). A second method detects the FWM in the form of a photocurrent in a collinear geometry. This second approach extends the horizon of MDCS to sub-diffraction nanostructures, such as single QDs, nanowires, or nanotubes, and small ensembles thereof. Examples of experimental results obtained on semiconductor QW structures are given for each method. In particular, it is shown how MDCS can assess coupling between excitons confined in separated QWs.
Abstract Multidimensional coherent optical spectroscopy (MDCS) is an elegant and versatile tool to measure the ultrafast nonlinear optical response of materials. Of particular interest for semiconductor nanostructures, MDCS enables the separation of homogeneous and inhomogeneous linewidths, reveals the nature of coupling between resonances, and is able to identify the signatures of many-body interactions. As an extension of transient four-wave mixing (FWM) experiments, MDCS can be implemented in various geometries, in which different strategies can be used to isolate the FWM signal and measure its phase. I review and compare different practical implementations of MDCS experiments adapted to the study of semiconductor materials. The power of MDCS is illustrated by discussing experimental results obtained on semiconductor nanostructures such as quantum dots, quantum wells, microcavities, and layered semiconductors.
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.
Optical two-dimensional Fourier transform (2DFT) spectroscopy has been developed over the last decade as a powerful tool for studying a variety of physical systems, ranging from atoms to molecules to solids. This review covers our use of 2DFT spectroscopy to study exciton dynamics in semiconductor nanostructures. In quantum wells, 2DFT spectroscopy confirms the importance of many-body contributions to the coherent optical response and reveals nonradiative double-quantum and Raman coherences. For natural quantum dots, 2DFT spectroscopy enables ensemble measurements of the homogeneous linewidth, including the temperature and density dependence. Relaxation from quantum well states into the quantum dots can also be studied using 2DFT spectroscopy.
Abstract Optical multidimensional coherent spectroscopy provides information about the structure and excitation dynamics in a broad range of material systems. This book focuses on systems of interest in physics, including atomic vapors, semiconductor nanostructures and two-dimensional materials. An introduction to ultrafast spectroscopy and the fundamental concepts of multidimensional coherent spectroscopy applies to all material systems. Relevant experimental implementations, including phase-stabilized crossed-beams, frequency-tagged fully-collinear, three-dimensional and frequency-comb based methods. The use of the method to study atomic vapors, semiconductor quantum wells, semiconductor quantum dots and two-dimensional materials are described in separate chapters. The final chapters survey the use of the method in some other areas and speculate on future directions.
Correlated electron-hole pairs, or excitons, in semiconductor nanostructures have been studied extensively over the past few decades. The optical response of excitons is complicated due to inhomogeneous broadening, presence of multiple states, and exciton-exciton interactions. In this work we bring new perspectives to exciton physics in semiconductor quantum wells (QWs) through two-dimensional coherent spectroscopy (2DCS).\nThe effect of QW growth direction on the optical properties of excitons is explored by studying (110)-oriented GaAs QWs. The homogeneous and inhomogeneous linewidths of the heavy-hole exciton resonance are measured. By probing the optical nonlinear response for polarization along the in-plane crystal axes [1-10] and [001], we measure different homogeneous linewidths for the two orthogonal directions. This difference is found to be due to anisotropic excitation-induced dephasing, caused by a crystal-axis-dependent absorption coefficient. The extrapolated zero-excitation density homogeneous linewidth exhibits an activation-like temperature dependence.\nSpectral diffusion of excitons in (001)-oriented QWs has been studied. We show that the spectral diffusion characteristics depend strongly on the sample temperature. Spectral diffusion is generally assumed to follow the strong-redistribution approximation, partly because of lack of any evidence to the contrary. We find that this assumption is violated at low sample temperatures for excitons in QWs; high-energy excitons preferentially relax due to a negligible phonon population at low temperatures. The frequency-frequency correlation function is measured through a numerical fitting procedure to quantify spectral diffusion for sample temperatures >20>20>20 K.\nExciton-exciton interactions affect the light-matter interactions in QWs significantly. We present an intuitive and simple model for these interactions by treating excitons as interacting bosons. We show that the polarization-dependent exciton dephasing rate in GaAs quantum wells is due to the bosonic character of excitons. We fit slices from simulated spectra to those from the experimentally measured spectra and show that interference between two different quantum mechanical pathways results in a slower dephasing rate for co-circular and co-linear polarization of optical excitation pulses. This interference does not exist for cross-linearly polarized excitation pulses resulting in a faster dephasing rate. Additionally, we were able to separately quantify inter- and intra-mode interactions between excitons through exciton-density-dependent measurements.