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Semiconductor Science and Technology

Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

Gaël Nardin

Published Nov 16, 2015• 14 citations
Publisher

Abstract

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.

DOI
10.1088/0268-1242/31/2/023001

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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.
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.
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.
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.
In article number 1800171, Christopher L. Smallwood and Steven T. Cundiff introduce a multidimensional coherent spectroscopy (MDCS) probe of the dynamics of excitons in an asymmetric In0.05Ga0.95As/GaAs double quantum well. Spectral information here is plotted as a correlation between the frequency of a first-order optical excitation interaction (ωτ) and a third-order emission interaction (ωt) at various intermediate-state mixing times (T), providing a window into a semiconductor's inhomogeneity, many-body interactions, and coherent coupling dynamics at femtosecond timescales. Image credit: Brad Baxley, Part to Whole.
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.