Multidimensional coherent optical spectroscopy of semiconductor nanostructures: a review

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.

Multidimensional Coherent Spectroscopy of Semiconductors

“…Although the roots of MDCS can be traced to the development of 2D nuclear magnetic resonance (2D‐NMR) by Ernst and collaborators in the 1970s, advances in both laser development and interferometric stabilization have pushed the technique far beyond its radio‐frequency origins, extending it into the infrared regime, the optical regime, and in a few recent cases even into the ultraviolet . Today, optical MDCS (with a wavelength range of 400–1000 nm) has emerged as a powerful method for studying properties ranging from many‐body dynamics in semiconductors to energy‐transfer processes in photosynthetic light harvesting complexes to interactions and dynamics in atomic and molecular vapors and solutions …”

Incoherent population mixing contributions to phase-modulation two-dimensional coherent excitation spectra

“…Multidimensional coherent optical spectroscopy has emerged as a powerful tool to unravel various electronic and vibrational coherent phenomena, to separate homogeneous and inhomogeneous linewidth contributions, and to dissect excitation dynamics with intricate detail beyond that routinely afforded by unidimensional ultrafast spectroscopic methods. [1][2][3][4] Numerous experimental implementations of 2D coherent spectroscopy have been developed over the last decade, each with unique advantages and disadvantages, providing the ultrafast spectroscopy community an extensive menu of experimental schemes. 3 In this work, we focus on population-detected 2D Fourier transform spectroscopy via phase modulation.…”

Two-dimensional infrared spectroscopy of vibrational polaritons of molecules in an optical cavity

“…Vibrational polaritons were experimentally reported 6,8,9 and calculated 7,25 recently. Multidimensional spectroscopic studies for electronically excited states in semiconductor cavity for nano-particles like In 0.04 Ga 0.96 As has been demonstrated 12,27 . Similarly, electronic exciton-polariton interactions of quantum wells in microcavity 28 has also been reported.…”