Lineshape Analysis of Double-Quantum Multidimensional Coherent Spectra

TL;DR

This paper models double-quantum 2D spectra using optical Bloch equations to understand peak lineshapes and correlation effects, clarifying discrepancies in experimental results across different studies.

Contribution

It introduces a theoretical model that explains lineshape features and correlation effects in double-quantum 2D spectra, addressing inconsistencies in experimental observations.

Findings

Correlation between coupled resonances affects lineshape.

Model explains discrepancies in experimental spectra.

Provides a framework for interpreting double-quantum spectra.

Abstract

Double-quantum two-dimensional coherent spectroscopy (MDCS) is a powerful optical method that is used to study optical properties of atomic and complex molecular systems and semiconductor materials. Double-quantum 2D spectra and particularly the peak lineshapes on the spectra can also provide information about many-body interactions. We model 2D spectra by solving the optical Bloch equations and show the effects of correlation between coupled resonances, which also explains the discrepancies between the experimental results reported by multiple groups.