Two-Dimensional Spectroscopy of Two-Dimensional Materials

Lachlan P Lindoy, Yao-Wen Chang, David R Reichman

Published 2022-06-03Version 1

In this work we provide an exact and efficient numerical approach to simulate multi-time correlation functions in the Mahan-Nozi\`{e}res-De Dominicis model, which crudely mimics the spectral properties of doped two-dimensional semiconductors such as monolayer transition metal dichalcogenides. We apply this approach to study the coherent two-dimensional electronic spectra of the model. We show that several experimentally observed phenomena, such as peak asymmetry and coherent oscillations in the waiting-time dependence of the trion-exciton cross peaks of the two-dimensional rephasing spectrum, emerge naturally in our approach. Additional features are also present which find no correspondence with experimentally expected behavior. We trace these features to the infinite hole mass property of the model. We use this understanding to construct an efficient approach which filters out configurations associated with the lack of exciton recoil, enabling the connection to previous work and providing a route to the construction of realistic two-dimensional spectra over a broad doping range in two-dimensional semiconductors.