Multi-dimensional spectroscopy of mobile excitons in two-dimensional semiconductors
Abstract
Multi-dimensional coherent spectroscopy (MDCS) goes beyond standard linear-response probes and provides a powerful tool for investigating correlations between quasiparticles such as excitons (bound electron-hole pairs). Here we present a microscopic theory of MDCS that accounts for the delocalized nature of excitons in two-dimensional semiconductors. In contrast to the more phenomenological few-level approaches typically employed for modelling MDCS, our theory features mobile excitons with continuous momentum degrees of freedom. We find that the energy continuum associated with exciton momenta is crucial for producing interaction-induced decoherence, as well as capturing the interference between different exciton-polaron quasiparticles in the case of charge-doped semiconductors. Crucially, our calculated MDCS spectra agree well with recent experiments on doped monolayer MoSe2 [Hao et al., Nature Communications 8, 15552 (2017)], and they suggest that the interactions between exciton polarons depend strongly on phase-space filling effects, where exciton polarons compete for electrons. Our results demonstrate that microscopic approaches allow one to gain new insights from the fine structure of MDCS on two-dimensional semiconductors, and they illustrate the utility of microscopic approaches to modelling MDCS experiments more generally.
Related
- Sub-diffraction-resolved spatial distribution of emitting excitons in scanning tunneling microscopy-induced luminescence of two-dimensional semiconductors via Richardson-Lucy deconvolution
- Generalized s-d model for Wannier-Mott excitons in layered magnetic semiconductors
- Magnon-induced hybridization brightens excitons in ferromagnetic semiconductors
- Davydov Splitting Without a Davydov Pair and Highly Mobile Singlet Excitons in Perylene Red Microcrystals
- Momentum-selective graphene spectroscopy of moiré excitons
BibTeX
@misc{wheaton2026multidimensional,
title = {{Multi-dimensional spectroscopy of mobile excitons in two-dimensional semiconductors}},
author = {Ned Wheaton and Jeffrey A. Davis and Jesper Levinsen and Meera M. Parish},
howpublished = {arXiv},
year = {2026},
month = aug,
doi = {10.48550/arxiv.2608.27951},
eprint = {2608.27951},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2608.27951},
}
RIS
TY - UNPB
TI - Multi-dimensional spectroscopy of mobile excitons in two-dimensional semiconductors
AU - Ned Wheaton
AU - Jeffrey A. Davis
AU - Jesper Levinsen
AU - Meera M. Parish
PY - 2026
DA - 2026/08/28
PB - arXiv
DO - 10.48550/arxiv.2608.27951
UR - https://arxiv.org/abs/2608.27951
AB - Multi-dimensional coherent spectroscopy (MDCS) goes beyond standard linear-response probes and provides a powerful tool for investigating correlations between quasiparticles such as excitons (bound electron-hole pairs). Here we present a microscopic theory of MDCS that accounts for the delocalized nature of excitons in two-dimensional semiconductors. In contrast to the more phenomenological few-level approaches typically employed for modelling MDCS, our theory features mobile excitons with continuous momentum degrees of freedom. We find that the energy continuum associated with exciton momenta is crucial for producing interaction-induced decoherence, as well as capturing the interference between different exciton-polaron quasiparticles in the case of charge-doped semiconductors. Crucially, our calculated MDCS spectra agree well with recent experiments on doped monolayer MoSe_2 [Hao et al., Nature Communications 8, 15552 (2017)], and they suggest that the interactions between exciton polarons depend strongly on phase-space filling effects, where exciton polarons compete for electrons. Our results demonstrate that microscopic approaches allow one to gain new insights from the fine structure of MDCS on two-dimensional semiconductors, and they illustrate the utility of microscopic approaches to modelling MDCS experiments more generally.
ER -