Abstract
Calculations combining first-principles electron-phonon (-ph) interactions with the Boltzmann equation enable studies of ultrafast carrier and phonon dynamics. However, in materials with weak Coulomb screening, electrons and holes form bound excitons so their scattering processes become correlated, posing additional challenges for modeling nonequilibrium physics. Here we show calculations of ultrafast exciton dynamics and related time-domain spectroscopies using ab initio exciton-phonon (ex-ph) interactions together with an excitonic Boltzmann equation. Starting from the nonequilibrium exciton populations, we develop simulations of time-domain absorption and photoemission spectra that take into account electron-hole correlations. We use this method to study monolayer , where our calculations predict subpicosecond timescales for exciton relaxation and valley depolarization and reveal the key role of intermediate dark excitons. The approach introduced in this paper enables a quantitative description of nonequilibrium dynamics and ultrafast spectroscopies in materials with strongly bound excitons.
- Received 13 October 2022
- Revised 23 November 2022
- Accepted 25 November 2022
DOI:https://doi.org/10.1103/PhysRevResearch.4.043203
Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article's title, journal citation, and DOI.
Published by the American Physical Society