2025/03/17 by Steinhoff, Alexander, Jahnke, Frank, Florian, Matthias · 1 citation
#FOS: Physical sciences #Mesoscale and Nanoscale Physics (cond-mat.mes-hall)
paper · doi:10.48550/arxiv.2503.13417
Marrying the predictive power of ab initio calculations with many-body effects remains a challenging task in two-dimensional (2d) materials, where efficient carrier-carrier interaction challenges established approximation schemes. In particular, understanding exciton-phonon interaction from first principles is a field of growing interest. Here, we present a many-body theory for coupled free-carrier, exciton, phonon and photon dynamics based on carrier-carrier and carrier-phonon interaction matrix elements obtained via projection on Wannier orbitals. The framework is applied to study the impact of carrier-phonon correlations on optical spectra and coupled nonequilibrium carrier-phonon kinetics in monolayer MoSe2. We find that non-Markovian effects and dynamical buildup of quasi-particles are only properly described if correlations at least on the two-phonon level are included. Our studies open a perspective to advance the material-realistic description of nonequilibrium physics in 2d nanostructures to new many-body realms.