Nonequilibrium photocarrier and phonon dynamics from first principles: a unified treatment of carrier-carrier, carrier-phonon, and phonon-phonon scattering

Abstract We develop a first-principles many-body framework to describe photocarrier and phonon dynamics in semiconductors after ultrafast excitation. The method includes explicit ab initio light-matter coupling, collision integrals for carrier-carrier, carrier-phonon, and phonon-phonon scattering, time-dependent quasiparticle and phonon-frequency renormalizations, and light-induced coherent atomic motion. The equations of motion are solved in a maximally localized Wannier basis, ensuring gauge-consistent scattering integrals and allowing for dense momentum sampling, enabling direct comparison with pump-probe experiments. The framework is computationally efficient, scalable, and can be combined with constrained density-functional theory to study longer-time light-induced structural phase transitions. We demonstrate the method for MoS 2 and h-BN monolayers. In MoS 2 , it captures photoinduced renormalizations of electronic and lattice properties, ultrafast carrier relaxation, hot-phonon dynamics, and coherent atomic motion. Including carrier-carrier scattering is essential for realistic photocarrier equilibration, while neglecting phonon-phonon scattering yields incorrect long-time lattice thermalization and overestimates the A 1 g coherent-phonon damping time by a factor of two. In h-BN, we quantify photoinduced changes in the electronic, optical, and lattice responses in quasi-equilibrium, demonstrating a fluence-dependent enhancement of screening and melting of excitonic features.