Coherent phonons in photoexcited semiconductors from first principles

Abstract

Coherent phonons are phase-locked lattice vibrations that provide a sensitive probe of nonequilibrium dynamics in materials. Existing first-principles equation-of-motion (EOM) approaches have successfully described coherent phonons in metals and semimetals, but their extension to semiconductors requires treating the long-lived electron--hole plasma created by above-gap excitation. Here we extend the first-principles EOM framework to photoexcited semiconductors by incorporating the residual plasma force that shifts the lattice equilibrium together with the plasma-induced renormalization of the electronic structure. For monolayer MoTe$_2$, the calculated carrier-density-dependent Te displacement agrees with constrained density-functional perturbation theory only when the renormalized band structure is included. We then show that increasing the photoexcited carrier density enhances both the initial total force and the plasma-shifted equilibrium position of the $A_{1g}$ mode, producing larger coherent lattice oscillations. This density-controlled response appears in both the atomic displacement and the coherent-phonon-induced band renormalization, providing complementary signatures for ultrafast reflectivity and time- and angle-resolved photoemission spectroscopy.