Zero-Point Renormalization Reshapes the Shift Current: The Role of Electron-Phonon Coupling

Abstract

Shift current (SC) drives the bulk photovoltaic effect, holding promise for near-instantaneous, low-dissipation photodetection and energy conversion. The current understanding of SC relies primarily on a single-particle picture, in which the SC is determined purely by band dispersion. While many-body effects from directly excited quasiparticles, such as excitons, magnons and phonons, have been explored, the renormalization of electronic states by quantum virtual-phonon coupling --- inherent in essentially all solids and particularly decisive for transport --- remains unaddressed. Here, using first-principles calculations, we identify this missing channel --- band-renormalized shift current (BRSC) --- in monolayer MoS2. We find that the zero-point renormalization alone, without any polarization-carrying photoexcited phonons and with barely any alteration of the band dispersion, dramatically reshapes the SC spectrum: emergent low-energy peaks arise from phonon-assisted optical transitions between momentum-distinct states, with a pronounced redshift of higher-energy features. A mere 1.0% strain sharply tunes the BRSC, whereas raising the temperature enhances it. Our findings overturn the band-structure-only paradigm, establishing electron-phonon coupling as an indispensable ingredient for nonlinear photocurrent and opening a strain-thermal route for engineering next-generation optoelectronic responses.