Ab initio electron-two-phonon scattering in GaAs from next-to-leading order perturbation theory

Electron-phonon ( e –ph) interactions are usually treated in the lowest order of perturbation theory. Here we derive next-to-leading order e –ph interactions, and compute from first principles the associated electron-two-phonon (2ph) scattering rates. The derivations involve Matsubara sums of two-loop Feynman diagrams, and the numerical calculations are challenging as they involve Brillouin zone integrals over two crystal momenta and depend critically on the intermediate state lifetimes. Using Monte Carlo integration together with a self-consistent update of the intermediate state lifetimes, we compute and converge the 2ph scattering rates, and analyze their energy and temperature dependence. We apply our method to GaAs, a weakly polar semiconductor with dominant optical-mode long-range e –ph interactions. We find that the 2ph scattering rates are as large as nearly half the value of the one-phonon rates, and that including the 2ph processes is necessary to accurately predict the electron mobility in GaAs from first principles. Electron-phonon scattering plays a decisive role in electron transport and is taken into account in ab initio calculations by leading-order perturbations involving scattering events with one phonon. Here, the authors show that higher-order effects are comparable in magnitude to the leading order in polar semiconductors.