Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

Abstract

First-principles calculations of e−ph interactions are becoming a pillar of electronic structure theory. However, the current approach is incomplete. The piezoelectric (PE) e−ph interaction, a long-range scattering mechanism due to acoustic phonons in noncentrosymmetric polar materials, is not accurately described at present. Current calculations include short-range e−ph interactions (obtained by interpolation) and the dipolelike Frölich long-range coupling in polar materials, but lack important quadrupole effects for acoustic modes and PE materials. Here we derive and compute the long-range e−ph interaction due to dynamical quadrupoles, and apply this framework to investigate e−ph interactions and the carrier mobility in the PE material wurtzite GaN. We show that the quadrupole contribution is essential to obtain accurate e−ph matrix elements for acoustic modes and to compute PE scattering. Our work resolves the outstanding problem of correctly computing e−ph interactions for acoustic modes from first principles, and enables studies of e−ph coupling and charge transport in PE materials.