Frequency-dependent electron-phonon coupling and vibrational responses in tight-binding and continuous Dirac models with nuclear velocity correction

Abstract

The nuclear motion induces in the electronic atomic orbitals a nuclear-velocity-dependent phase (also known as electron-translation factor), which modifies the effective Hamiltonians constructed from localised atomic orbitals. In this work, using an Ehrenfest Lagrangian approach for the localised atomic orbitals (LCAO) and tight-binding methods, we determine, at any order in the nuclear velocity, the equations of motion and the vibrational responses within a linear response formalism, focusing on the tight-binding assessment of the Born effective charges and the force-constant matrix. The appearance of nuclear-velocity-dependent Peierls-like phases in the non-local part of the interactions restores the all-electron sum rules for frequency-dependent vibrational responses. In tight-binding models these corrections crucially modify the vibrational response from a qualitative point of view, also yielding contributions required to capture phenomena such as vibrational circular dichroism. We test these corrections in the tight-binding model for metallic gapped graphene - finding excellent agreement with \textit{ab initio} calculations - and for the topological time-reversal symmetry breaking Haldane model.