English

First-principles electron-phonon scattering in real-time TDDFT

Materials Science 2026-07-19 v1

Abstract

Real-time time-dependent density functional theory provides a first-principles description of coherent electron dynamics in laser-driven solids, but its unitary formulation cannot capture the irreversible scattering, relaxation, and decoherence processes that drive excited carriers toward equilibrium. Here, we develop a dissipative rt-TDDFT framework in which first-principles electron-phonon interactions enter the evolution of the reduced one-body density matrix through self-energy-derived collision integrals within the Born-Markov approximation. The approach retains the quantum-coherent real-time propagation of the electronic system while introducing phonon-mediated transitions that redistribute carriers in energy and crystal momentum, thereby incorporating the microscopic momentum-transfer processes responsible for relaxation in real materials. The resulting framework provides a practical first-principles route to simulate relaxation, decoherence, and time-resolved spectroscopic signatures in realistic crystalline materials.

Cite

@article{arxiv.2607.17265,
  title  = {First-principles electron-phonon scattering in real-time TDDFT},
  author = {Zhengwei Nie and Subhojit Pal and Marti Lüders and Alexander Buccheri and Hannes Hübener and Shunsuke A. Sato and Umberto De Giovannini},
  journal= {arXiv preprint arXiv:2607.17265},
  year   = {2026}
}