Time-dependent density functional theory for a unified description of ultrafast dynamics: pulsed light, electrons, and atoms in crystalline solids

TL;DR

This paper introduces a multiscale computational approach combining time-dependent density functional theory with electromagnetic field dynamics to model ultrafast phenomena in crystalline solids, demonstrated through a diamond phonon experiment.

Contribution

A novel multiscale method integrating light, electrons, and atoms dynamics in solids using first-principles simulations for ultrafast optical phenomena.

Findings

Successfully modeled coherent phonon dynamics in diamond.

Captured Raman amplification during probe pulse propagation.

Validated the method's applicability to nonlinear ultrafast optics.

Abstract

We have developed a novel multiscale computational scheme to describe coupled dynamics of light electromagnetic field with electrons and atoms in crystalline solids, where first-principles molecular dynamics based on time-dependent density functional theory is used to describe the microscopic dynamics. The method is applicable to wide phenomena in nonlinear and ultrafast optics. To show usefulness of the method, we apply it to a pump-probe measurement of coherent phonon in diamond where a Raman amplification takes place during the propagation of the probe pulse.