Time-dependent density functional theory for interaction of ultrashort light pulse with thin materials

TL;DR

This paper develops a first-principles time-dependent density functional theory framework to model ultrashort light pulse interactions with thin materials, capturing complex electromagnetic and electronic dynamics, and proposes simplified models for different thickness regimes.

Contribution

The authors introduce the microscopic Maxwell-TDDFT scheme for thin materials and derive approximate models for extremely thin and thick films, enhancing understanding of light-matter interactions at the nanoscale.

Findings

The scheme accurately describes electronic structure and nonlinear interactions.

Approximate models work well for extreme thin and thick regimes.

Comparison with macroscopic electromagnetism validates the models.

Abstract

We present a comprehensive theoretical description for an irradiation of an ultrashort light pulse normally on thin materials based on first-principles time-dependent density functional theory. As the most elaborate scheme, we develop a microscopic description solving Maxwell equations for light electromagnetic fields and the time-dependent Kohn-Sham equation for electron dynamics simultaneously in the time domain using a common spatial grid. We call it the microscopic Maxwell-TDDFT scheme. We test this scheme for silicon thin films of various thickness, from a few atomic layers to a few tens of nm. We show that the microscopic Maxwell-TDDFT scheme provides a satisfactory description incorporating the electronic structure of thin films in the first-principles level, multiple reflections of the electromagnetic fields at the surfaces, and nonlinear light-matter interaction when the incident light pulse is strong. However, the calculation becomes expensive as the thickness increases. We then consider two limiting cases of extremely thin and sufficiently thick films and develop approximate schemes. For the extremely thin case including two-dimensional atomic-layered materials, a two-dimensional macroscopic electromagnetism is developed: a two-dimensional susceptibility is introduced for a weak field, while time evolution equation is derived for an intense field. For sufficiently thick films, the microscopic Maxwell-TDDFT scheme is expected to coincide with a description utilizing ordinary macroscopic electromagnetism. We numerically confirm it comparing the calculated results: For a weak field, a comparison is made with a description using the bulk dielectric susceptibility. For a strong field, a comparison is made with a multiscale Maxwell-TDDFT scheme which the authors' group developed previously.