Work

Nonlinear polarization evolution using time-dependent density functional theory

Year: 2019

Type: article

Abstract: We propose a theoretical and computational approach to investigate temporal behavior of a nonlinear polarization in a perturbative regime induced by an intense and ultrashort pulsed electric field. First-principles time-dependent density functional theory is employed to describe the electron dynamics. Temporal evolution of third-order nonlinear polarization is extracted from a few calculations of electron dynamics induced by pulsed electric fields with the same time profile but different amplitudes. We discuss characteristic features of the nonlinear polarization evolution as well as an extraction of nonlinear susceptibilities and time delays by fitting the polarization. We also carry out a decomposition of temporal and spatial changes in the electron density in power series with respect to the field amplitude. It helps to get insight into the origin of the nonlinear polarization in atomic scale.

Source: The Journal of Chemical Physics

DOI: 10.1063/1.5068711

Authors: Mitsuharu Uemoto, Yuki Kuwabara, Shunsuke A. Sato, Kazuhiro Yabana

Institutions: University of Tsukuba, Max Planck Institute for the Structure and Dynamics of Matter

Language: English

Topic: Laser-Matter Interactions and Applications

Subfield: Atomic and Molecular Physics, and Optics

Field: Physics and Astronomy

Domain: Physical Sciences

Open Access status: bronze

Funders: Ministry of Education, Culture, Sports, Science and Technology, University of Tsukuba, Japan Society for the Promotion of Science, Core Research for Evolutional Science and Technology

Awards: G1136630272, G2583623727, Investigation for interaction of matter with extreme pulsed light based on first-principles calculations, G6718509927, G7879866177