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Nonlinear polarization evolution using time-dependent density functional theory.

Mitsuharu Uemoto1, Yuki Kuwabara2, Shunsuke A Sato3

  • 1Center for Computational Sciences, University of Tsukuba, 1-1-1 Tennodai, Tsukuba, Ibaraki, Japan.

The Journal of Chemical Physics
|March 10, 2019
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Summary
This summary is machine-generated.

We developed a new computational method to study nonlinear polarization dynamics in materials. This approach uses first-principles time-dependent density functional theory to analyze electron behavior under intense electric fields.

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Area of Science:

  • Quantum mechanics
  • Computational physics
  • Materials science

Background:

  • Understanding electron dynamics is crucial for designing new materials.
  • Nonlinear optical phenomena are key to advanced technologies.
  • Pulsed electric fields induce complex electronic responses.

Purpose of the Study:

  • To develop a theoretical and computational framework for investigating nonlinear polarization.
  • To analyze the temporal behavior of electron dynamics under intense ultrashort pulsed electric fields.
  • To extract nonlinear susceptibilities and time delays from simulations.

Main Methods:

  • Utilizing first-principles time-dependent density functional theory (TD-DFT).
  • Performing calculations with pulsed electric fields of varying amplitudes.
  • Analyzing electron dynamics and nonlinear polarization evolution.
  • Decomposing electron density changes into power series.

Main Results:

  • Successfully extracted temporal evolution of third-order nonlinear polarization.
  • Identified characteristic features of nonlinear polarization.
  • Determined nonlinear susceptibilities and time delays through fitting.
  • Gained atomic-scale insights into the origins of nonlinear polarization.

Conclusions:

  • The proposed method effectively captures nonlinear polarization dynamics.
  • TD-DFT provides a robust tool for studying electron responses to pulsed fields.
  • The findings offer a deeper understanding of light-matter interactions at the atomic level.