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Real-Time Exciton Dynamics with Time-Dependent Density-Functional Theory.

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|August 30, 2021
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Summary
This summary is machine-generated.

Real-time time-dependent density-functional theory (TDDFT) models excitons using a novel vector potential. This approach accurately captures exciton dynamics in materials, offering insights into optical spectra.

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Area of Science:

  • Computational Physics
  • Quantum Chemistry
  • Materials Science

Background:

  • Linear-response time-dependent density-functional theory (TDDFT) is established for describing excitonic features in optical spectra.
  • Accurate modeling requires specific exchange-correlation (xc) kernels, particularly those behaving as -1/k^{2}.

Purpose of the Study:

  • To demonstrate the modeling of excitons within a real-time TDDFT framework.
  • To investigate the dynamics of excitons following short-pulse excitations.
  • To assess the consistency and applicability of the real-time approach in both linear and nonlinear regimes.

Main Methods:

  • Development of a real-time TDDFT approach utilizing an xc vector potential.
  • Construction of the xc vector potential from approximate, long-range corrected xc kernels.
  • Application to various materials to validate the method.

Main Results:

  • The real-time TDDFT approach is consistent with frequency-dependent linear response calculations.
  • The method provides access to femtosecond exciton dynamics after short-pulse excitations.
  • The approach shows potential for extension into the nonlinear optical regime with careful consideration.

Conclusions:

  • Real-time TDDFT offers a viable and consistent method for modeling excitons and their dynamics.
  • This approach enhances the understanding of optical spectra in insulators and semiconductors.
  • The method opens new avenues for studying ultrafast phenomena in materials.