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Towards time-dependent current-density-functional theory in the non-linear regime.

J M Escartín1, M Vincendon1, P Romaniello2

  • 1Université de Toulouse, UPS, Laboratoire de Physique Théorique, IRSAMC, F-31062 Toulouse Cedex, France.

The Journal of Chemical Physics
|March 2, 2015
PubMed
Summary
This summary is machine-generated.

Time-Dependent Current-Density-Functional Theory (TDCDFT) advances beyond limitations of TDDFT for irradiation processes. An approximation to the Vignale-Kohn functional enables real-time calculations, revealing insights into relaxation dynamics in atomic systems.

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Area of Science:

  • Quantum chemistry
  • Theoretical physics
  • Computational materials science

Background:

  • Time-Dependent Density-Functional Theory (TDDFT) with the adiabatic local density approximation (ALDA) has limitations in describing dynamic processes due to neglecting memory and long-range effects.
  • Time-Dependent Current-Density-Functional Theory (TDCDFT) offers a potential improvement by utilizing current density and incorporating dissipation, particularly with the Vignale-Kohn (VK) functional in the linear regime.

Purpose of the Study:

  • To extend TDCDFT beyond the linear regime into the time domain for describing irradiation processes.
  • To develop a computationally feasible approximation to the Vignale-Kohn functional for real-time dynamics calculations.
  • To investigate the time-dependent dipole moments and relaxation dynamics in atomic systems (Ca, Mg, Na2) under excitation.

Main Methods:

  • Development of an approximate Vignale-Kohn functional to overcome computational challenges in TDCDFT.
  • Real-time simulation of the time-dependent dipole moment for selected atomic systems.
  • Analysis of relaxation times in relation to deposited excitation energy.

Main Results:

  • The proposed approximate VK functional allows for real-time calculations while retaining key physics.
  • Calculated time-dependent dipole moments for Ca, Mg, and Na2 show trends consistent with previous studies.
  • In the non-linear regime, relaxation times were observed to be independent of excitation energy, indicating limitations for highly excited states.

Conclusions:

  • The developed approximate TDCDFT approach provides a viable method for studying non-linear dynamics in atomic and molecular systems.
  • The findings highlight the importance of accounting for memory and long-range effects in describing irradiation processes.
  • The observed behavior of relaxation times suggests constraints on the applicability of TDCDFT for very high energy excitations.