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Relativistic Two-Component Particle-Particle Tamm-Dancoff Approximation.

David Williams-Young1, Franco Egidi1, Xiaosong Li1

  • 1Department of Chemistry, University of Washington , Seattle, Washington 98195, United States.

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We extended the particle-particle Tamm-Dancoff approximation to include relativistic effects in excited states. This new method accurately calculates fine structure splittings in atomic and molecular systems.

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Area of Science:

  • Quantum Chemistry
  • Relativistic Effects in Excited States

Background:

  • Particle-particle random-phase and Tamm-Dancoff approximations enable studying challenging systems like diradicals.
  • Current methods are limited to spin-collinear systems, excluding noncollinearity and spin-orbit effects in excited states.

Purpose of the Study:

  • Extend the particle-particle Tamm-Dancoff approximation to handle two-component Hamiltonians.
  • Explicitly incorporate relativistic effects in excited-state calculations.

Main Methods:

  • Theoretical extension of the particle-particle Tamm-Dancoff approximation.
  • Implementation for two-component Hamiltonians.
  • Evaluation of fine structure splittings.

Main Results:

  • Successfully extended the particle-particle Tamm-Dancoff approximation to include relativistic effects.
  • Demonstrated the accuracy of the extended method.
  • Accurate calculation of fine structure splittings for atomic and molecular systems.

Conclusions:

  • The new method enables the study of relativistic excited states.
  • Provides a more comprehensive approach to quantum chemical calculations.
  • Opens avenues for investigating complex molecular systems with spin-orbit coupling.