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Excimer Energies.

Ruoqi Zhao1,2, Christian Hettich3, Jun Zhang2

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A new multistate energy decomposition analysis (MS-EDA) method quantifies excited-state interactions in excimers. This approach reveals exciton coupling, superexchange, and delocalization energies critical for understanding excimer stability.

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Area of Science:

  • Computational Chemistry
  • Quantum Chemistry
  • Theoretical Chemistry

Background:

  • Energy Decomposition Analysis (EDA) is established for ground-state intermolecular interactions.
  • Limited methods exist for analyzing excited-state complexes like excimers.

Purpose of the Study:

  • Introduce a novel Multistate Energy Decomposition Analysis (MS-EDA) for excimers.
  • Provide a theoretical framework to dissect excited-state interactions in excimer systems.

Main Methods:

  • Developed MS-EDA using density functional theory.
  • Optimized monomer localized excited and charge-transfer states.
  • Employed nonorthogonal state interaction (NOSI) calculations within multistate density functional theory.

Main Results:

  • Excimer energy is decomposed into exciton excitation, superexchange stabilization, and orbital-and-configuration delocalization energies.
  • Charge-transfer state resonance is crucial for stabilizing excimers, even without net charge transfer.
  • Excited-state energy splitting depends on monomer excited states and wave function phase-matching.

Conclusions:

  • The MS-EDA method offers insights into exciton coupling, superexchange, and delocalization in excited states.
  • The method was successfully applied to acetone and pentacene excimer systems.
  • Relative monomer excited state energies and wave function phase-matching significantly influence excimer energy splitting.