The intermediate state approach for doubly excited dark states in EOM-coupled-cluster theory

Abstract

Solution of dark, doubly excited states using equation-of-motion coupled-cluster (EOM-CC) usually equires at least triple excitations or even quadruples beyond the standard singles and doubles (EOM-CCSD) for an appropriate treatment. A new route to obtain these doubly excited states using EOM-CCSD is demonstrated. Traditionally, EOM-CC is performed on a closed shell reference state that has a well-described single reference CC wavefunction. In this Communication, we attempt to use low spin open-shell states such as the MS = 0 triplet and open-shell singlet as a reference state. Using this intermediate excited state as a reference state provides us with the benefit of obtaining a doubly excited state, as a single excitation at the cost of EOM-CCSD.

Document Details

Document Type
Pub Defense Publication
Publication Date
May 23, 2022
Source ID
10.1063/5.0091715

Entities

People

  • Ajith Perera
  • Moneesha Ravi
  • Rodney J. Bartlett
  • Young Choon Park

Organizations

  • Air Force Office of Scientific Research
  • University of Florida

Tags

Fields of Study

  • Physics

Readers

  • Molecular Photonics/Laser Physics
  • Quantum Chemistry