Analytic gradients and derivative couplings for configuration interaction with all single excitations and one double excitation—En route to nonadiabatic dynamics

Abstract

We present analytic gradients and derivative couplings for the simplest possible multireference configuration interaction method, CIS-1D, an electronic structure Ansatz that includes all single excitations and one lone double excitation on top of a Hartree–Fock reference state. We show that the resulting equations are numerically stable and require the evaluation of a similar number of integrals as compared to standard CIS theory; one can easily differentiate the required frontier orbitals (h and l) with minimal cost. The resulting algorithm has been implemented within the Q-Chem electronic structure package and should be immediately useful for understanding photochemistry with S0–S1 crossings.

Document Details

Document Type
Pub Defense Publication
Publication Date
Nov 11, 2020
Source ID
10.1063/5.0018441

Entities

People

  • Hung-Hsuan Teh
  • Joseph E Subotnik

Organizations

  • Air Force Office of Scientific Research
  • University of Pennsylvania

Tags

Fields of Study

  • Physics

Readers

  • Operations Research
  • Quantum Chemistry
  • Quantum spin resonance or Electron Paramagnetic Resonance spectroscopy.

Technology Areas

  • Microelectronics
  • Microelectronics - Graphene
  • Space