On the inclusion of one double within CIS and TDDFT

Abstract

We present an improved approach for generating a set of optimized frontier orbitals (HOMO and LUMO) that minimizes the energy of one double configuration. We further benchmark the effect of including such a double within a rigorous configuration interaction singles or a parameterized semi-empirical time-dependent density functional theory Hamiltonian for a set of test cases. Although we cannot quite achieve quantitative accuracy, the algorithm is quite robust and routinely delivers an enormous qualitative improvement to standard single-reference electronic structure calculations.

Document Details

Document Type
Pub Defense Publication
Publication Date
Oct 20, 2021
Source ID
10.1063/5.0064269

Entities

People

  • Hung-Hsuan Teh
  • Joseph E Subotnik
  • Vishikh Athavale

Organizations

  • Air Force Office of Scientific Research
  • University of Pennsylvania

Tags

Fields of Study

  • Physics

Readers

  • Computational Modeling and Simulation
  • Quantum Chemistry

Technology Areas

  • Microelectronics
  • Microelectronics - Microelectromechanical Systems
  • Space