Compact Real-Space Representation of Excited States Using Frequency-Dependent Explicitly Correlated Electron-Hole Interaction Kernel

Peter F. McLaughlin, Arindam Chakraborty

Research output: Contribution to journalArticle

Abstract

We present the frequency-dependent geminal-screened electron-hole interaction kernel (FD-GSIK) method for describing electron-hole correlation in electronically excited many-electron systems. The FD-GSIK is a parameter-free, first-principles method derived from excited-state wave function that was both frequency-dependent and r12-explicitly correlated. The FD-GSIK avoids using unoccupied orbitals for kernel construction by performing an infinite-order summation of particle-hole excitation and representing it as a compact real-space operator. It bypasses the computationally demanding steps of evaluation, storage, and transformation of atomic-orbital integrals by directly evaluating molecular orbital integrals in real space using the stratified Monte Carlo method. We demonstrate and discuss the advantages of this method by presenting excitation and electron-hole binding energies of large nanoparticles including Pb140S140, Pb140Se140, Cd144Se144, and Cd72S72.

Original languageEnglish (US)
Pages (from-to)5762-5770
Number of pages9
JournalJournal of Chemical Theory and Computation
Volume16
Issue number9
DOIs
StatePublished - Sep 8 2020

ASJC Scopus subject areas

  • Computer Science Applications
  • Physical and Theoretical Chemistry

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