Quantifying local exciton, charge resonance, and multiexciton character in correlated wave functions of multichromophoric systems
- Kimika Fakultatea, Euskal Herriko Unibersitatea (UPV/EHU) and Donostia International Physics Center (DIPC), P.K. 1072, 20018 Donostia (Spain)
- Department of Chemistry, University of Southern California, Los Angeles, California 90089-0482 (United States)
A new method for quantifying the contributions of local excitation, charge resonance, and multiexciton configurations in correlated wave functions of multichromophoric systems is presented. The approach relies on fragment-localized orbitals and employs spin correlators. Its utility is illustrated by calculations on model clusters of hydrogen, ethylene, and tetracene molecules using adiabatic restricted-active-space configuration interaction wave functions. In addition to the wave function analysis, this approach provides a basis for a simple state-specific energy correction accounting for insufficient description of electron correlation. The decomposition scheme also allows one to compute energies of the diabatic states of the local excitonic, charge-resonance, and multi-excitonic character. The new method provides insight into electronic structure of multichromophoric systems and delivers valuable reference data for validating excitonic models.
- OSTI ID:
- 22493611
- Journal Information:
- Journal of Chemical Physics, Vol. 144, Issue 1; Other Information: (c) 2016 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
- Country of Publication:
- United States
- Language:
- English
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