A Multiconfigurational Wave Function Implementation of the Frenkel Exciton Model for Molecular Aggregates

Andy Kaiser, Razan E. Daoud, Francesco Aquilante, Oliver Kühn, Luca De Vico, Sergey I. Bokarev

Research output: Contribution to journalArticlepeer-review

3 Scopus citations

Abstract

We present an implementation of the Frenkel exciton model into the OpenMolcas program package enabling calculations of collective electronic excited states of molecular aggregates based on a multiconfigurational wave function description of the individual monomers. The computational protocol avoids using diabatization schemes and, thus, supermolecule calculations. Additionally, the use of the Cholesky decomposition of the two-electron integrals entering pair interactions enhances the efficiency of the computational scheme. The application of the method is exemplified for two test systems, that is, a formaldehyde oxime and a bacteriochlorophyll-like dimer. For the sake of comparison with the dipole approximation, we restrict our considerations to situations where intermonomer exchange can be neglected. The protocol is expected to be beneficial for aggregates composed of molecules with extended πsystems, unpaired electrons such as radicals or transition metal centers, where it should outperform widely used methods based on time-dependent density functional theory.

Original languageEnglish
Pages (from-to)2918-2928
Number of pages11
JournalJournal of Chemical Theory and Computation
Volume19
Issue number10
DOIs
StatePublished - 23 May 2023

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