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  4. A Multiconfigurational Wave Function Implementation of the Frenkel Exciton Model for Molecular Aggregates
 
research article

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

Kaiser, Andy
•
Daoud, Razan E.
•
Aquilante, Francesco  
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April 28, 2023
Journal of Chemical Theory and Computation

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 twoelectron 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 pi systems, unpaired electrons such as radicals or transition metal centers, where it should outperform widely used methods based on time-dependent density functional theory.

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Type
research article
DOI
10.1021/acs.jctc.3c00185
Web of Science ID

WOS:000984957300001

Author(s)
Kaiser, Andy
Daoud, Razan E.
Aquilante, Francesco  
Kuhn, Oliver
De Vico, Luca
Bokarev, Sergey I.
Date Issued

2023-04-28

Publisher

AMER CHEMICAL SOC

Published in
Journal of Chemical Theory and Computation
Subjects

Chemistry, Physical

•

Physics, Atomic, Molecular & Chemical

•

Chemistry

•

Physics

•

excitation-energy transfer

•

electronic-structure calculations

•

perturbation-theory

•

scale interpretation

•

coupled-cluster

•

basis-sets

•

resolution

•

systems

•

atoms

•

lh2

Editorial or Peer reviewed

REVIEWED

Written at

EPFL

EPFL units
THEOS  
Available on Infoscience
June 5, 2023
Use this identifier to reference this record
https://infoscience.epfl.ch/handle/20.500.14299/198051
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