Journal
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
Volume 13, Issue 8, Pages 3493-3504Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jctc.7b00171
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Funding
- AMOS program within the Chemical Sciences, Geosciences and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, US Department of Energy
- NSF MRI Program [ACI-1429830]
- Knut and Alice Wallenberg Foundation [KAW 2014.0391]
- Direct For Computer & Info Scie & Enginr
- Office of Advanced Cyberinfrastructure (OAC) [1429830] Funding Source: National Science Foundation
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The Frenkel exciton model is a useful tool for theoretical studies of multichromophore systems. We recently showed that the exciton model could be used to coarse-grain electronic structure in multichromophoric systems, focusing on singly excited exciton states [Acc. Chem. Res. 2014, 47, 2857-2866]. However, our previous implementation excluded charge-transfer excited states, which can play an important role in light-harvesting systems and near-infrared optoelectronic materials. Recent studies have also emphasized the significance of charge-transfer in singlet fission, which mediates the coupling between the locally excited states and the multiexcitonic states. In this work, we report on an ab initio exciton model that incorporates charge-transfer excited states and demonstrate that the model provides correct charge-transfer excitation energies and asymptotic behavior. Comparison with TDDFT and EOM-CC2 calculations shows that our exciton model is robust with respect to system size, screening parameter, and different density functionals. Inclusion of charge-transfer excited states makes the exciton model more useful for studies of singly excited states and provides a starting point for future construction of a model that also includes double-exciton states.
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