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An MS-CASPT2 Calculation of the Excited Electronic States of an Axial Difluoroborondipyrromethene (BODIPY) Dimer
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SYSNO ASEP 0493068 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title An MS-CASPT2 Calculation of the Excited Electronic States of an Axial Difluoroborondipyrromethene (BODIPY) Dimer Author(s) Wen, Jin (UOCHB-X) RID, ORCID
Han, B. (US)
Havlas, Zdeněk (UOCHB-X) RID, ORCID
Michl, Josef (UOCHB-X) RID, ORCIDSource Title Journal of Chemical Theory and Computation . - : American Chemical Society - ISSN 1549-9618
Roč. 14, č. 8 (2018), s. 4291-4297Number of pages 7 s. Language eng - English Country US - United States Keywords second-order perturbation theory ; Gaussian basis sets ; photodynamic therapy Subject RIV CF - Physical ; Theoretical Chemistry OECD category Physical chemistry R&D Projects GA15-19143S GA ČR - Czech Science Foundation (CSF) Institutional support UOCHB-X - RVO:61388963 UT WOS 000442186100032 EID SCOPUS 85048372945 DOI 10.1021/acs.jctc.8b00136 Annotation The previously reported (Duman et al., J. Org. Chem. 2012, 77, 4516) calculated state energies of monomeric difluoroborondipyrromethene (BODIPY) and its axial dimer would suggest that these dyes are promising candidates for singlet fission, and the dimer was computed to have an unusual low-lying doubly excited state. We find that these results were affected by the use of an imbalanced active space in multireference calculations and are not correct. Multistate complete-active-space second-order perturbation theory (MS-CASPT2/cc-pVDZ) calculations using an [8,8] (8 electrons in 8 orbitals) active space for the monomer and a [16,16] active space for the dimer reproduce quite well the observed excitation energies of the S-1 states of both, and yield T-1 excitation energies well in excess of half of the S-1 excitation energies. We conclude that neither BODIPY monomer nor its axial dimer would permit exothermic singlet fission and are not worthy of investigation as potentially useful candidates, and that the unusual low-energy doubly excited states of the dimer were artifacts. Workplace Institute of Organic Chemistry and Biochemistry Contact asep@uochb.cas.cz ; Kateřina Šperková, Tel.: 232 002 584 ; Jana Procházková, Tel.: 220 183 418 Year of Publishing 2019
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