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dc.contributor.authorChołuj, Marta
dc.contributor.authorAlam, MD Mehboob
dc.contributor.authorBeerepoot, Maarten
dc.contributor.authorSitkiewicz, Sebastian P.
dc.contributor.authorMatito, Eduard
dc.contributor.authorRuud, Kenneth
dc.contributor.authorZaleśny, Robert
dc.date.accessioned2022-02-24T14:14:19Z
dc.date.available2022-02-24T14:14:19Z
dc.date.issued2022-01-26
dc.description.abstractWe present a benchmark study of density functional approximation (DFA) performances in predicting the two-photon-absorption strengths in π-conjugated molecules containing electron-donating/-accepting moieties. A set of 48 organic molecules is chosen for this purpose, for which the two-photon-absorption (2PA) parameters are evaluated using different DFAs, including BLYP, PBE, B3LYP, PBE0, CAM-B3LYP, LC-BLYP, and optimally tuned LC-BLYP. Minnesota functionals and ωB97X-D are also used, applying the two-state approximation, for a subset of molecules. The efficient resolution-of-identity implementation of the coupled-cluster CC2 model (RI-CC2) is used as a reference for the assessment of the DFAs. Two-state models within the framework of both DFAs and RI-CC2 are used to gain a deeper insight into the performance of different DFAs. Our results give a clear picture of the performance of the density functionals in describing the two-photon activity in dipolar π-conjugated systems. The results show that global hybrids are best suited to reproduce the absolute values of 2PA strengths of donor–acceptor molecules. The range-separated functionals CAM-B3LYP and optimally tuned LC-BLYP, however, show the highest linear correlations with the reference RI-CC2 results. Hence, we recommend the latter DFAs for structure–property studies across large series of dipolar compounds.en_US
dc.identifier.citationChołuj, Alam, Beerepoot, Sitkiewicz, Matito, Ruud, Zaleśny. Choosing Bad versus Worse: Predictions of Two-Photon-Absorption Strengths Based on Popular Density Functional Approximations. Journal of Chemical Theory and Computation. 2021;18:1046-1060en_US
dc.identifier.cristinIDFRIDAID 2002989
dc.identifier.doi10.1021/acs.jctc.1c01056
dc.identifier.issn1549-9618
dc.identifier.issn1549-9626
dc.identifier.urihttps://hdl.handle.net/10037/24145
dc.language.isoengen_US
dc.publisherAmerican Chemical Societyen_US
dc.relation.journalJournal of Chemical Theory and Computation
dc.relation.projectIDNorges forskningsråd: 262695en_US
dc.relation.urihttps://doi.org/10.1021/acs.jctc.1c01056
dc.rights.accessRightsopenAccessen_US
dc.rights.holderCopyright 2021 The Author(s)en_US
dc.titleChoosing Bad versus Worse: Predictions of Two-Photon-Absorption Strengths Based on Popular Density Functional Approximationsen_US
dc.type.versionpublishedVersionen_US
dc.typeJournal articleen_US
dc.typeTidsskriftartikkelen_US
dc.typePeer revieweden_US


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