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Nonempirical Simulations of Inhomogeneous Broadening of Electronic Transitions in Solution: Predicting Band Shapes in One- and Two-Photon Absorption Spectra of Chalcones
KTH, School of Biotechnology (BIO), Theoretical Chemistry and Biology.ORCID iD: 0000-0003-0185-5724
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2017 (English)In: Molecules, ISSN 1420-3049, E-ISSN 1420-3049, Vol. 22, no 10, article id 1643Article in journal (Refereed) Published
Abstract [en]

We have examined several approaches relying on the Polarizable Embedding (PE) scheme to predict optical band shapes for two chalcone molecules in methanol solution. The PE-TDDFT and PERI-CC2 methods were combined with molecular dynamics simulations, where the solute geometry was kept either as rigid, flexible or partly-flexible (restrained) body. The first approach, termed RBMD-PE-TDDFT, was employed to estimate the inhomogeneous broadening for subsequent convolution with the vibrationally-resolved spectra of the molecule in solution determined quantum-mechanically (QM). As demonstrated, the RBMD-PE-TDDFT/QM-PCM approach delivers accurate band widths, also reproducing their correct asymmetric shapes. Further refinement can be obtained by the estimation of the inhomogeneous broadening using the RBMD-PERI-CC2 method. On the other hand, the remaining two approaches (FBMD-PE-TDDFT and ResBMD-PE-TDDFT), which lack quantum-mechanical treatment of molecular vibrations, lead to underestimated band widths. In this study, we also proposed a simple strategy regarding the rapid selection of the exchange-correlation functional for the simulations of vibrationally-resolved one-and two-photon absorption spectra based on two easy-to-compute metrics.

Place, publisher, year, edition, pages
2017. Vol. 22, no 10, article id 1643
Keywords [en]
density functional theory, two-photon absorption, vibrationally-resolved spectra, hybrid QM/MM solvation models
National Category
Organic Chemistry
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URN: urn:nbn:se:kth:diva-220293DOI: 10.3390/molecules22101643ISI: 000414670600070OAI: oai:DiVA.org:kth-220293DiVA, id: diva2:1169078
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QC 20171222

Available from: 2017-12-22 Created: 2017-12-22 Last updated: 2017-12-22Bibliographically approved

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Natarajan Arul, MuruganÅgren, Hans

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