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Inter-Excited-State Phosphorescence in the Four-Component Relativistic Kohn-Sham Approximation: A Case Study on Lumiflavin
Linköping University, Sweden.ORCID iD: 0000-0002-1191-4954
2015 (English)In: Journal of Physical Chemistry A, ISSN 1089-5639, E-ISSN 1520-5215, Vol. 119, no 49, p. 11911-11921Article in journal (Refereed) Published
Abstract [en]

Electronic transitions from one excited state to another excited state of different spin symmetry play important roles in many biochemical reactions. Although recent years have seen much progress in the elucidation of nonradiative (intersystem crossing) relaxation mechanisms for such transitions, there is presently a scarcity of data available to assess whether also radiative (phosphorescence) mechanisms are relevant for these processes. Here, we demonstrate that the well-established ability of quantum chemical methods to describe intersystem crossing events between excited states can be supplemented by the ability to also describe inter-excited-state phosphorescence. Specifically, by performing four-component relativistic time-dependent density functional theory calculations, we obtain rate constants for the radiative transitions from the absorbing 1(πHπL∗) singlet state of lumiflavin to the 3(πHπL∗), 3(nN2πL∗), and 3(πH-1πL∗) triplet states, and subsequently, we compare these results with rate constants calculated for the corresponding nonradiative transitions. Thereby, it is found that the radiative rate constants for these particular transitions are typically 2 to 5 orders of magnitude smaller than the nonradiative ones.

Place, publisher, year, edition, pages
American Chemical Society (ACS), 2015. Vol. 119, no 49, p. 11911-11921
Keywords [en]
Density functional theory, Light emission, Phosphorescence, Quantum chemistry, Quantum theory, Rate constants, Biochemical reactions, Electronic transition, Inter-system crossings, Non-radiative transitions, Quantum-chemical methods, Radiative rate constants, Radiative transitions, Time dependent density functional theory calculations, Excited states, lumiflavine, riboflavin derivative, chemical structure, chemistry, Flavins, Molecular Structure
National Category
Theoretical Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-198708DOI: 10.1021/acs.jpca.5b08908ISI: 000366339400016PubMedID: 26565664Scopus ID: 2-s2.0-84949023935OAI: oai:DiVA.org:kth-198708DiVA, id: diva2:1059136
Funder
Swedish Research Council, 621-2011-4353 621-2014-4646
Note

QC 20170118

Available from: 2016-12-22 Created: 2016-12-21 Last updated: 2017-11-29Bibliographically approved

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