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Nonadiabatic excited-state dynamics of ReCl(CO)3(bpy) in two different solvents
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SYSNO ASEP 0563307 Document Type J - Journal Article R&D Document Type Journal Article Subsidiary J Článek ve WOS Title Nonadiabatic excited-state dynamics of ReCl(CO)3(bpy) in two different solvents Author(s) Šrut, A. (CZ)
Mai, S. (AT)
Sazanovich, I. (GB)
Heyda, Jan (UFCH-W) ORCID, RID
Vlček, Antonín (UFCH-W) RID, ORCID
González, L. (AT)
Záliš, Stanislav (UFCH-W) RID, ORCIDSource Title Physical Chemistry Chemical Physics. - : Royal Society of Chemistry - ISSN 1463-9076
Roč. 24, č. 42 (2022), s. 25864-25877Number of pages 14 s. Language eng - English Country GB - United Kingdom Keywords RESOLVED INFRARED-SPECTROSCOPY ; TRANSITION-METAL-COMPLEXES ; CARBONYL-DIIMINE-COMPLEXES Subject RIV CF - Physical ; Theoretical Chemistry OECD category Physical chemistry R&D Projects GA21-05180S GA ČR - Czech Science Foundation (CSF) EF18_054/0014591 GA MŠMT - Ministry of Education, Youth and Sports (MEYS) Research Infrastructure e-INFRA CZ - 90140 - CESNET, zájmové sdružení právnických osob Method of publishing Open access Institutional support UFCH-W - RVO:61388955 UT WOS 000871600700001 EID SCOPUS 85141862345 DOI 10.1039/d2cp02981b Annotation We present a study of excited-states relaxation of the complex ReCl(CO)3(bpy) (bpy = 2,2-bipyridine) using a nonadiabatic TD-DFT dynamics on spin-mixed potential energy surfaces in explicit acetonitrile (ACN) and dimethylsulfoxide (DMSO) solutions up to 800 fs. ReCl(CO)3(bpy) belongs to a group of important photosensitizers which show ultrafast biexponential subpicosecond fluorescence decay kinetics. The choice of solvents was motivated by the different excited-state relaxation dynamics observed in subpicosecond time-resolved IR (TRIR) experiments. Simulations of intersystem crossing (ISC) showed the development of spin-mixed states in both solvents. Transformation of time-dependent populations of spin-mixed states enabled to monitor the temporal evolution of individual singlet and triplet states, fitting of bi-exponential decay kinetics, and simulating the time-resolved fluorescence spectra that show only minor differences between the two solvents. Analysis of structural relaxation and solvent reorganization employing time-resolved proximal distribution functions pointed to the factors influencing the fluorescence decay time constants. Nonadiabatic dynamics simulations of time-evolution of electronic, molecular, and solvent structures emerge as a powerful technique to interpret time-resolved spectroscopic data and ultrafast photochemical reactivity.
Workplace J. Heyrovsky Institute of Physical Chemistry Contact Michaela Knapová, michaela.knapova@jh-inst.cas.cz, Tel.: 266 053 196 Year of Publishing 2023 Electronic address https://hdl.handle.net/11104/0335304
Number of the records: 1