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  Excited-state dynamics of [Ru(S–Sbpy)(bpy)2]2+to form long-lived localized triplet states

Heindl, M., Jiang, H., Hua, S.-A., Oelschlegel, M., Meyer, F., Schwarzer, D., et al. (2021). Excited-state dynamics of [Ru(S–Sbpy)(bpy)2]2+to form long-lived localized triplet states. Inorganic Chemistry, 60(3), 1672-1682. doi:10.1021/acs.inorgchem.0c03163.

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 Creators:
Heindl, M., Author
Jiang, H.1, Author           
Hua, S.-A., Author
Oelschlegel, M., Author
Meyer, F., Author
Schwarzer, D.1, Author           
González, L., Author
Affiliations:
1Department of Dynamics at Surfaces, MPI for Biophysical Chemistry, Max Planck Society, ou_578600              

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Free keywords: Computational chemistry, Quantum mechanics, Absorption, Energy, Ligands
 Abstract: The novel photosensitizer [Ru( S−S bpy)(bpy) 2 ] 2+
harbors two distinct sets of excited states in the UV/Vis region
of the absorption spectrum located on either bpy or S−S
bpy ligands.
Here, we address the question of whether following excitation into
these two types of states could lead to the formation of different
long-lived excited states from where energy transfer to a reactive
species could occur. Femtosecond transient absorption spectros-
copy identifies the formation of the final state within 80 fs for both
excitation wavelengths. The recorded spectra hint at very similar
dynamics following excitation toward either the parent or sulfur-
decorated bpy ligands, indicating ultrafast interconversion into a
unique excited-state species regardless of the initial state. Non-adiabatic surface hopping dynamics simulations show that ultrafast
spin−orbit-mediated mixing of the states within less than 50 fs strongly increases the localization of the excited electron at the S−S
bpy
ligand. Extensive structural relaxation within this sulfurated ligand is possible, via S−S bond cleavage that results in triplet state
energies that are lower than those in the analogue [Ru(bpy)3 ]2+ . This structural relaxation upon localization of the charge on S−S
bpy
is found to be the reason for the formation of a single long-lived species independent of the excitation wavelength.

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Language(s): eng - English
 Dates: 2020-10-262021-01-122021-02-01
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.inorgchem.0c03163
 Degree: -

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Project name : L.G., D.S., and F.M. are grateful to the Deutsche Forschungsgemeinschaft (DFG) for financial support of this work (projects Go1059/8-1, SCHW 661/4-1, and Me1313/ 15-1 within the SPP 2102 “Light-Controlled Reactivity of Metal Complexes”).
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Title: Inorganic Chemistry
Source Genre: Journal
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Pages: - Volume / Issue: 60 (3) Sequence Number: - Start / End Page: 1672 - 1682 Identifier: ISSN: 0020-1669
ISSN: 1520-510X