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Ultrafast Photochemistry of the [Cr(NCS)6]3- Complex in Dimethyl Sulfoxide and Dimethylformamide upon Excitation into Ligand-Field Electronic State. / Khvorost, Taras A.; Beliaev, Leonid Yu.; Potalueva, Ekaterina; Laptenkova, Anastasia V.; Selyutin, Artem A.; Bogachev, Nikita A.; Skripkin, Mikhail Yu; Ryazantsev, Mikhail N.; Tkachenko, Nikolai; Mereshchenko, Andrey S.

в: Journal of Physical Chemistry B, Том 124, № 18, 07.05.2020, стр. 3724-3733.

Результаты исследований: Научные публикации в периодических изданияхстатьяРецензирование

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@article{504ce82a655240968caf87be5cff3c1e,
title = "Ultrafast Photochemistry of the [Cr(NCS)6]3- Complex in Dimethyl Sulfoxide and Dimethylformamide upon Excitation into Ligand-Field Electronic State",
abstract = "The ultrafast photochemistry of the [Cr(NCS)6]3- complex upon excitation to the 4T2 ligand-field (LF) state was studied in dimethyl sulfoxide (DMSO) and N,N-dimethylformamide (DMF) in a wide temporal range (100 fs to 9 ms) by a combination of femtosecond and nanosecond transient absorption spectroscopy techniques and supported by quantum-chemical DFT/TD-DFT calculations. The initially excited 4T2 state undergoes intersystem crossing to the vibrationally hot 2E state with time constants of 1.1 ± 0.2 and 1.8 ± 0.1 ps in DMSO and DMF, respectively. Vibrational relaxation occurs in the same time scale and takes 1-5 ps. A major part of the [Cr(NCS)6]3- complex in the 2E state undergoes intersystem crossing to the ground state with time constants of 65 ± 5 and 85 ± 5 ns in DMSO and DMF, respectively. A minor part of electronically excited [Cr(NCS)6]3- undergoes irreversible photochemical decomposition. In DMSO, the photolysis of the [Cr(NCS)6]3- complex results in single or double isothiocyanate ion release followed by the coordination of the solvent molecules with a time constant of 1 ± 0.2 ms.",
keywords = "TRANSIENT ABSORPTION-SPECTROSCOPY, EXCITED-STATE, DYNAMICS, RELAXATION, SPECTRA, CHROMIUM(3)",
author = "Khvorost, {Taras A.} and Beliaev, {Leonid Yu.} and Ekaterina Potalueva and Laptenkova, {Anastasia V.} and Selyutin, {Artem A.} and Bogachev, {Nikita A.} and Skripkin, {Mikhail Yu} and Ryazantsev, {Mikhail N.} and Nikolai Tkachenko and Mereshchenko, {Andrey S.}",
year = "2020",
month = may,
day = "7",
doi = "10.1021/acs.jpcb.0c00088",
language = "English",
volume = "124",
pages = "3724--3733",
journal = "Journal of Physical Chemistry B",
issn = "1520-6106",
publisher = "American Chemical Society",
number = "18",

}

RIS

TY - JOUR

T1 - Ultrafast Photochemistry of the [Cr(NCS)6]3- Complex in Dimethyl Sulfoxide and Dimethylformamide upon Excitation into Ligand-Field Electronic State

AU - Khvorost, Taras A.

AU - Beliaev, Leonid Yu.

AU - Potalueva, Ekaterina

AU - Laptenkova, Anastasia V.

AU - Selyutin, Artem A.

AU - Bogachev, Nikita A.

AU - Skripkin, Mikhail Yu

AU - Ryazantsev, Mikhail N.

AU - Tkachenko, Nikolai

AU - Mereshchenko, Andrey S.

PY - 2020/5/7

Y1 - 2020/5/7

N2 - The ultrafast photochemistry of the [Cr(NCS)6]3- complex upon excitation to the 4T2 ligand-field (LF) state was studied in dimethyl sulfoxide (DMSO) and N,N-dimethylformamide (DMF) in a wide temporal range (100 fs to 9 ms) by a combination of femtosecond and nanosecond transient absorption spectroscopy techniques and supported by quantum-chemical DFT/TD-DFT calculations. The initially excited 4T2 state undergoes intersystem crossing to the vibrationally hot 2E state with time constants of 1.1 ± 0.2 and 1.8 ± 0.1 ps in DMSO and DMF, respectively. Vibrational relaxation occurs in the same time scale and takes 1-5 ps. A major part of the [Cr(NCS)6]3- complex in the 2E state undergoes intersystem crossing to the ground state with time constants of 65 ± 5 and 85 ± 5 ns in DMSO and DMF, respectively. A minor part of electronically excited [Cr(NCS)6]3- undergoes irreversible photochemical decomposition. In DMSO, the photolysis of the [Cr(NCS)6]3- complex results in single or double isothiocyanate ion release followed by the coordination of the solvent molecules with a time constant of 1 ± 0.2 ms.

AB - The ultrafast photochemistry of the [Cr(NCS)6]3- complex upon excitation to the 4T2 ligand-field (LF) state was studied in dimethyl sulfoxide (DMSO) and N,N-dimethylformamide (DMF) in a wide temporal range (100 fs to 9 ms) by a combination of femtosecond and nanosecond transient absorption spectroscopy techniques and supported by quantum-chemical DFT/TD-DFT calculations. The initially excited 4T2 state undergoes intersystem crossing to the vibrationally hot 2E state with time constants of 1.1 ± 0.2 and 1.8 ± 0.1 ps in DMSO and DMF, respectively. Vibrational relaxation occurs in the same time scale and takes 1-5 ps. A major part of the [Cr(NCS)6]3- complex in the 2E state undergoes intersystem crossing to the ground state with time constants of 65 ± 5 and 85 ± 5 ns in DMSO and DMF, respectively. A minor part of electronically excited [Cr(NCS)6]3- undergoes irreversible photochemical decomposition. In DMSO, the photolysis of the [Cr(NCS)6]3- complex results in single or double isothiocyanate ion release followed by the coordination of the solvent molecules with a time constant of 1 ± 0.2 ms.

KW - TRANSIENT ABSORPTION-SPECTROSCOPY

KW - EXCITED-STATE

KW - DYNAMICS

KW - RELAXATION

KW - SPECTRA

KW - CHROMIUM(3)

UR - http://www.scopus.com/inward/record.url?scp=85084379376&partnerID=8YFLogxK

U2 - 10.1021/acs.jpcb.0c00088

DO - 10.1021/acs.jpcb.0c00088

M3 - Article

C2 - 32283018

AN - SCOPUS:85084379376

VL - 124

SP - 3724

EP - 3733

JO - Journal of Physical Chemistry B

JF - Journal of Physical Chemistry B

SN - 1520-6106

IS - 18

ER -

ID: 60312120