Initial metal-metal bond breakage detected by fs X-ray scattering in the photolysis of Ru3(CO)12 in cyclohexane at 400 nm

Research output: Contribution to journalJournal article – Annual report year: 2019Researchpeer-review

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Initial metal-metal bond breakage detected by fs X-ray scattering in the photolysis of Ru3(CO)12 in cyclohexane at 400 nm. / Kong, Q. Y.; Laursen, M. G.; Haldrup, K.; Kjær, K. S.; Khakhulin, D.; Biasin, E.; van Driel, T. B.; Wulff, M.; Kabanova, V.; Vuilleumier, R.; Bratos, S.; Nielsen, M. M.; Gaffney, K. J.; Weng, T. C.; Koch, M. H. J.

In: Photochemical & Photobiological Sciences, Vol. 18, No. 2, 2019, p. 319-327.

Research output: Contribution to journalJournal article – Annual report year: 2019Researchpeer-review

Harvard

Kong, QY, Laursen, MG, Haldrup, K, Kjær, KS, Khakhulin, D, Biasin, E, van Driel, TB, Wulff, M, Kabanova, V, Vuilleumier, R, Bratos, S, Nielsen, MM, Gaffney, KJ, Weng, TC & Koch, MHJ 2019, 'Initial metal-metal bond breakage detected by fs X-ray scattering in the photolysis of Ru3(CO)12 in cyclohexane at 400 nm', Photochemical & Photobiological Sciences, vol. 18, no. 2, pp. 319-327. https://doi.org/10.1039/c8pp00420j

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Author

Kong, Q. Y. ; Laursen, M. G. ; Haldrup, K. ; Kjær, K. S. ; Khakhulin, D. ; Biasin, E. ; van Driel, T. B. ; Wulff, M. ; Kabanova, V. ; Vuilleumier, R. ; Bratos, S. ; Nielsen, M. M. ; Gaffney, K. J. ; Weng, T. C. ; Koch, M. H. J. / Initial metal-metal bond breakage detected by fs X-ray scattering in the photolysis of Ru3(CO)12 in cyclohexane at 400 nm. In: Photochemical & Photobiological Sciences. 2019 ; Vol. 18, No. 2. pp. 319-327.

Bibtex

@article{590b1c385a504056ae47e7b00736571f,
title = "Initial metal-metal bond breakage detected by fs X-ray scattering in the photolysis of Ru3(CO)12 in cyclohexane at 400 nm",
abstract = "Using femtosecond resolution X-ray solution scattering at a free electron laser we were able to directly observe metal-metal bond cleavage upon photolysis at 400 nm of Ru3(CO)12, a prototype for the photochemistry of transition metal carbonyls. This leads to the known single intermediate Ru3(CO)11(μ-CO)*, with a bridging ligand (μCO) and where the asterisk indicates an open Ru3-ring. This loses a CO ligand on a picosecond time scale yielding a newly observed triple bridge intermediate, Ru3(CO)8(μ-CO)3*. This loses another CO ligand to form the previously observed Ru3(CO)10, which returns to Ru3(CO)12 via the known single-bridge Ru3(CO)10(μ-CO). These results indicate that contrary to long standing hypotheses, metal-metal bond breakage is the only chemical reaction immediately following the photolysis of Ru3(CO)12 at 400 nm. Combined with previous picosecond resolution X-ray scattering data and time resolved infrared spectroscopy these results yield a new mechanism for the photolysis of Ru3(CO)12.",
author = "Kong, {Q. Y.} and Laursen, {M. G.} and K. Haldrup and Kj{\ae}r, {K. S.} and D. Khakhulin and E. Biasin and {van Driel}, {T. B.} and M. Wulff and V. Kabanova and R. Vuilleumier and S. Bratos and Nielsen, {M. M.} and Gaffney, {K. J.} and Weng, {T. C.} and Koch, {M. H. J.}",
year = "2019",
doi = "10.1039/c8pp00420j",
language = "English",
volume = "18",
pages = "319--327",
journal = "Photochemical & Photobiological Sciences",
issn = "1474-905X",
publisher = "Royal Society of Chemistry",
number = "2",

}

RIS

TY - JOUR

T1 - Initial metal-metal bond breakage detected by fs X-ray scattering in the photolysis of Ru3(CO)12 in cyclohexane at 400 nm

AU - Kong, Q. Y.

AU - Laursen, M. G.

AU - Haldrup, K.

AU - Kjær, K. S.

AU - Khakhulin, D.

AU - Biasin, E.

AU - van Driel, T. B.

AU - Wulff, M.

AU - Kabanova, V.

AU - Vuilleumier, R.

AU - Bratos, S.

AU - Nielsen, M. M.

AU - Gaffney, K. J.

AU - Weng, T. C.

AU - Koch, M. H. J.

PY - 2019

Y1 - 2019

N2 - Using femtosecond resolution X-ray solution scattering at a free electron laser we were able to directly observe metal-metal bond cleavage upon photolysis at 400 nm of Ru3(CO)12, a prototype for the photochemistry of transition metal carbonyls. This leads to the known single intermediate Ru3(CO)11(μ-CO)*, with a bridging ligand (μCO) and where the asterisk indicates an open Ru3-ring. This loses a CO ligand on a picosecond time scale yielding a newly observed triple bridge intermediate, Ru3(CO)8(μ-CO)3*. This loses another CO ligand to form the previously observed Ru3(CO)10, which returns to Ru3(CO)12 via the known single-bridge Ru3(CO)10(μ-CO). These results indicate that contrary to long standing hypotheses, metal-metal bond breakage is the only chemical reaction immediately following the photolysis of Ru3(CO)12 at 400 nm. Combined with previous picosecond resolution X-ray scattering data and time resolved infrared spectroscopy these results yield a new mechanism for the photolysis of Ru3(CO)12.

AB - Using femtosecond resolution X-ray solution scattering at a free electron laser we were able to directly observe metal-metal bond cleavage upon photolysis at 400 nm of Ru3(CO)12, a prototype for the photochemistry of transition metal carbonyls. This leads to the known single intermediate Ru3(CO)11(μ-CO)*, with a bridging ligand (μCO) and where the asterisk indicates an open Ru3-ring. This loses a CO ligand on a picosecond time scale yielding a newly observed triple bridge intermediate, Ru3(CO)8(μ-CO)3*. This loses another CO ligand to form the previously observed Ru3(CO)10, which returns to Ru3(CO)12 via the known single-bridge Ru3(CO)10(μ-CO). These results indicate that contrary to long standing hypotheses, metal-metal bond breakage is the only chemical reaction immediately following the photolysis of Ru3(CO)12 at 400 nm. Combined with previous picosecond resolution X-ray scattering data and time resolved infrared spectroscopy these results yield a new mechanism for the photolysis of Ru3(CO)12.

U2 - 10.1039/c8pp00420j

DO - 10.1039/c8pp00420j

M3 - Journal article

VL - 18

SP - 319

EP - 327

JO - Photochemical & Photobiological Sciences

JF - Photochemical & Photobiological Sciences

SN - 1474-905X

IS - 2

ER -