Photodissociation structural dynamics of trirutheniumdodecacarbonyl investigated by X-ray transient absorption spectroscopy

Michael R. Harpham; Andrew B. Stickrath; Xiaoyi Zhang; Jier Huang; Michael William Mara; Lin X Chen; Di Jia Liu

doi:10.1021/jp312663q

Photodissociation structural dynamics of trirutheniumdodecacarbonyl investigated by X-ray transient absorption spectroscopy

Michael R. Harpham, Andrew B. Stickrath, Xiaoyi Zhang, Jier Huang, Michael William Mara, Lin X Chen^*, Di Jia Liu

^*Corresponding author for this work

Chemistry

Research output: Contribution to journal › Article › peer-review

13 Scopus citations

Abstract

The molecular and electronic structures of the transient intermediates generated from the photolysis of trirutheniumdodecacarbonyl, Ru ₃(CO)₁₂, by ultrafast UV (351 nm) laser excitation were investigated using X-ray transient absorption (XTA) spectroscopy. The electronic configuration change and nuclear rearrangement after the dissociation of carbonyls were observed at ruthenium K-edge X-ray absorption near edge structure and X-ray absorption fine structure spectra. Analysis of XTA data, acquired after 100, 200, and 400 ps and 300 ns time delay following the photoexcitation, identified the presence of three intermediate species with Ru ₃(CO)₁₀ being the most dominating one. The results set an example of applying XTA in capturing both transient electronic and nuclear configurations in metal clusters simulating catalysts in chemical reactions.

Original language	English (US)
Pages (from-to)	9807-9813
Number of pages	7
Journal	Journal of Physical Chemistry A
Volume	117
Issue number	39
DOIs	https://doi.org/10.1021/jp312663q
State	Published - Oct 3 2013

ASJC Scopus subject areas

Physical and Theoretical Chemistry

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title = "Photodissociation structural dynamics of trirutheniumdodecacarbonyl investigated by X-ray transient absorption spectroscopy",

abstract = "The molecular and electronic structures of the transient intermediates generated from the photolysis of trirutheniumdodecacarbonyl, Ru 3(CO)12, by ultrafast UV (351 nm) laser excitation were investigated using X-ray transient absorption (XTA) spectroscopy. The electronic configuration change and nuclear rearrangement after the dissociation of carbonyls were observed at ruthenium K-edge X-ray absorption near edge structure and X-ray absorption fine structure spectra. Analysis of XTA data, acquired after 100, 200, and 400 ps and 300 ns time delay following the photoexcitation, identified the presence of three intermediate species with Ru 3(CO)10 being the most dominating one. The results set an example of applying XTA in capturing both transient electronic and nuclear configurations in metal clusters simulating catalysts in chemical reactions.",

author = "Harpham, {Michael R.} and Stickrath, {Andrew B.} and Xiaoyi Zhang and Jier Huang and Mara, {Michael William} and Chen, {Lin X} and Liu, {Di Jia}",

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T1 - Photodissociation structural dynamics of trirutheniumdodecacarbonyl investigated by X-ray transient absorption spectroscopy

AU - Harpham, Michael R.

AU - Stickrath, Andrew B.

AU - Zhang, Xiaoyi

AU - Huang, Jier

AU - Mara, Michael William

AU - Chen, Lin X

AU - Liu, Di Jia

PY - 2013/10/3

Y1 - 2013/10/3

N2 - The molecular and electronic structures of the transient intermediates generated from the photolysis of trirutheniumdodecacarbonyl, Ru 3(CO)12, by ultrafast UV (351 nm) laser excitation were investigated using X-ray transient absorption (XTA) spectroscopy. The electronic configuration change and nuclear rearrangement after the dissociation of carbonyls were observed at ruthenium K-edge X-ray absorption near edge structure and X-ray absorption fine structure spectra. Analysis of XTA data, acquired after 100, 200, and 400 ps and 300 ns time delay following the photoexcitation, identified the presence of three intermediate species with Ru 3(CO)10 being the most dominating one. The results set an example of applying XTA in capturing both transient electronic and nuclear configurations in metal clusters simulating catalysts in chemical reactions.

AB - The molecular and electronic structures of the transient intermediates generated from the photolysis of trirutheniumdodecacarbonyl, Ru 3(CO)12, by ultrafast UV (351 nm) laser excitation were investigated using X-ray transient absorption (XTA) spectroscopy. The electronic configuration change and nuclear rearrangement after the dissociation of carbonyls were observed at ruthenium K-edge X-ray absorption near edge structure and X-ray absorption fine structure spectra. Analysis of XTA data, acquired after 100, 200, and 400 ps and 300 ns time delay following the photoexcitation, identified the presence of three intermediate species with Ru 3(CO)10 being the most dominating one. The results set an example of applying XTA in capturing both transient electronic and nuclear configurations in metal clusters simulating catalysts in chemical reactions.

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Photodissociation structural dynamics of trirutheniumdodecacarbonyl investigated by X-ray transient absorption spectroscopy

Abstract

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