Capturing a photoexcited molecular structure through time-domain x-ray absorption fine structure

L. X. Chen*, W. J H Jäger, G. Jennings, D. J. Gosztota, A. Munkholm, J. P. Hessler

*Corresponding author for this work

Research output: Contribution to journalArticle

243 Scopus citations

Abstract

The determination of the structure of transient molecules, such as photoexcited states, in disordered media (such as in solution) usually requires methods with high temporal resolution. The transient molecular structure of a reaction intermediate produced by photoexcitation of NiTPP-L2 (NiTPP, nickeltetraphenylporphyrin; L, piperidine) in solution was determined by x-ray absorption fine structure (XAFS) data obtained on a 14-nanosecond time scale from a third-generation synchrotron source. The XAFS measurements confirm that photoexcitation leads to the rapid removal of both axial ligands to produce a transient square-planar intermediate, NiTPP, with a lifetime of 28 nanoseconds. The transient structure of the photodissociated intermediate is nearly identical to that of the ground state NiTPP, suggesting that the intermediate adopts the same structure as the ground state in a noncoordinating solvent before it recombines with two ligands to form the more stable octahedrally coordinated NiTPP-L2.

Original languageEnglish (US)
Pages (from-to)262-264
Number of pages3
JournalScience
Volume292
Issue number5515
DOIs
StatePublished - Apr 13 2001

ASJC Scopus subject areas

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    Chen, L. X., Jäger, W. J. H., Jennings, G., Gosztota, D. J., Munkholm, A., & Hessler, J. P. (2001). Capturing a photoexcited molecular structure through time-domain x-ray absorption fine structure. Science, 292(5515), 262-264. https://doi.org/10.1126/science.1057063