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Kim KH, Kim J, Oang KY, et al. Identifying the major intermediate species by combining time-resolved X-ray solution scattering and X-ray absorption spectroscopy. Phys Chem Chem Phys. 2015;17(36):23298-302doi: 10.1039/c5cp03686k.
Kim, K. H., Kim, J., Oang, K. Y., Lee, J. H., Grolimund, D., Milne, C. J., Penfold, T. J., Johnson, S. L., Galler, A., Kim, T. W., Kim, J. G., Suh, D., Moon, J., Kim, J., Hong, K., Guérin, L., Kim, T. K., Wulff, M., Bressler, C., & Ihee, H. (2015). Identifying the major intermediate species by combining time-resolved X-ray solution scattering and X-ray absorption spectroscopy. Physical chemistry chemical physics : PCCP, 17(36), 23298-302. https://doi.org/10.1039/c5cp03686k
Kim, Kyung Hwan, et al. "Identifying the major intermediate species by combining time-resolved X-ray solution scattering and X-ray absorption spectroscopy." Physical chemistry chemical physics : PCCP vol. 17,36 (2015): 23298-302. doi: https://doi.org/10.1039/c5cp03686k
Kim KH, Kim J, Oang KY, Lee JH, Grolimund D, Milne CJ, Penfold TJ, Johnson SL, Galler A, Kim TW, Kim JG, Suh D, Moon J, Kim J, Hong K, Guérin L, Kim TK, Wulff M, Bressler C, Ihee H. Identifying the major intermediate species by combining time-resolved X-ray solution scattering and X-ray absorption spectroscopy. Phys Chem Chem Phys. 2015 Sep 28;17(36):23298-302. doi: 10.1039/c5cp03686k. PMID: 26300122.
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Phys Chem Chem Phys. 2015 Sep 28;17(36):23298-302. doi: 10.1039/c5cp03686k.

Identifying the major intermediate species by combining time-resolved X-ray solution scattering and X-ray absorption spectroscopy.

Physical chemistry chemical physics : PCCP

Kyung Hwan Kim, Jeongho Kim, Key Young Oang, Jae Hyuk Lee, Daniel Grolimund, Christopher J Milne, Thomas J Penfold, Steven L Johnson, Andreas Galler, Tae Wu Kim, Jong Goo Kim, Deokbeom Suh, Jiwon Moon, Joonghan Kim, Kiryong Hong, Laurent Guérin, Tae Kyu Kim, Michael Wulff, Christian Bressler, Hyotcherl Ihee

Affiliations

  1. Center for Nanomaterials and Chemical Reactions, Institute for Basic Science (IBS), Daejeon 305-701, Republic of Korea. [email protected].

PMID: 26300122 DOI: 10.1039/c5cp03686k

Abstract

Identifying the intermediate species along a reaction pathway is a first step towards a complete understanding of the reaction mechanism, but often this task is not trivial. There has been a strong on-going debate: which of the three intermediates, the CHI2 radical, the CHI2-I isomer, and the CHI2(+) ion, is the dominant intermediate species formed in the photolysis of iodoform (CHI3)? Herein, by combining time-resolved X-ray liquidography (TRXL) and time-resolved X-ray absorption spectroscopy (TR-XAS), we present strong evidence that the CHI2 radical is dominantly formed from the photolysis of CHI3 in methanol at 267 nm within the available time resolution of the techniques (∼20 ps for TRXL and ∼100 ps for TR-XAS). The TRXL measurement, conducted using the time-slicing scheme, detected no CHI2-I isomer within our signal-to-noise ratio, indicating that, if formed, the CHI2-I isomer must be a minor intermediate. The TR-XAS transient spectra measured at the iodine L1 and L3 edges support the same conclusion. The present work demonstrates that the application of these two complementary time-resolved X-ray methods to the same system can provide a detailed understanding of the reaction mechanism.

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