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Ultrafast structural dynamics of in-cage isomerization of diiodomethane in solution

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Title
Ultrafast structural dynamics of in-cage isomerization of diiodomethane in solution
Author(s)
Hanui Kim; Jong Goo Kim; Tae Wu Kim; Sang Jin Lee; Nozawa, Shunsuke; Adachi, Shin-Ichi; Yoon, Kihwan; Kim, Joonghan; Hyotcherl Ihee
Publication Date
2021-02
Journal
CHEMICAL SCIENCE, v.12, no.6, pp.2114 - 2120
Publisher
ROYAL SOC CHEMISTRY
Abstract
Despite extensive studies on the isomer species formed by photodissociation of haloalkanes in solution, the molecular structure of the precursor of the isomer, which is often assumed to be a vibrationally hot isomer formed from the radical pair, and its in-cage isomerization mechanism remain elusive. Here, the structural dynamics of CH2I2 upon 267 nm photoexcitation in methanol were probed with femtosecond X-ray solution scattering at an X-ray free-electron laser. The determined molecular structure of the transiently formed species that converts to the CH2I-I isomer has the I-I distance of 4.17 angstrom, which is longer than that of the isomer (3.15 angstrom) by more than 1.0 angstrom and the mean-squared displacement of 0.45 angstrom(2), which is about 100 times larger than those of typical regular chemical bonds. These unusual structural characteristics are consistent with either a vibrationally hot form of the CH2I-I isomer or the loosely-bound radical pair (CH2IMIDLINE HORIZONTAL ELLIPSISI).
URI
https://pr.ibs.re.kr/handle/8788114/9319
DOI
10.1039/d0sc05108j
ISSN
2041-6520
Appears in Collections:
Center for Nanomaterials and Chemical Reactions(나노물질 및 화학반응 연구단) > 1. Journal Papers (저널논문)
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