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Time-resolved high-harmonic spectroscopy of ultrafast photoisomerization dynamics

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Title: Time-resolved high-harmonic spectroscopy of ultrafast photoisomerization dynamics
Authors: Kaneshima, Keisuke Browse this author
Ninota, Yuki Browse this author
Sekikawa, Taro Browse this author →KAKEN DB
Issue Date: 12-Nov-2018
Publisher: Optical Society of America
Journal Title: Optics express
Volume: 26
Issue: 23
Start Page: 31039
End Page: 31054
Publisher DOI: 10.1364/OE.26.031039
Abstract: We report the first time-resolved high-harmonic spectroscopy (TR-HHS) study of a chemical bond rearrangement. We investigate the transient change of the high-harmonic signal from 1,3-cyclohexadiene (CHD), which undergoes ring-opening and isomerizes to 1,3,5-hexatriene (HT) upon photoexcitation. We associated the harmonic yield variation with the changes in the molecule's electronic state and vibrational frequencies, which are caused by isomerization. This showed us that the electronic excited state of CHD created through two-photon absorption of 3.1 eV photons relaxes almost completely within 100 fs to the electronic ground state of CHD with vibrational excitation. Subsequently, the molecule isomerizes to HT (i.e., ring-opening occurs, around 400 fs after the excitation). The present results demonstrate that TR-HHS, which can track both electronic and nuclear dynamics, is a powerful tool for studying ultrafast photochemical reactions.
Rights: © 2018 Optical Society of America. Users may use, reuse, and build upon the article, or use the article for text or data mining, so long as such uses are for non-commercial purposes and appropriate attribution is maintained. All other rights are reserved.
Type: article
Appears in Collections:工学院・工学研究院 (Graduate School of Engineering / Faculty of Engineering) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 金島 圭佑

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