Femtosecond charge and molecular dynamics of I-containing organic molecules induced by intense X-ray free-electron laser pulses

doi:10.1039/c6fd00085a

CAS OpenIR > 中科院上海应用物理研究所2011-2018年

	Femtosecond charge and molecular dynamics of I-containing organic molecules induced by intense X-ray free-electron laser pulses
	Nagaya, K; Motomura, K; Kukk, E; Takahashi, Y; Yamazaki, K; Ohmura, S; Fukuzawa, H; Wada, S; Mondal, S; Tachibana, T; Ito, Y; Koga, R; Sakai, T; Matsunami, K; Nakamura, K; Kanno, M; Rudenko, A; Nicolas, C; Liu, XJ; Miron, C; Zhang, Y; Jiang, Y; Chen, J; Anand, M; Kim, DE; Tono, K; Yabashi, M; Yao, M; Konoe, H; Ueda, K; Ueda, K (reprint author), RIKEN SPring 8 Ctr, Sayo, Hyogo 6795148, Japan.; Ueda, K (reprint author), Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Sendai, Miyagi 9808577, Japan.
	2016
发表期刊	FARADAY DISCUSSIONS
ISSN	1359-6640
卷号	194 页码:537-562
文章类型	期刊论文
摘要	We studied the electronic and nuclear dynamics of I-containing organic molecules induced by intense hard X-ray pulses at the XFEL facility SACLA in Japan. The interaction with the intense XFEL pulse causes absorption of multiple X-ray photons by the iodine atom, which results in the creation of many electronic vacancies (positive charges) via the sequential electronic relaxation in the iodine, followed by intramolecular charge redistribution. In a previous study we investigated the subsequent fragmentation by Coulomb explosion of the simplest I-substituted hydrocarbon, iodomethane (CH3I). We carried out three-dimensional momentum correlation measurements of the atomic ions created via Coulomb explosion of the molecule and found that a classical Coulomb explosion model including charge evolution (CCE-CE model), which accounts for the concerted dynamics of nuclear motion and charge creation/charge redistribution, reproduces well the observed momentum correlation maps of fragment ions emitted after XFEL irradiation. Then we extended the study to 5-iodouracil (C4H3IN2O2, 5-IU), which is a more complex molecule of biological relevance, and confirmed that, in both CH3I and 5-IU, the charge build-up takes about 10 fs, while the charge is redistributed among atoms within only a few fs. We also adopted a self-consistent charge density-functional based tight-binding (SCC-DFTB) method to treat the fragmentations of highly charged 5-IU ions created by XFEL pulses. Our SCC-DFTB modeling reproduces well the experimental and CCE-CE results. We have also investigated the influence of the nuclear dynamics on the charge redistribution (charge transfer) using nonadiabatic quantum-mechanical molecular dynamics (NAQMD) simulation. The time scale of the charge transfer from the iodine atomic site to the uracil ring induced by nuclear motion turned out to be only similar to 5 fs, indicating that, besides the molecular Auger decay in which molecular orbitals delocalized over the iodine site and the uracil ring are involved, the nuclear dynamics also play a role for ultrafast charge redistribution. The present study illustrates that the CCE-CE model as well as the SCC-DFTB method can be used for reconstructing the positions of atoms in motion, in combination with the momentum correlation measurement of the atomic ions created via XFEL-induced Coulomb explosion of molecules.
DOI	10.1039/c6fd00085a
收录类别	SCI
语种	英语
WOS记录号	WOS:000392422200025
引用统计
文献类型	期刊论文
条目标识符	http://ir.sinap.ac.cn/handle/331007/26510
专题	中科院上海应用物理研究所2011-2018年
通讯作者	Ueda, K (reprint author), RIKEN SPring 8 Ctr, Sayo, Hyogo 6795148, Japan.; Ueda, K (reprint author), Tohoku Univ, Inst Multidisciplinary Res Adv Mat, Sendai, Miyagi 9808577, Japan.
推荐引用方式 GB/T 7714	Nagaya, K,Motomura, K,Kukk, E,et al. Femtosecond charge and molecular dynamics of I-containing organic molecules induced by intense X-ray free-electron laser pulses[J]. FARADAY DISCUSSIONS,2016,194:537-562.
APA	Nagaya, K.,Motomura, K.,Kukk, E.,Takahashi, Y.,Yamazaki, K.,...&Ueda, K .(2016).Femtosecond charge and molecular dynamics of I-containing organic molecules induced by intense X-ray free-electron laser pulses.FARADAY DISCUSSIONS,194,537-562.
MLA	Nagaya, K,et al."Femtosecond charge and molecular dynamics of I-containing organic molecules induced by intense X-ray free-electron laser pulses".FARADAY DISCUSSIONS 194(2016):537-562.

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