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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
Source PublicationFARADAY DISCUSSIONS
ISSN1359-6640
Volume194Pages:537-562
Subtype期刊论文
AbstractWe 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.
DOI10.1039/c6fd00085a
Indexed BySCI
Language英语
WOS IDWOS:000392422200025
Citation statistics
Cited Times:8[WOS]   [WOS Record]     [Related Records in WOS]
Document Type期刊论文
Identifierhttp://ir.sinap.ac.cn/handle/331007/26510
Collection中科院上海应用物理研究所2011-2018年
Corresponding AuthorUeda, 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.
Recommended Citation
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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