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
ISSN1359-6640
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.
DOI10.1039/c6fd00085a
收录类别SCI
语种英语
WOS记录号WOS:000392422200025
引用统计
被引频次:7[WOS]   [WOS记录]     [WOS相关记录]
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.
条目包含的文件 下载所有文件
文件名称/大小 文献类型 版本类型 开放类型 使用许可
Femtosecond charge a(1679KB)期刊论文作者接受稿开放获取CC BY-NC-SA浏览 下载
个性服务
推荐该条目
保存到收藏夹
查看访问统计
导出为Endnote文件
谷歌学术
谷歌学术中相似的文章
[Nagaya, K]的文章
[Motomura, K]的文章
[Kukk, E]的文章
百度学术
百度学术中相似的文章
[Nagaya, K]的文章
[Motomura, K]的文章
[Kukk, E]的文章
必应学术
必应学术中相似的文章
[Nagaya, K]的文章
[Motomura, K]的文章
[Kukk, E]的文章
相关权益政策
暂无数据
收藏/分享
文件名: Femtosecond charge and molecular dynamics of I-containing organic molecules induced by intense X-ray free-electron laser pulses.pdf
格式: Adobe PDF
所有评论 (0)
暂无评论
 

除非特别说明,本系统中所有内容都受版权保护,并保留所有权利。