Direct single-molecule dynamic detection of chemical reactions
文献类型：期刊论文
| 作者 | Guan, Jianxin1; Jia, Chuancheng1,2; Li, Yanwei3,4; Liu, Zitong2; Wang, Jinying1; Yang, Zhongyue3; Gu, Chunhui1; Su, Dingkai1; Houk, Kendall N.3; Zhang, Deqing2 |
| 刊名 | SCIENCE ADVANCES
 |
| 出版日期 | 2018-02-01 |
| 卷号 | 4期号:2 |
| ISSN号 | 2375-2548 |
| DOI | 10.1126/sciadv.aar2177 |
| 英文摘要 | Single-molecule detection can reveal time trajectories and reaction pathways of individual intermediates/transition states in chemical reactions and biological processes, which is of fundamental importance to elucidate their intrinsic mechanisms. We present a reliable, label-free single-molecule approach that allows us to directly explore the dynamic process of basic chemical reactions at the single-event level by using stable graphene-molecule single-molecule junctions. These junctions are constructed by covalently connecting a single molecule with a 9-fluorenone center to nanogapped graphene electrodes. For the first time, real-time single-molecule electrical measurements unambiguously show reproducible large-amplitude two-level fluctuations that are highly dependent on solvent environments in a nucleophilic addition reaction of hydroxylamine to a carbonyl group. Both theoretical simulations and ensemble experiments prove that this observation originates from the reversible transition between the reactant and a new intermediate state within a time scale of a few microseconds. These investigations open up a new route that is able to be immediately applied to probe fast single-molecule physics or biophysics with high time resolution, making an important contribution to broad fields beyond reaction chemistry. |
| 语种 | 英语 |
| WOS记录号 | WOS:000426845500065 |
| 出版者 | AMER ASSOC ADVANCEMENT SCIENCE |
| 源URL | [http://ir.iccas.ac.cn/handle/121111/45837]  |
| 专题 | 中国科学院化学研究所 |
| 通讯作者 | Houk, Kendall N.; Zhang, Deqing; Guo, Xuefeng |
| 作者单位 | 1.Peking Univ, Coll Chem & Mol Engn, State Key Lab Struct Chem Unstable & Stable Speci, Beijing Natl Lab Mol Sci, Beijing 100871, Peoples R China 2.Chinese Acad Sci, Beijing Natl Lab Mol Sci, Key Lab Organ Solids, Inst Chem, Beijing 100190, Peoples R China 3.Univ Calif Los Angeles, Dept Chem & Biochem, Los Angeles, CA 90095 USA 4.Shandong Univ, Environm Res Inst, Jinan 250100, Shandong, Peoples R China 5.Peking Univ, Dept Mat Sci & Engn, Coll Engn, Beijing 100871, Peoples R China |
| 推荐引用方式 GB/T 7714 | Guan, Jianxin,Jia, Chuancheng,Li, Yanwei,et al. Direct single-molecule dynamic detection of chemical reactions[J]. SCIENCE ADVANCES,2018,4(2). |
| APA | Guan, Jianxin.,Jia, Chuancheng.,Li, Yanwei.,Liu, Zitong.,Wang, Jinying.,...&Guo, Xuefeng.(2018).Direct single-molecule dynamic detection of chemical reactions.SCIENCE ADVANCES,4(2). |
| MLA | Guan, Jianxin,et al."Direct single-molecule dynamic detection of chemical reactions".SCIENCE ADVANCES 4.2(2018). |
入库方式： OAI收割
来源：化学研究所
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