Direct single-molecule dynamic detection of chemical reactions

doi:10.1126/sciadv.aar2177

CORC > 化学研究所 > 中国科学院化学研究所

	Direct single-molecule dynamic detection of chemical reactions
	Guan, Jianxin 1; Jia, Chuancheng 1,2; Li, Yanwei 3,4; Liu, Zitong 2; Wang, Jinying 1; Yang, Zhongyue 3; Gu, Chunhui 1; Su, Dingkai 1; Houk, Kendall N.3; Zhang, Deqing 2
刊名	SCIENCE ADVANCES
	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
出版者	AMER ASSOC ADVANCEMENT SCIENCE
WOS记录号	WOS:000426845500065
内容类型	期刊论文
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).