Single-molecule chemical reaction reveals molecular reaction kinetics and dynamics

被引：53

作者：

Zhang, Yuwei ^{[1
]}

Song, Ping ^{[1
]}

Fu, Qiang ^{[1
,2
]}

Ruan, Mingbo ^{[1
]}

Xu, Weilin ^{[1
]}

机构：

[1] Chinese Acad Sci, Changchun Inst Appl Chem, Jilin Prov Key Lab Low Carbon Chem Power, State Key Lab Electroanalyt Chem, Changchun 130022, Peoples R China

[2] Grad Univ Chinese Acad Sci, Beijing 100049, Peoples R China

来源：

NATURE COMMUNICATIONS | 2014年 / 5卷

基金：

国家高技术研究发展计划(863计划); 中国国家自然科学基金;

关键词：

INTERFACIAL ELECTRON-TRANSFER; REACTION PATHWAYS; CONDENSED-PHASE; REDUCTION; DIFFUSION; FLUCTUATIONS; SPECTROSCOPY; CHEMISTRY; RESORUFIN; SYSTEM;

D O I：

10.1038/ncomms5238

中图分类号：

O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];

学科分类号：

07 ; 0710 ; 09 ;

摘要：

Understanding the microscopic elementary process of chemical reactions, especially in condensed phase, is highly desirable for improvement of efficiencies in industrial chemical processes. Here we show an approach to gaining new insights into elementary reactions in condensed phase by combining quantum chemical calculations with a single-molecule analysis. Elementary chemical reactions in liquid-phase, revealed from quantum chemical calculations, are studied by tracking the fluorescence of single dye molecules undergoing a reversible redox process. Statistical analyses of single-molecule trajectories reveal molecular reaction kinetics and dynamics of elementary reactions. The reactivity dynamic fluctuations of single molecules are evidenced and probably arise from either or both of the low-frequency approach of the molecule to the internal surface of the SiO2 nanosphere or the molecule diffusion-induced memory effect. This new approach could be applied to other chemical reactions in liquid phase to gain more insight into their molecular reaction kinetics and the dynamics of elementary steps.

引用

页数：8

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