物理化学学报 >> 2019, Vol. 35 >> Issue (8): 829-839.doi: 10.3866/PKU.WHXB201811027

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基于裂结技术的单分子尺度化学反应研究进展

余培锴,冯安妮,赵世强,魏珺颖,杨扬*(),师佳,洪文晶*()   

  • 收稿日期:2018-11-16 录用日期:2018-12-20 发布日期:2018-12-25
  • 通讯作者: 杨扬,洪文晶 E-mail:yangyang@xmu.edu.cn;whong@xmu.edu.cn
  • 作者简介:杨扬,1986年生。2014年在厦门大学获博士学位;现为厦门大学萨本栋微米纳米科学技术研究院助理教授、硕士生导师。主要研究方向为单分子器件、界面电化学和纳米尺度构筑方法|洪文晶,1985年生。2013年在瑞士的伯尔尼大学获博士学位;国家优秀青年基金获得者,现为厦门大学化学化工学院教授、博士生导师、教授委员会副主任、化工系主任。主要研究方向为单分子尺度研究、精密科学仪器研发和人工智能的工业应用
  • 基金资助:
    国家重点研发计划(2017YFA0204902);福建省自然科学基金(2016J05162)

Recent Progress of Break Junction Technique in Single-Molecule Reaction Chemistry

Peikai YU,Anni FENG,Shiqiang ZHAO,Junying WEI,Yang YANG*(),Jia SHI,Wenjing HONG*()   

  • Received:2018-11-16 Accepted:2018-12-20 Published:2018-12-25
  • Contact: Yang YANG,Wenjing HONG E-mail:yangyang@xmu.edu.cn;whong@xmu.edu.cn
  • Supported by:
    the National Key R & D Program of China(2017YFA0204902);the Natural Science Foundation of Fujian Province, China(2016J05162)

摘要:

分子电子学是研究单分子器件的构筑、性质以及功能调控的一门新兴学科。其中,金属/分子/金属结的构筑和表征是现阶段分子电子学的主要研究内容。裂结技术是当前分子电子学研究的主要实验方法,主要包括机械可控裂结技术和扫描隧道显微镜裂结技术。本文对裂结技术进行了介绍,并对近年来利用这些技术,在单分子尺度化学反应的检测和动力学研究,以及将这些技术与溶液环境、静电场、电化学门控等方法相结合,调控单分子器件的电输运性质等方面所取得的进展进行了概述。

关键词: 分子电子学, 单分子, 电输运, 机械可控裂结, 扫描隧道显微镜裂结

Abstract:

Molecular electronics has been the subject of increasing interest since 1974. Although it describes the utilization of single molecules as active components of electrical devices, molecular electronics remains a fundamental subject to date. Considering that the length of a single molecule is typically several nanometers, the electrical characterization of a probe molecule is a significant experimental challenge. A metal/molecule/metal junction can bridge the gap between nanometer-sized molecules and the macroscopic measuring circuit and is, thus, generally considered as the most common prototype in molecular electronics. For the fabrication and characterization of single-molecule junctions, break junction methods, which include the mechanically controllable break junction (MCBJ) technique and the scanning tunneling microscopy-break junction (STM-BJ) technique, were proposed at the turn of the century and have been developed rapidly in recent years. These methods are widely employed in the experimental study of charge transport through single-molecule junctions and provide a platform to investigate the physical and chemical processes at the single-molecule level. In this review, we mainly focus on MCBJ and STM-BJ techniques applicable for single-molecule conductance measurement and highlight the progress of these techniques in the context of identification and modulation of chemical reactions and evaluation of their reaction kinetics at the single-molecule level. We begin by presenting the operation principles of MCBJ and STM-BJ and stating their brief comparison. Subsequently, we summarize the recent advances in modulating single-molecule chemical reactions. In this regard, we introduce several examples that involve changing the environmental solution, applying an external electrical field, and resorting to electrochemical gating. Next, we overview the application of the break junction techniques in the investigation of reaction kinetics at the single-molecule level. In this section, we also present a brief introduction to studies on single-molecule reaction kinetics using graphene-based nanogaps, wherein conventional metallic electrodes were replaced by graphene electrodes. Furthermore, we discuss the combination of break junction techniques and surface-enhanced Raman spectroscopy for detecting single-molecule reactions occurring at nanometer-scale separation. We discuss the historical development of this combined method and present the latest advancement explaining the origin of the low conductance of 1, 4-benzenedithiol, which is a topic of significant concern in single-molecule electronics. Finally, we discuss some future issues in molecular electronics, including the expansion from simple molecules to complex molecular systems and the introduction of multi-physical fields into single-molecule junctions. Moreover, we provide a list of critical characterization tools in molecular electronics and discuss their potential applications.

Key words: Molecular electronics, Single molecule, Charge transport, Mechanically controllable break junction, STM break junction