金属/分子/金属结的电子输运机理与表征

doi:10.7503/cjcu20140941

高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (1): 9-23.doi: 10.7503/cjcu20140941

金属/分子/金属结的电子输运机理与表征

杨扬, 刘俊扬, 晏润文, 吴德印, 田中群()

固体表面物理化学国家重点实验室, 厦门大学化学化工学院化学系, 厦门 361005

收稿日期:2014-10-24 修回日期:2014-12-23 出版日期:2015-01-10 发布日期:2014-12-23
作者简介:联系人简介:田中群, 男,博士,教授, 博士生导师, 中国科学院院士, 主要从事拉曼光谱、电化学、合成化学、催组装和分子电子学等方面的研究. E-mail: zqtian@xmu.edu.cn
基金资助:
科技部鄄国家重大科学仪器设备开发专项项目(批准号: 2011YQ030124) 和国家自然科学基金(批准号: 21321062,21373172)资助.

Mechanism and Characterization of Electron Transport Through Metal/Molecule/Metal Junctions^†

YANG Yang, LIU Junyang, YAN Runwen, WU Deyin, TIAN Zhongqun^*()

State Key Laboratory of Physical Chemistry of Solid Surfaces, Department of Chemistry, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, China

Received:2014-10-24 Revised:2014-12-23 Online:2015-01-10 Published:2014-12-23
Contact: TIAN Zhongqun E-mail:zqtian@xmu.edu.cn
Supported by:
Supported by the National Key Scientific Instrument and Equipment Development Projects of the Ministry of Science and Technology of China(No. 2011YQ030124) and the National Natural Science Foundation of China(Nos. 21321062, 21373172).

摘要/Abstract

摘要：

金属/分子/金属结是分子电子学中的基本单元. 根据电子的相位是否发生改变, 分子结中的电子输运可以分为相干输运和非相干输运两类. 在实验上, 分子结的表征方法可以分为电学性质表征和非电学性质表征两类. 本文借助能级图, 首先对分子结的电子输运机理作了简明解释. 在此基础上, 结合文献报道和本课题组此前的工作, 对分子结的一些常用电学表征方法, 包括电流-电压特性曲线、电流-时间曲线、电导统计柱状图、转变电压谱、散粒噪声测试、非弹性电子隧道谱和热电效应法进行了介绍.

关键词: 分子电子学, 金属/分子/金属结, 电子输运, 自组装, 单分子电导

Abstract:

Although molecular electronics emerged several decades ago, it is still concerning about fundamental issues so far. Metal/molecule/metal junction is a conceptually basic unit in molecular electronics. The mechanism of electron transport through metal/molecule/metal junction has attracted great interest. In general, the mechanisms for electron transport through metal/molecule/metal junctions can be divided into two categories: coherent transport and non-coherent transport according to the phase change of tunneling electrons. In this review, the electron transport mechanism is illustrated briefly by employing energy diagrams. More-over, several extensively measured approaches for studying metal/molecule/metal junctions, including I-V characteristic curve, I-t trace and conductance histogram, transition voltage spectroscopy, shot noise, inelastic electron tunneling spectroscopy, and thermoelectricity are introduced through referring to some recent publications including our works.

Key words: Molecular electronics, Metal/molecule/metal junction, Electron transport, Self-assembly, Single molecule conductance

中图分类号:

O641

杨扬, 刘俊扬, 晏润文, 吴德印, 田中群. 金属/分子/金属结的电子输运机理与表征[J]. 高等学校化学学报, 2015, 36(1): 9-23.

YANG Yang, LIU Junyang, YAN Runwen, WU Deyin, TIAN Zhongqun. Mechanism and Characterization of Electron Transport Through Metal/Molecule/Metal Junctions^†[J]. Chemical Journal of Chinese Universities, 2015, 36(1): 9-23.

图/表 13

Fig.1 Typical representation of metal/molecule/ metal junction A 4,4'-bipyridine molecule is covalently bound to Au electrodes pair.

Fig.2 Energy diagram for a D-B-A protocol molecular junction Ef: Fermi enegy. ϕ: barrier height.

Fig.3 Energy diagram showing the hopping mechanism in a D-B-A protocol molecular junction

Fig.4 Relationship between most probable electron transport mechanisms for metal/molecule/metal junction[35,40]

Table 1 Relationship between transporting current and experimental condition for metal/molecule/metal junction under different electron transport mechanisms[35,40]*

Mechanism	Temperature	Length	Voltage
Superexchange	None	I∝exp(-βd)	I∝V
Fowler-Nordheim Tunneling	None	I∝exp(-βd)	ln(I/V²)∝1/V
Steady state hopping	ln(I/V)∝1/T	I∝d^-1	I∝V
Non-directional hopping	ln(I/V)∝1/T	I∝d^-2	I∝V

Fig.5 Typical I-V characteristic and conductance-voltage(G-V) curves for Au/BDT/Au single molecules junction[27]

Fig.6 Energy diagrams of a metal/molecule/metal junction under Vbias=0(A) and Vbias≠0(B), respectively

Fig.7 Schematic description of STM-break junction method for fabricating metal/molecule/metal junction(A), (C) and(E) give the measured conductance curves, while (B), (D) and (F) illustrate the corresponding conductance histograms. Herein (E) and (F) are the data obtained without probe molecule[30].

Table 2 Comparison of conductance values of Au/BDT/Au by employing different approaches

Approach	Normalized value/G₀	Ref.	Approach	Normalized value/G₀	Ref.
I-V curve	5.86× 10^-4	[27]	Conductance histogram	1.0×10^-2	[67]
I-V curve	1.43×10^-3	[64]	Conductance histogram	4.0×10^-3	[68]
I-V curve	4.96×10^-5	[65]	Conductance histogram	1.0×10^-2	[69]
Conductance histogram	1.1×10^-2	[66]	Conductance histogram	1.0×10^-2	[18]

Fig.8 Measured Fowler-Nordheim plot corresponding to the I-V curve(the inset) of an Au/anthracenethiol/Au molecular junction The dashed curve indicates the transition from direct to Fowler-Nordheim tunneling[70].

Fig.9 Measured shot noise as a function of current for Pt/D2/Pt molecular junction(filled circle) The molecular junction conductance for this set of shot noise data is 1.010 G0. The shot noise can be described quite well with theory assuming {τi}= {0.995, 0.015}. Nevertheless, if {τi} is slightly changed to {0.985, 0.025}, the fitted curve cannot describe the shot noise at all[89].

Fig.10 Schematic presentation of inelastic electron tunneling spectroscopy(IETS)

Fig.11 Measured thermoelectric voltage for Au/1,4-bezenedithiol/Au junction and clean Au/Au junction as there is a temperature differential(ΔT = 20 K)(A), response of molecule thermoelectric voltage for Au/1,4-bezenedithiol/Au junction as ΔT changed(C), theoretically predicted transmission function for Au/1,4-bezenedithiol/Au junction by employing nonequilibrium Green’s function formalism combined with extended Hückel theory(B) and theoretically predicted Seebeck coefficient for Au/1,4-bezenedithiol/Au junction[124](D)

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金属/分子/金属结的电子输运机理与表征

Mechanism and Characterization of Electron Transport Through Metal/Molecule/Metal Junctions^†

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金属/分子/金属结的电子输运机理与表征

Mechanism and Characterization of Electron Transport Through Metal/Molecule/Metal Junctions†

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Mechanism and Characterization of Electron Transport Through Metal/Molecule/Metal Junctions^†