单分子器件电输运中基于量子干涉效应的调控策略

李瑞豪; 刘俊扬; 洪文晶

doi:10.7498/aps.71.20211819

摘要

单分子器件电输运中的量子干涉效应是电子在分子独立的轨道能级内传输时因保持量子相干性, 从而在不同能级之间发生相互干涉的现象. 这种现象导致了电子在单分子器件内透射概率的增加或减小, 在实验中体现为单分子器件电导值的升高或降低. 近些年, 利用量子干涉效应对不同的单分子器件进行调控在实验中被证实是有效的调控手段, 如对单分子开关、单分子热电器件、单分子自旋器件等器件性能的调控. 本文介绍了量子干涉效应的相关理论与预测、实验观测与证实, 以及其在不同单分子器件上的调控作用.

关键词:

Abstract

The quantum interference effect in single-molecule devices is a phenomenon in which electrons are coherently transported through different frontier molecular orbitals with multiple energy levels, and the interference will occur between different energy levels. This phenomenon results in the increase or decrease of the probability of electron transmission in the electrical transport of the single-molecule device, and it is manifested in the experiment when the conductance value of the single-molecule device increases or decreases. In recent years, the use of quantum interference effects to control the electron transport in single-molecule device has proved to be an effective method, such as single-molecule switches, single-molecule thermoelectric devices, and single-molecule spintronic devices. In this work, we introduce the related theories of quantum interference effects, early experimental observations, and their regulatory role in single-molecule devices.

Keywords:

作者及机构信息

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

通信作者: 刘俊扬, jyliu@xmu.edu.cn ; 洪文晶, whong@xmu.edu.cn

基金项目: 国家自然科学基金(批准号: 21933012, 31871877)、国家重点研发计划(批准号: 2017YFA0204902)和中央高校基本科研业务费专项资金(批准号: 20720200068, 20720190002)资助的课题

Authors and contacts

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

Corresponding author: Liu Jun-Yang, jyliu@xmu.edu.cn ; Hong Wen-Jing, whong@xmu.edu.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant Nos. 21933012, 31871877), the National Key R&D Program of China (Grant No. 2017YFA0204902), and the Fundamental Research Funds for the Central Universities, China (Grant Nos. 20720200068, 20720190002).

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施引文献

图 1 单分子器件量子干涉效应的理论预测、实验观测以及对于器件性能的调控

Fig. 1. Theoretical prediction, experimental observation and regulation of quantum interference effect in single-molecule devices.

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图 2 (a)分子结的电学测量示意图; (b)分子结的电输运原理图; (c)通过苯环的对位和间位进行连接的分子上的电输运通路; (d)具有相增量子干涉效应(红色)和相消量子干涉效应(蓝色)的分子的透射谱^[20]

Fig. 2. (a) Schematic of the electrical measurement of molecular junction; (b) the mechanism of electron transport in a molecular junction; (c) different electron transport pathways in Para and Meta site connected benzene ring; (d) the transmission spectrum of molecules with CQI (red) and DQI (blue) effects respectively^[20].

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图 3 (a)分子AC, AQ和AH的结构^[35]; (b)—(d)分别为AC, AQ和AH的单分子一维电导图^[35]; (e)分子AQ-DT, AQ-MT, AC-DT以及OPE3-DT的分子结构^[37]; (f), (g)分别为AC-DT和AQ-DT分子层的I-V特性曲线^[37]; (h)理论计算的AQ-MT, AC-DT以及AQ-DT的透射谱^[37]

Fig. 3. (a) Molecular structure of AC, AQ and AH respectively^[35]; (b)–(d) the one-dimensional conductance histogram of AC, AQ and AH respectively^[35]; (e) the molecular structure of AQ-DT, AQ-MT, AC-DT and OPE3-DT^[37]; (f), (g) the two-dimensional I-V histogram of AC-DT and AQ-DT respectively^[37]; (h) the transmission spectrum of AQ-MT, AC-DT, and AQ-DT^[37].

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图 4 (a)上方图表示费米能级在2个相同相位的分子轨道之间引起的相消量子干涉示意图, 下方图表示费米能级在2个具有相反相位的分子轨道上方引起的相消量子干涉示意图; (b)分别对应图(a)中2种相消量子干涉效应的透射谱; (c) 3个目标分子的一维电导统计图; (d) 3个目标分子的I-V特性曲线图; (e) 3号分子在方波电压激励下的电流响应; (f) 3个目标分子的透射谱^[49]

Fig. 4. (a) Schematic diagram of DQI caused by Fermi level between two molecular orbitals with the same phase (upper) and the schematic diagram of DQI caused by Fermi level above two molecular orbitals with opposite phase (lower); (b) the transmission spectrum corresponding to the two DQI mechanisms shown in (a); (c) one-dimensional conductance histograms of three target molecules; (d) I-V curves of three target molecules; (e) the current response square wave voltage modulation of molecular 3; (f) transmission spectrum of three target molecules^[49].

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图 5 (a), (b)分别为Para-OPE3和Meta-OPE3的分子结构; (c), (d)分别为Para-OPE3和Meta-OPE3在不同温度下的热电势; (e) Para-OPE3和Meta-OPE3的透射谱; (f)由透射谱得到的Para-OPE3和Meta-OPE3的透射概率斜率随能级的变化谱^[69]

Fig. 5. (a), (b) Geometry of Para-OPE3 and Meta-OPE3 molecular junctions respectively; (c), (d) the thermoelectric voltages as a function of ΔT of Para-OPE3 and Meta-OPE3 respectively; (e) the transmission spectrum of Para-OPE3 and Meta-OPE3; (f) the slope of transmission at logarithm scale of Para-OPE3 and Meta-OPE3^[69].

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图 6 (a)银/钒烯/银单分子结量子电流通路引起的自旋滤波示意图; (b)银/钒烯/银单分子结的自旋极化电导图; (c), (d)分别为银/钒烯/银和银/二茂铁/银单分子结的法诺系数; (e)银/钒烯/银单分子结垂直构型电子输运路径; (f)不同输运路径的自旋分辨电子输运透射率^[73]

Fig. 6. (a) Schematic of the Ag/vanadocene/Ag molecular junction of spin filter that induced by quantum interference; (b) schematic of the Ag/vanadocene molecular spin polarization junction; (c), (d) Fano factor of Ag/vanadocene/Ag and Ag/ferrocene/Ag junctions respectively; (e) spin transmission across the Ag/vanadocene/Ag junction of perpendicular molecular junction; (f) spin transmission in different charge transport pathways^[73].

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图 7 (a) SPPO分子加酸之后的2种共振式; (b), (c)分别为SPPO分子以及加酸之后形成的SPPO-H⁺的二维电导-长度统计图, 插入的小图为台阶长度统计图^[74]; (d) DTB-A与DTB-B分子结示意图; (e), (f)分别为DTB-A与DTB-B加氟离子前后一维电导图^[75]

Fig. 7. (a) Two resonance structures of SPPO after protonation with acid; (b), (c) the 1D conductance-displacement histogram of SPPO and SPPO-H⁺ respectively, where the inset is the displacement count histogram^[74]; (d) the molecular structure of DTB-A and DTB-B; (e), (f) the one-dimensional conductance histograms of DTB-A and DTB-B in TMB solvent and introduction of the fluoride ion respectively^[75].

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单分子器件电输运中基于量子干涉效应的调控策略