Effect of side group on mechanically induced conductance switching in 4,40-dipyridyl-based single-molecule junctions

doi:10.1088/1674-1056/adce98

中国物理B ›› 2025, Vol. 34 ›› Issue (8): 87202-087202.doi: 10.1088/1674-1056/adce98

Effect of side group on mechanically induced conductance switching in 4,40-dipyridyl-based single-molecule junctions

Zhen Wan(万振)^1,†, Chang-Feng Zheng(郑长风)^1,†, Lin Liu(刘琳)¹, Yun-Long Ge(葛云龙)¹, Guang-Ping Zhang(张广平)^1,‡, Shuai Qiu(邱帅)¹, Hui Wang(王辉)², and Zong-Liang Li(李宗良)^1,§

1 Shandong Key Laboratory of Medical Physics and Image Processing & Shandong Provincial Engineering and Technical Center of Light Manipulations, School of Physics and Electronics, Shandong Normal University, Jinan 250358, China;
2 College of Physics and Electronic Engineering, Qilu Normal University, Jinan 250200, China

收稿日期:2025-02-11 修回日期:2025-03-11 接受日期:2025-04-21 出版日期:2025-07-17 发布日期:2025-08-05
通讯作者: Guang-Ping Zhang, Zong-Liang Li E-mail:zhangguangping@sdnu.edu.cn;lizongliang@sdnu.edu.cn
基金资助:
Project supported by the National Natural Science Foundation of China (Grant Nos. 12474286, 22173052, and 12204281).

Effect of side group on mechanically induced conductance switching in 4,40-dipyridyl-based single-molecule junctions

1 Shandong Key Laboratory of Medical Physics and Image Processing & Shandong Provincial Engineering and Technical Center of Light Manipulations, School of Physics and Electronics, Shandong Normal University, Jinan 250358, China;
2 College of Physics and Electronic Engineering, Qilu Normal University, Jinan 250200, China

Received:2025-02-11 Revised:2025-03-11 Accepted:2025-04-21 Online:2025-07-17 Published:2025-08-05
Contact: Guang-Ping Zhang, Zong-Liang Li E-mail:zhangguangping@sdnu.edu.cn;lizongliang@sdnu.edu.cn
Supported by:
Project supported by the National Natural Science Foundation of China (Grant Nos. 12474286, 22173052, and 12204281).

摘要/Abstract

摘要： The forming processes of $4,4^{\prime}$-dipyridyl-based single-molecule junctions and mechanically induced conductance switching as well as the side-group effects are systematically investigated by applying the ab initio-based adiabatic geometric optimization method and the one-dimensional transmission combined with three-dimensional correction approximation (OTCTCA) method. The numerical results show that for the $4,4^{\prime}$-dipyridyl with a $\pi$-conjugated phenyl-phosphoryl or diphenylsilyl side group, the pyridyl vertically anchors on the second atomic layer of the pyramid-shaped Au tip electrode at small inter-electrode distances by laterally pushing the apical Au atom aside, which induces stronger pyridyl-electrode coupling and high-conductance state of the formed junctions. As the inter-electrode distance increases, the pyridyl shifts to the apical Au atom of the tip electrode. This apical Au atom introduces additional scatterings to the tunneling electrons and significantly decreases the conductance of the junctions. Furthermore, for the $4,4^{\prime}$-dipyridyl with a phenyl-phosphoryl side group, the probability of manifesting the high-conductance state is decreased due to the oxygen atom reducing the probability of the pyridyl adsorbing on the second layer of Au tip electrode. In contrast, for the $4,4^{\prime}$-dipyridyl with a non-conjugated cyclohexyl-phosphoryl side group, the steric hindrance from the bulky cyclohexyl group leads the molecule to preferentially form the O-Au contact, which prevents both the high conductance and mechanically induced conductance switching of the junction. Our results provide a theoretical understanding of the side-group effects on electronic transport properties of single-molecule junctions, offering an alternative explanation for the experimental observations.

关键词: single-molecule junction, electron transport properties, conductance switching, side-group effects

Abstract: The forming processes of $4,4^{\prime}$-dipyridyl-based single-molecule junctions and mechanically induced conductance switching as well as the side-group effects are systematically investigated by applying the ab initio-based adiabatic geometric optimization method and the one-dimensional transmission combined with three-dimensional correction approximation (OTCTCA) method. The numerical results show that for the $4,4^{\prime}$-dipyridyl with a $\pi$-conjugated phenyl-phosphoryl or diphenylsilyl side group, the pyridyl vertically anchors on the second atomic layer of the pyramid-shaped Au tip electrode at small inter-electrode distances by laterally pushing the apical Au atom aside, which induces stronger pyridyl-electrode coupling and high-conductance state of the formed junctions. As the inter-electrode distance increases, the pyridyl shifts to the apical Au atom of the tip electrode. This apical Au atom introduces additional scatterings to the tunneling electrons and significantly decreases the conductance of the junctions. Furthermore, for the $4,4^{\prime}$-dipyridyl with a phenyl-phosphoryl side group, the probability of manifesting the high-conductance state is decreased due to the oxygen atom reducing the probability of the pyridyl adsorbing on the second layer of Au tip electrode. In contrast, for the $4,4^{\prime}$-dipyridyl with a non-conjugated cyclohexyl-phosphoryl side group, the steric hindrance from the bulky cyclohexyl group leads the molecule to preferentially form the O-Au contact, which prevents both the high conductance and mechanically induced conductance switching of the junction. Our results provide a theoretical understanding of the side-group effects on electronic transport properties of single-molecule junctions, offering an alternative explanation for the experimental observations.

Key words: single-molecule junction, electron transport properties, conductance switching, side-group effects

中图分类号: (Molecular electronic devices)

85.65.+h

73.63.-b (Electronic transport in nanoscale materials and structures) 73.63.Rt (Nanoscale contacts) 82.20.Wt (Computational modeling; simulation)

Zhen Wan(万振), Chang-Feng Zheng(郑长风), Lin Liu(刘琳), Yun-Long Ge(葛云龙), Guang-Ping Zhang(张广平), Shuai Qiu(邱帅), Hui Wang(王辉), and Zong-Liang Li(李宗良). Effect of side group on mechanically induced conductance switching in 4,40-dipyridyl-based single-molecule junctions[J]. 中国物理B, 2025, 34(8): 87202-087202.

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Effect of side group on mechanically induced conductance switching in 4,40-dipyridyl-based single-molecule junctions

Effect of side group on mechanically induced conductance switching in 4,40-dipyridyl-based single-molecule junctions

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