Collaborative Research: Probing and Controlling Binding Structure and Electron Transport in Molecular Electronic Devices--A Coordinated Computational and Experimental Study

合作研究：探测和控制分子电子器件中的结合结构和电子传输——协调计算和实验研究

• 批准号: 1609788
• 负责人: Bingqian Xu
• 金额: $ 17.82万
• 依托单位: University of Georgia Research Foundation Inc
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-06-01 至 2019-12-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1609788&HistoricalAwards=false
• 关键词: Collaborative; Research; Probing; Controlling; Binding

Abstract:Non-Technical:Molecular electronics started with the idea of wiring an individual molecule to two metal electrodes, called single-molecule junctions, as an analogy of single electronic components in commercial microelectronic devices to overcome the limit of famous Moore's prediction. In a single molecular junction, perhaps the most elusive factor that influences the electron transport properties lies in the molecule-electrode contact interfaces. Despite continuous experimental achievements and the conceptual simplicity of molecular electronic devices, challenges for their theoretical understanding of the correlation between electron transport and molecular binding structures are still unresolved. Therefore, probing and controlling the structure and dynamics of single-molecule junctions and consequently controlling the molecular transport of these junctions are critical to the development of this field. The project will integrate molecular simulations for the self-assembly and nanocontact dynamics at surface and interface, and experimental mechanics and electron transport measurements of single-molecule junctions. The project will provide a deep understanding of many transition phenomena observed in molecular force and conductance measurements. If successful, the research will have tremendous impact on molecular electronics community and many other areas, such as energy research and molecular force spectroscopy. The education and outreach objective of this proposal is to tightly integrate the research efforts and results with graduate, undergraduate, and K-12 education and to globally disseminate both research and the education outcomes.Technical:Although the electrical conductance and mechanical properties of single-molecule junctions have achieved significant progress over the past decade, challenges of a detailed understanding of molecular binding structures and electron transport, and the structure-force-conductance correlations, are still unresolved. This research will develop a combined molecular simulation and scanning probe microscope break-junction technique to probe and control the structure and dynamics in molecular electronics devices: (1) Performing molecular simulations by using as close as possible the experimental parameters, dynamics of electrode and realistic atomic interactions to understand the binding structure and force measurement in scanning probe experiment; (2) Developing a dual-mode feedback system with AC-coupled high speed amplifier at radio frequency to capture the key transitions of molecular binding sites that induce conductance changes. The experimental data at nanosecond (ns) timescale will be directly compared with molecular simulation results; (3) Using the coordinated molecular simulation and scanning probe break-junction experiment to probe the structure and dynamics of selected benchmark systems under different mode trainings. Multi-variable force-conductance two-dimensional cross-correlation histogram analyses for the force and conductance traces will be performed in experiments and simulations, and the distinct stable configurations of molecular junctions will be identified. The coordinated computational and experimental research project will also provide an interdisciplinary research for students in materials, mechanics, chemistry, electronics, and computational materials science.

摘要：非技术性：分子电子学始于将单个分子连接到两个金属电极（称为单分子结）的想法，类似于商业微电子设备中的单个电子元件，以克服著名的摩尔预测的限制。在单个分子结中，影响电子传输特性的最难以捉摸的因素可能在于分子-电极接触界面。尽管不断取得实验成果并且分子电子器件的概念简单，但对电子传输和分子结合结构之间相关性的理论理解的挑战仍未解决。因此，探测和控制单分子连接的结构和动力学，从而控制这些连接的分子运输对于该领域的发展至关重要。该项目将整合表面和界面自组装和纳米接触动力学的分子模拟，以及单分子结的实验力学和电子传输测量。该项目将深入了解分子力和电导测量中观察到的许多转变现象。如果成功，该研究将对分子电子学界和许多其他领域产生巨大影响，例如能源研究和分子力谱学。该提案的教育和推广目标是将研究工作和成果与研究生、本科生和 K-12 教育紧密结合，并在全球范围内传播研究和教育成果。分子连接在过去十年中取得了重大进展，但详细理解分子结合结构和电子传输以及结构-力-电导相关性的挑战仍未解决。本研究将开发一种结合分子模拟和扫描探针显微镜断结技术来探测和控制分子电子器件的结构和动力学：（1）使用尽可能接近的实验参数、电极动力学和现实进行分子模拟。原子相互作用，以了解扫描探针实验中的结合结构和力测量； (2)开发具有射频交流耦合高速放大器的双模式反馈系统，以捕获引起电导变化的分子结合位点的关键转变。纳秒（ns）时间尺度的实验数据将直接与分子模拟结果进行比较； (3)利用协调分子模拟和扫描探针断裂连接实验来探究所选基准系统在不同模式训练下的结构和动力学。将在实验和模拟中对力和电导迹线进行多变量力-电导二维互相关直方图分析，并将识别分子连接的独特稳定构型。协调的计算和实验研究项目还将为材料、力学、化学、电子和计算材料科学的学生提供跨学科研究。

项目成果

Metallo‐Helicoid with Double Rims: Polymerization Followed by Folding by Intramolecular Coordination

具有双环的金属螺旋：聚合，然后通过分子内配位折叠

• DOI: 10.1002/ange.202010696
• 发表时间: 2020-11-18
• 期刊: Angewandte Chemie
• 作者: Guangqiang Yin;S. K;apal;apal;Chung;Heng Wang;Jianxiang Huang;Shu‐Ting Jiang;Tan Ji;Yu Yan;S;ra Khalife;ra;Ruhong Zhou;Libin Ye;Bingqian Xu;Hai‐Bo Yang;M. Nieh;Xiaopeng Li
• 通讯作者: Xiaopeng Li

Hierarchical Self-Assembly of Nanowires on the Surface by Metallo-Supramolecular Truncated Cuboctahedra

金属超分子截断立方八面体表面纳米线的分层自组装

• DOI: 10.1021/jacs.1c00625
• 发表时间: 2021-04
• 期刊: Journal of the American Chemical Society
• 影响因子: 15
• 作者: Wang, Heng;Wang, Kun;Xu, Yaping;Wang, Wu;Chen, Shaohua;Hart, Matthew;Wojtas, Lukasz;Zhou, Li;Gan, Lin;Yan, Xuzhou;et al
• 通讯作者: et al