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Nearfield trapping increases lifetime of single-molecule junction by one order of magnitude
Cell Reports Physical Science ( IF 8.9 ) Pub Date : 2021-04-01 , DOI: 10.1016/j.xcrp.2021.100389
Albert C. Aragonès , Katrin F. Domke

Progress in molecular electronics (ME) is largely based on improved understanding of the properties of single molecules (SMs) trapped for seconds or longer to enable their detailed characterization. We present a plasmon-supported break-junction (PBJ) platform to significantly increase the lifetime of SM junctions of 1,4-benzenedithiol (BDT) without the need for chemical modification of molecule or electrode. Moderate far-field power densities of ca. 11 mW/μm2 lead to a >10-fold increase in minimum lifetime compared with laser-OFF conditions. The nearfield trapping efficiency is twice as large for bridge-site contact compared with hollow-site geometry, which can be attributed to the difference in polarizability. Current measurements and tip-enhanced Raman spectra confirm that native structure and contact geometry of BDT are preserved during the PBJ experiment. By providing a non-invasive pathway to increase short lifetimes of SM junctions, PBJ is a valuable approach for ME, paving the way for improved SM sensing and recognition platforms.



中文翻译:

近场捕获将单分子结的寿命提高了一个数量级

分子电子学(ME)的进步主要基于对单个分子(SM)的性能的更好理解,这些分子被困了几秒钟或更长时间才能对其进行详细的表征。我们提出了一种等离激元支持的断裂连接(PBJ)平台,可以显着增加1,4-苯二硫醇(BDT)的SM连接的寿命,而无需对分子或电极进行化学修饰。中等的远场功率密度约为 11毫瓦/微米2与激光关闭条件相比,可导致最小寿命增加10倍以上。与空心部位的几何形状相比,桥部位接触的近场俘获效率是空心部位几何形状的两倍,这可以归因于极化率的差异。当前的测量结果和尖端增强的拉曼光谱证实,在PBJ实验过程中,BDT的天然结构和接触几何形状得以保留。通过提供非侵入性途径来增加SM连接的短寿命,PBJ是ME的一种有价值的方法,为改善SM感应和识别平台铺平了道路。

更新日期:2021-04-21
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