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Visualization of Nanoplasmonic Coupling to Molecular Orbital in Light Emission Induced by Tunneling Electrons
Nano Letters ( IF 10.8 ) Pub Date : 2018-04-16 00:00:00 , DOI: 10.1021/acs.nanolett.8b00613
Arthur Yu 1 , Shaowei Li 1 , Hui Wang 1 , Siyu Chen 1 , Ruqian Wu 1 , W. Ho 1, 2
Affiliation  

The coupling between localized plasmon and molecular orbital in the light emission from a metallic nanocavity has been directly detected and imaged with sub-0.1 nm resolution. The light emission intensity was enhanced when the energy difference between the tunneling electrons and the lowest unoccupied molecular orbital (LUMO) of an azulene molecule matches the energy of a plasmon mode of the nanocavity defined by the Ag-tip and Ag (110) substrate of a scanning tunneling microscope (STM). The spatially resolved image of the light emission intensity matches the spatial distribution of the LUMO obtained by scanning tunneling spectroscopy (STS) and density functional theory (DFT) calculations. Our results highlight the near-field coupling of a molecular orbital to the radiative decay of a plasmonic excitation in a confined nanoscale junction.

中文翻译:

隧穿电子诱导的发光中的纳米等离子体耦合到分子轨道的可视化

从金属纳米腔发出的光中的局部等离子体激元和分子轨道之间的耦合已被直接检测到并以低于0.1 nm的分辨率成像。当隧穿电子与an烯分子的最低未占据分子轨道(LUMO)之间的能量差与纳米尖端的Ag-tip和Ag(110)衬底定义的纳米腔的等离振子模式的能量匹配时,发光强度增强。扫描隧道显微镜(STM)。发光强度的空间分辨图像与通过扫描隧道光谱(STS)和密度泛函理论(DFT)计算获得的LUMO的空间分布相匹配。我们的结果强调了在有限的纳米级结中分子轨道的近场耦合与等离子体激元的辐射衰减。
更新日期:2018-04-16
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