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扫描隧道显微镜诱导单分子发光热荧光现象的全量子理论
陈功,李晓光*,董振超*
作者单位E-mail
陈功 中国科学技术大学合肥微尺度物质科学国家实验室(筹)国际功能材料量子设计中心合肥230026  
李晓光* 中国科学技术大学合肥微尺度物质科学国家实验室(筹)国际功能材料量子设计中心合肥230026中国科学院深圳先进技术研究院深圳518055 lixg@siat.ac.cn 
董振超* 中国科学技术大学合肥微尺度物质科学国家实验室(筹)国际功能材料量子设计中心合肥230026 zcdong@ustc.edu.cn 
摘要:
使用量子主方程方法从理论上研究了STM诱导分子电致发光现象,并特别考虑了分子和量子化等离激元相互作用对于单分子光学性质的影响. 分子-等离激元相互作用大大增加了分子的自发辐射速率和分子发光的的强度,而且当分子自发辐射速率和振动弛豫速率可比拟的时候,将会出现热荧光现象.
关键词:  扫描隧道显微镜诱导发光,热荧光,表面等离激元,量子主方程
DOI:10.1063/1674-0068/28/cjcp1505106
分类号:
基金项目:
Full Quantum Theory of Molecular Hot-Electroluminescence in Scanning Tunneling Microscope Tunnel Junctions
Gong Chen,Xiao-guang Li*,Zhen-chao Dong*
Abstract:
The pursuit of nanoscale photonics and molecular optoelectronics has stimulated a lot of interests in scanning tunneling microscope (STM) induced molecular emission. In this work, we have introduced a full quantum mechanical approach instead of the previous semiclassical theory to consider the quantized surface plasmon modes in this system. By considering the mutual interactions between a single molecule and the quantized surface plasmon, we have studied the molecular electroluminescence from STM tunnel junctions. Due to the coupling to the surface plasmons, the spontaneous emission rate and the fluorescence intensity of the molecule are both enormously enhanced. In particular, we show that when the radiative decay rate becomes comparable to the vibrational damping rate, hot-electroluminescence can be observed. All these findings are believed to be instructive for further developments of both molecular electronics and photonics.
Key words:  Scanning tunneling microscope induced luminescence, Master equation, Surface plasmon, Hot-electroluminescence