Plasmonic Hot Carriers-Controlled Second Harmonic Generation in WSe2 Bilayers

被引:78
作者
Wen, Xinglin [1 ]
Xu, Weigao [1 ]
Zhao, Weijie [1 ]
Khurgin, Jacob B. [2 ]
Xiong, Qihua [1 ,3 ]
机构
[1] Nanyang Technol Univ, Sch Phys & Math Sci, Div Phys & Appl Phys, Singapore 637371, Singapore
[2] Johns Hopkins Univ, Dept Elect & Comp Engn, Baltimore, MD 21218 USA
[3] Nanyang Technol Univ, Sch Elect & Elect Engn, Nanoelect Ctr Excellence, NOVITAS, Singapore 639798, Singapore
基金
新加坡国家研究基金会;
关键词
Plasmonic hot carrier injection; bilayer transitional metal dichalcogenides; inversion symmetry; charge induced second harmonic generation; transient absorption spectroscopy; RAMAN-SCATTERING; NONLINEAR OPTICS; ELECTRON; NANOANTENNAS; INTERFACES; MONOLAYER; RESONANCE; MOS2; SPECTROSCOPY; ENHANCEMENT;
D O I
10.1021/acs.nanolett.7b04707
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Modulating second harmonic generation (SHG) by a static electric field through either electric-field-induced SHG or charge-induced SHG has been well documented. Nonetheless, it is essential to develop the ability to dynamically control and manipulate the nonlinear properties, preferably at high speed. Plasmonic hot carriers can be resonantly excited in metal nanoparticles and then injected into semiconductors within 10-100 fs, where they eventually decay on a comparable time scale. This allows one to rapidly manipulate all kinds of characteristics of semiconductors, including their nonlinear properties. Here we demonstrate that plasmonically generated hot electrons can be injected from plasmonic nanostructure into bilayer (2L) tungsten diselenide (WSe2), breaking the material inversion symmetry and thus inducing an SHG. With a set of pump-probe experiments we confirm that it is the dynamic separation electric field resulting from the hot carrier injection (rather than a simple optical field enhancement) that is the cause of SHG. Transient absorption measurement further substantiate the plasmonic hot electrons injection and allow us to measure a rise time of similar to 120 fs and a fall time of 1.9 ps. Our study creates opportunity for the ultrafast all-optical control of SHG in an all-optical manner that may enable a variety of applications.
引用
收藏
页码:1686 / 1692
页数:7
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