Kang Bowen, Zhang Tingting, Yan Lei, Gou Chengxiang, Jiang Zihe, Ji Min, Chen Li, Zhang Zhenglong, Zheng Hairong, Xu Hongxing
School of Physics and Information Technology, Shaanxi Normal University, Xi'an, 710062, China.
Department of Electrical and Computer Engineering, University of California San Diego, La Jolla, California, USA.
Nanophotonics. 2022 Feb 16;11(6):1195-1202. doi: 10.1515/nanoph-2021-0780. eCollection 2022 Feb.
The control of hot electron (HE) and thermal effects induced by plasmonic nanostructures has recently attracted considerable attention. When illuminated by light with different circular polarization states, the circular dichroism signal of molecules adsorbed by plasmonic chiral nanostructures can control HE and thermal effects. These effects have the potential to enhance reaction rates and to change selectivity patterns in photothermal catalysis. Here, we propose an aluminum L-shaped chiral nanostructure system in which HE and thermal effects can be controlled in different regions of the nanostructure by changing the chirality of the excitation light. A large difference of 12.75% in the HE effect but a virtually identical thermal effect can be achieved in different regions of the nanostructure by selecting the appropriate probed region, while a large thermal effect difference of 65.67% but a virtually identical HE effect can be achieved in one region of the nanostructure by changing the polarization state of the excitation light. In addition, the HE and thermal chiral selectivity effects of double L-shaped nanostructures are investigated as these structures can be more easily controlled during asymmetric chiral growth and crystallization. This work combined with plasmonic chirality is beneficial for quantifying HE and thermal effects in photochemical reactions and provides theoretical support for designing catalysts and optimizing plasmonic platforms. Additionally, the local controllability of HE and thermal effects plays an essential role in high-resolution photochemical reactions, especially in single-molecule photochemical reactions.
等离子体纳米结构所引发的热电子(HE)及热效应的控制近来备受关注。当用不同圆偏振态的光照射时,被等离子体手性纳米结构吸附的分子的圆二色性信号能够控制热电子及热效应。这些效应有潜力提高反应速率并改变光热催化中的选择性模式。在此,我们提出一种铝制L形手性纳米结构系统,在该系统中,通过改变激发光的手性,可在纳米结构的不同区域控制热电子及热效应。通过选择合适的探测区域,在纳米结构的不同区域可实现热电子效应12.75%的显著差异,而热效应几乎相同;同时,通过改变激发光的偏振态,在纳米结构的一个区域可实现65.67%的大热效应差异,而热电子效应几乎相同。此外,还研究了双L形纳米结构的热电子和热手性选择性效应,因为这些结构在不对称手性生长和结晶过程中更容易控制。这项结合了等离子体手性的工作有利于量化光化学反应中的热电子和热效应,并为设计催化剂和优化等离子体平台提供理论支持。此外,热电子和热效应的局部可控性在高分辨率光化学反应中,尤其是在单分子光化学反应中起着至关重要的作用。