Abstract
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 indifferent 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.
Highlights
Surface plasmon has recently emerged as a route for driving chemical reactions using hot carrier generation, local heating effects, and optical near-field enhancement [1, 2]
A large difference of 12.75% in the hot electron (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
The chiral response of the L-shaped chiral nanostructures (LCNs) can be tuned by changing the aspect ratio between its long arm (L1) and short arm (L2), which is attributed to the breaking of different LCN
Summary
Surface plasmon has recently emerged as a route for driving chemical reactions using hot carrier generation, local heating effects, and optical near-field enhancement [1, 2]. Accurate measurement of the HE generation rate and the surface temperature at reaction regions remain exceptionally difficulty tasks for current techniques. Quantification of these two effects is paramount for designing catalysts and optimizing plasmonic platforms. An understanding of chiral responses between different regions on one nanostructure, which plays a key role in enantioselective catalysis, has been lacking [11, 12]. For these reasons, it is necessary to locally control HE and thermal effects in plasmonic photochemistry reactions. The local controllability of HE and thermal effects on the micro- or nano-scale plays a key role in high-resolution single-molecule photochemical reactions
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