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Controlling Plasmonic Catalysis via Strong Coupling with Electromagnetic Resonators
Nano Letters ( IF 9.6 ) Pub Date : 2024-09-12 , DOI: 10.1021/acs.nanolett.4c03153
Jakub Fojt 1 , Paul Erhart 1 , Christian Schäfer 1
Affiliation  

Plasmonic excitations decay within femtoseconds, leaving nonthermal (often referred to as “hot”) charge carriers behind that can be injected into molecular structures to trigger chemical reactions that are otherwise out of reach─a process known as plasmonic catalysis. In this Letter, we demonstrate that strong coupling between resonator structures and plasmonic nanoparticles can be used to control the spectral overlap between the plasmonic excitation energy and the charge injection energy into nearby molecules. Our atomistic description couples real-time density-functional theory self-consistently to an electromagnetic resonator structure via the radiation-reaction potential. Control over the resonator provides then an additional knob for nonintrusively enhancing plasmonic catalysis, here more than 6-fold, and dynamically reacting to deterioration of the catalyst─a new facet of modern catalysis.

中文翻译:


通过电磁谐振器的强耦合控制等离激元催化



等离激元激发在飞秒内衰减,留下非热(通常称为“热”)电荷载流子,可以将其注入分子结构中,以触发原本无法达到的化学反应,这一过程称为等离激元催化。在这封信中,我们证明了谐振器结构和等离子体纳米颗粒之间的强耦合可用于控制等离子体激发能量和附近分子的电荷注入能量之间的光谱重叠。我们的原子描述通过辐射反应势将实时密度泛函理论自洽地耦合到电磁谐振器结构。对谐振器的控制为非侵入式增强等离子体催化提供了一个额外的旋钮,此处增强了 6 倍以上,并对催化剂的劣化做出动态反应——这是现代催化的一个新方面。
更新日期:2024-09-12
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