发表机构
Beijing Computational Science Research Center; Nankai University; Donostia International Physics Center; Imperial College London（北京计算科学研究中心; 南开大学; 多诺西亚国际物理中心; 伦敦帝国理工学院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本文通过原子级模拟揭示等离激元催化中热载流子的量子化分布随纳米颗粒尺寸减小而增强，提升氧的振动激发与解离效率，为选择性控制和非热能量转换提供新途径。
AI 中文摘要
金属纳米颗粒上吸附分子的振动激活是等离激元催化的一个基本步骤，然而在量子体系中由热载流子驱动的潜在动力学尚未被完全理解。利用等离激元热载流子产生的原子级描述，我们研究了银纳米颗粒上氧的振动激发和解离随直径D的变化。当D从经典尺度减小到量子尺度时，热载流子的量子化分布出现，且高能区域的布居数增加。这些高能热载流子提供更有效的振动耦合和解离。振动激发速率表现出线性的1/D标度关系，这源于朗道阻尼。在增强的光照强度下，由于多次电子散射产生的振动加热，该速率变为非线性。等离激元催化中热载流子量子化分布的发现为选择性控制和非热能量转换开辟了新途径。
英文摘要
Vibrational activation of admolecules on metal nanoparticles is an elementary step in plasmonic catalysis, yet the underlying dynamics driven by hot carriers is not fully understood in the quantum regime. Using an atomistic description of plasmonic hot carrier generation, we investigate vibrational excitation and dissociation of oxygen on silver nanoparticles as a function of diameter D. As D reduces from the classical to quantum-sized regime, quantized distribution of hot carriers emerges with increasing population in the high-energy regions. These highly energetic hot carriers deliver more efficient vibrational coupling and dissociation. The rate of vibrational excitation shows a linear 1/D scaling, which results from Landau damping. It turns nonlinear at elevated light intensities due to vibrational heating generated by multiple electron scattering. The finding of quantized distribution of hot carrier in plasmonic catalysis opens new avenues for selective control and nonthermal energy conversion.
