论文标题
等离子体纳米颗粒中的热载体生成：原子结构的重要性
Hot-Carrier Generation in Plasmonic Nanoparticles: The Importance of Atomic Structure
论文作者
论文摘要
金属纳米颗粒对于等离子体增强的热载体具有吸引力，这可能在光化学反应中得到利用。在这项工作中，我们通过使用第一原理模拟来分析光子吸收，等离子体形成和随后的热载体生成的相干飞秒动力学。我们预测小型金属纳米颗粒中的能量和空间热载体分布，并表明热电子的分布对局部结构非常敏感。我们的结果表明，与大部分纳米颗粒相比，表面位点具有增强的热电子产生。尽管分布的细节取决于粒径和形状，但作为一般趋势低调的表面位点，例如角，边缘和{100}方面的热电子比例更高，比{111}方面或核心位置等高配位的表面位点。目前的结果表明，如何通过仔细设计纳米级系统中的原子尺度结构来量身定制热载体。
Metal nanoparticles are attractive for plasmon-enhanced generation of hot carriers, which may be harnessed in photochemical reactions. In this work, we analyze the coherent femtosecond dynamics of photon absorption, plasmon formation, and subsequent hot-carrier generation through plasmon dephasing using first-principles simulations. We predict the energetic and spatial hot-carrier distributions in small metal nanoparticles and show that the distribution of hot electrons is very sensitive to the local structure. Our results show that surface sites exhibit enhanced hot-electron generation in comparison to the bulk of the nanoparticle. While the details of the distribution depend on particle size and shape, as a general trend lower-coordinated surface sites such as corners, edges, and {100} facets exhibit a higher proportion of hot electrons than higher-coordinated surface sites such as {111} facets or the core sites. The present results thereby demonstrate how hot carriers could be tailored by careful design of atomic-scale structures in nanoscale systems.
