Plasmon-Induced Hot Carriers in Metallic Nanoparticles

摘要

Plasmon-induced hot carrier formation is attracting an increasing research interest due to its potential for applications in photocatalysis, photodetection and solar energy harvesting. However, despite very significant experimental effort, a comprehensive theoretical description of the hot carrier generation process is still missing. In this work we develop a theoretical model for the plasmon-induced hot carrier process and apply it to spherical silver nanoparticles and nanoshells. In this model, the conduction electrons of the metal are described as free particles in a finite spherical potential well, and the plasmon-induced hot carrier production is calculated using Fermi's golden rule. We show that the inclusion of many-body interactions has only a minor influence on the results. Using the model we calculate the rate of hot carrier generation, finding that it closely follows the spectral profile of the plasmon. Our analysis reveals that particle size and hot carrier lifetime play a central role in determining both the production rate and the energy distribution of the hot carriers. Specifically, larger nanoparticle sizes and shorter lifetimes result in higher carrier production rates but smaller energies, and vice versa. We characterize the efficiency of the hot carrier generation process by introducing a figure of merit that measures the number of high energy carriers generated per plasmon. Furthermore, we analyze the spatial distribution and directionality of these excitations. The results presented here contribute to the basic understanding of plasmon-induced hot carrier generation and provide insight for optimization of the process.