Transport of plasmonic hot carriers published in Phys. Rev. Mater.


A. S. Jermyn, G. Tagliabue, H. A. Atwater, W. A. Goddard III, P. Narang and R. Sundararaman, “Transport of hot carriers in plasmonic nanostructures”, Phys. Rev. Mater. 3, 075201 (2019) (Preprint: arXiv:1707.07060)

Where do hot electrons and holes generated by plasmon decay in metallic nanostructures go? The precise evolution of carrier distributions in both space and energy critically determines their utility for hot carrier devices, because these carriers must be rapidly collected before they collide repeatedly with other electrons and approach equilibrium. However, this situation is a strong deviation from equilibrium that makes it a challenge to describe theoretically or simulate computationally.

Understanding and designing plasmonic hot carrier devices requires computational techniques to efficiently predict how electrons are distributed in space, time and energy. This work introduces a computational framework NESSE - nonequilibrium scattering in space and energy - that brings together two classic computational paradigms for transport phenomena: probabilistic approaches that work with continuous probability distribution functions, and stochastic approaches that work with individual discrete particles. Using NESSE, we predict spatially-resolved energy distributions from first principles and quantitatively establish the complex interplay between nanoscale geometry, electromagnetic field distributions and material electronic structure in determining useful plasmonic hot carrier distributions.