Dielectric engineering of hot carrier generation by quantized plasmons in embedded silver nanoparticles

TL;DR

This paper presents a quantum-mechanical approach to engineer hot-carrier generation in silver nanoparticles by embedding them in dielectric materials, enabling control over carrier energy and quantity for improved photovoltaic and photocatalytic applications.

Contribution

It introduces a method to optimize hot-carrier generation rates through dielectric environment engineering, accounting for both external and internal screening effects.

Findings

Maximized hot-carrier generation when plasmon energy matches the joint density of states.

Embedding in strongly screening environments produces many low-energy carriers.

The approach enables tailored hot-carrier properties for device applications.

Abstract

Understanding and controlling properties of plasmon-induced hot carriers is a key step towards next-generation photovoltaic and photocatalytic devices. Here, we uncover a route to engineering hot-carrier generation rates of silver nanoparticles by designed embedding in dielectric host materials. Extending our recently established quantum-mechanical approach to describe the decay of quantized plasmons into hot carriers we capture both external screening by the nanoparticle environment and internal screening by silver d-electrons through an effective electron-electron interaction. We find that hot-carrier generation can be maximized by engineering the dielectric host material such that the energy of the localized surface plasmon coincides with the highest value of the nanoparticle joint density of states. This allows us to uncover a path to control the energy of the carriers and the amount produced, for example a large number of relatively low-energy carriers are obtained by embedding in strongly screening environments.