Real-Time Formulation of Atomistic Electromagnetic Models for Plasmonics

TL;DR

This paper introduces a real-time, atomistic modeling approach for nanoplasmonics that captures quantum size effects, tunneling, and decoherence in metal nanostructures, enabling dynamic optical property analysis.

Contribution

It extends existing atomistic methods to real-time simulations, allowing dynamic study of plasmonic phenomena with quantum effects included.

Findings

Successfully reproduces quantum size effects in metal nanoparticles.

Effectively describes optical responses of subnanometer junctions.

Provides an efficient framework for time-dependent plasmonic studies.

Abstract

Investigating nanoplasmonics using time-dependent approaches permits shedding light on the dynamic optical properties of plasmonic structures, which are intrinsically connected with their potential applications in photochemistry and photoreactivity. This work proposes a real-time extension of our recently developed fully atomistic approaches $\omega$FQ and $\omega$FQF$\mu$. These methods successfully reproduce quantum size effects in metal nanoparticles, including plasmon shifts for both simple and $d$-metals, even below the quantum size limit. Also, thanks to their atomistic nature and the phenomenological inclusion of quantum tunneling effects, they can effectively describe the optical response of subnanometer junctions. By incorporating real-time dynamics, the approach provides an efficient framework for studying the time-dependent optical behavior of metal nanostructures, including the decoherence of plasmon excitations.