Non-equilibrium quantum plasmonics in nanoparticle-on-mirror nanocavities

TL;DR

This paper introduces a new ultrafast optical modulation method for quantum plasmonic phenomena in nanoparticle-on-mirror nanocavities, enabling control over plasmonic properties via laser-induced hot electrons without damaging the system.

Contribution

It presents a novel approach combining experimental techniques and microscopic modeling to achieve ultrafast, reversible control of quantum plasmonics in nanogaps, expanding active nanophotonics.

Findings

Successful numerical simulations supporting the model

Potential for ultrafast control in photochemistry and quantum emitters

No irreversible damage during modulation

Abstract

We develop a novel approach to ultrafast optical modulation of quantum-mechanical phenomena at the interface of plasmonic metals. Focusing on efficient and versatile nanoparticle-on-mirror plasmonic nanocavities, we discuss indirect control of plasmonic properties through laser-induced ballistic hot electron injection. Overcoming the limitations precluding the observations of laser-driven mesoscopic phenomena in the time domain with state-of-the-art amplified sources, our proposed experimental approach can be readily realized without irreversible optical damage and holds immense potential for the future development of ultrafast electrodynamics in nanogaps, applications in photochemistry and nanoscale control of quantum emitters. Agreeing with the results of numerical simulations, an intuitive microscopic model for the proposed time-dependent mesoscopic electrodynamics facilitates the analysis of the temperature-induced modulation of quantum plasmonic properties in a broad parameter space. Our work expands the realm of quantum nanophotonics onto non-equilibrium electronic systems and facilitates the development of ultrafast methods in active plasmonics.