Nonlocal effects in plasmon-emitter interactions

Nonlocal and quantum mechanical phenomena in noble metal nanostructures become increasingly crucial when the relevant length scales in hybrid nanostructures reach the few-nanometer regime. In practice, such mesoscopic effects at metal–dielectric interfaces can be described using exemplary surface-response functions (SRFs) embodied by the Feibelman d-parameters. Here we show that SRFs dramatically influence quantum electrodynamic phenomena – such as the Purcell enhancement and Lamb shift – for quantum light emitters close to a diverse range of noble metal nanostructures interfacing different homogeneous media. Dielectric environments with higher permittivities are shown to increase the magnitude of SRFs calculated within the specular-reflection model. In parallel, the role of SRFs is enhanced in noble metal nanostructures characterized by large surface-to-volume ratios, such as thin planar metallic films or shells of core–shell nanoparticles, for which the spill-in of electron wave functions enhances plasmon hybridization. By investigating emitter quantum dynamics close to such plasmonic architectures, we show that decreasing the width of the metal region, or increasing the permittivity of the interfacing dielectric, leads to a significant change in the Purcell enhancement, Lamb shift, and visible far-field spontaneous emission spectrum, as an immediate consequence of SRFs. We anticipate that fitting the theoretically modelled spectra to experiments could allow for experimental determination of the d-parameters.