Madelung Formalism for Electron Spill-Out in Nonlocal Nanoplasmonics

J Phys Chem C Nanomater Interfaces. 2022 Sep 1;126(34):14758-14765. doi: 10.1021/acs.jpcc.2c04828. Epub 2022 Aug 19.

Abstract

Current multiscale plasmonic systems pose a modeling challenge. Classical macroscopic theories fail to capture quantum effects in such systems, whereas quantum electrodynamics is impractical given the total size of the experimentally relevant systems, as the number of interactions is too large to be addressed one by one. To tackle the challenge, in this paper we propose to use the Madelung form of the hydrodynamic Drude model, in which the quantum effect electron spill-out is incorporated by describing the metal-dielectric interface using a super-Gaussian function. The results for a two-dimensional nanoplasmonic wedge are correlated to those from nonlocal full-wave numerical calculations based on a linearized hydrodynamic Drude model commonly employed in the literature, showing good qualitative agreement. Additionally, a conformal transformation perspective is provided to explain qualitatively the findings. The methodology described here may be applied to understand, both numerically and theoretically, the modular inclusions of additional quantum effects, such as electron spill-out and nonlocality, that cannot be incorporated seamlessly by using other approaches.