Ab initio nanoplasmonics: The impact of atomic structure

Under the terms of the Creative Commons Attribution License 3.0 (CC-BY).We present an ab initio study of the hybridization of localized surface plasmons in a metal nanoparticle dimer. The atomic structure, which is often neglected in theoretical studies of quantum nanoplasmonics, has a strong impact on the optical absorption properties when subnanometric gaps between the nanoparticles are considered. We demonstrate that this influences the hybridization of optical resonances of the dimer, and leads to significantly smaller electric field enhancements as compared to the standard jellium model. In addition, we show that the corrugation of the metal surface at a microscopic scale becomes as important as other well-known quantum corrections to the plasmonic response, implying that the atomic structure has to be taken into account to obtain quantitative predictions for realistic nanoplasmonic devices.This work has been funded by the European Research Council (ERC-2011-AdG Proposal No. 290981). We also acknowledge financial support from the European Research Council (ERC-2010-AdG Proposal No. 267374), Spanish Grants (No. MAT2011-28581-C02-01 and No. FIS2010-21282-C02), Grupos Consolidados UPV/EHU (IT-578-13), COST actions CM1204, MP1306, and EC project CRONOS (Grant No. 280879-2).Peer Reviewe