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Title

Atomic-scale lightning rod effect in plasmonic picocavities: A classical view to a quantum effect

AuthorsUrbieta, Mattin; Barbry, Marc; Zhang, Yao; Koval, P. CSIC ORCID; Sánchez-Portal, Daniel CSIC ORCID ; Zabala, Nerea CSIC ORCID; Aizpurua, Javier CSIC ORCID
KeywordsPicocavities
Nanoplasmonics
Ab initio calculations
Effective mode volume
Lightning rod effect
Issue Date2018
PublisherAmerican Chemical Society
CitationACS Nano 12(1): 585-595 (2018)
AbstractPlasmonic gaps are known to produce nanoscale localization and enhancement of optical fields, providing small effective mode volumes of about a few hundred nm. Atomistic quantum calculations based on time-dependent density functional theory reveal the effect of subnanometric localization of electromagnetic fields due to the presence of atomic-scale features at the interfaces of plasmonic gaps. Using a classical model, we explain this as a nonresonant lightning rod effect at the atomic scale that produces an extra enhancement over that of the plasmonic background. The near-field distribution of atomic-scale hot spots around atomic features is robust against dynamical screening and spill-out effects and follows the potential landscape determined by the electron density around the atomic sites. A detailed comparison of the field distribution around atomic hot spots from full quantum atomistic calculations and from the local classical approach considering the geometrical profile of the atoms' electronic density validates the use of a classical framework to determine the effective mode volume in these extreme subnanometric optical cavities. This finding is of practical importance for the community of surface-enhanced molecular spectroscopy and quantum nanophotonics, as it provides an adequate description of the local electromagnetic fields around atomic-scale features with use of simplified classical methods.
Publisher version (URL)https://doi.org/10.1021/acsnano.7b07401
URIhttp://hdl.handle.net/10261/177483
DOIhttp://dx.doi.org/10.1021/acsnano.7b07401
Identifiersdoi: 10.1021/acsnano.7b07401
e-issn: 1936-086X
issn: 1936-0851
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