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dc.contributor.authorMarchesin, Federico-
dc.contributor.authorKoval, P.-
dc.contributor.authorBarbry, Marc-
dc.contributor.authorAizpurua, Javier-
dc.contributor.authorSánchez-Portal, Daniel-
dc.identifierdoi: 10.1021/acsphotonics.5b00609-
dc.identifiere-issn: 2330-4022-
dc.identifier.citationACS Photonics 3(2): 269-277 (2016)-
dc.description.abstractThe correlation between transport properties across subnanometric metallic gaps and the optical response of the system is a complex effect that is determined by the fine atomic-scale details of the junction structure. As experimental advances are progressively accessing transport and optical characterization of smaller nanojunctions, a clear connection between the structural, electronic, and optical properties in these nanocavities is needed. Using ab initio calculations, we present here a study of the simultaneous evolution of the structure and the optical response of a plasmonic junction as the particles forming the cavity, two Na380 clusters, approach and retract. Atomic reorganizations are responsible for a large hysteresis of the plasmonic response of the system, which shows a jump-to-contact instability during the approach process and the formation of an atom-sized neck across the junction during retraction. Our calculations demonstrate that, due to the quantization of the conductance in metal nanocontacts, atomic-scale reconfigurations play a crucial role in determining the optical response of the whole system. We observe abrupt changes in the intensities and spectral positions of the dominating plasmon resonances and find a one-to-one correspondence between these jumps and those of the quantized transport as the neck cross-section diminishes. These results reveal an important connection between transport and optics at the atomic scale, which is at the frontier of current optoelectronics and can drive new options in optical engineering of signals driven by the motion and manipulation of single atoms.-
dc.description.sponsorshipWe acknowledge financial support from Projects FIS2013-41184-P and MAT2013-46593-C6-2-P from MINECO. M.B., P.K., F.M., and D.S.P. also acknowledge support from the ANR-ORGAVOLT project and the Euroregion Aquitaine-Euskadi program. M.B. acknowledges support from the Departamento de Educacion of the Basque Government through a Ph.D. grant. P.K. acknowledges financial support from the Fellows Gipuzkoa program of the Gipuzkoako Foru Aldundia through the FEDER funding scheme of the European Union. J.A. also acknowledges support from Grant 70NANB15H321, “PLASMOQUANTUM”, from the US Department of Commerce (NIST).-
dc.publisherAmerican Chemical Society-
dc.subjectQuantum transport-
dc.subjectTDDFT calculations-
dc.subjectOptical response-
dc.titlePlasmonic response of metallic nanojunctions driven by single atom motion: Quantum transport revealed in optics-
dc.description.versionPeer Reviewed-
dc.contributor.funderEurorregión Aquitania Euskadi-
dc.contributor.funderAgence Nationale de la Recherche (France)-
dc.contributor.funderMinisterio de Economía y Competitividad (España)-
dc.contributor.funderEusko Jaurlaritza-
dc.contributor.funderDiputación Foral de Guipúzcoa-
dc.contributor.funderEuropean Commission-
dc.contributor.funderDepartment of Commerce (US)-
dc.contributor.funderNational Institute of Standards and Technology (US)-
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