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Controlling Optically Driven Atomic Migration Using Crystal-Facet Control in Plasmonic Nanocavities.

Accepted version
Peer-reviewed

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Authors

Xomalis, Angelos 
Oksenberg, Eitan 
Shlesinger, Ilan 
Huang, Junyang 

Abstract

Plasmonic nanoconstructs are widely exploited to confine light for applications ranging from quantum emitters to medical imaging and biosensing. However, accessing extreme near-field confinement using the surfaces of metallic nanoparticles often induces permanent structural changes from light, even at low intensities. Here, we report a robust and simple technique to exploit crystal facets and their atomic boundaries to prevent the hopping of atoms along and between facet planes. Avoiding X-ray or electron microscopy techniques that perturb these atomic restructurings, we use elastic and inelastic light scattering to resolve the influence of crystal habit. A clear increase in stability is found for {100} facets with steep inter-facet angles, compared to multiple atomic steps and shallow facet curvature on spherical nanoparticles. Avoiding atomic hopping allows Raman scattering on molecules with low Raman cross-section while circumventing effects of charging and adatom binding, even over long measurement times. These nanoconstructs allow the optical probing of dynamic reconstruction in nanoscale surface science, photocatalysis, and molecular electronics.

Description

Keywords

SERS, atomic hopping, crystal facet, nano-optics, nanocavity, picocavity, single-molecule

Journal Title

ACS Nano

Conference Name

Journal ISSN

1936-0851
1936-086X

Volume Title

14

Publisher

American Chemical Society (ACS)

Rights

All rights reserved
Sponsorship
Engineering and Physical Sciences Research Council (EP/L015978/1)
Engineering and Physical Sciences Research Council (EP/L027151/1)
Engineering and Physical Sciences Research Council (EP/S022953/1)
Engineering and Physical Sciences Research Council (EP/P029426/1)
Engineering and Physical Sciences Research Council (EP/R020965/1)
European Commission Horizon 2020 (H2020) Future and Emerging Technologies (FET) (829067)
Engineering and Physical Sciences Research Council (EP/N016920/1)
European Commission Horizon 2020 (H2020) Research Infrastructures (RI) (861950)
Engineering and Physical Sciences Research Council (EP/G060649/1)
ERC
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