Giant mid-IR resonant coupling to molecular vibrations in sub-nm gaps of plasmonic multilayer metafilms


Type
Article
Change log
Authors
Benjamin-Grys, David 
Abstract

Nanomaterials capable of confining light are desirable for enhancing spectroscopies such as Raman scattering, infrared absorption, and nonlinear optical processes. Plasmonic superlattices have shown the ability to host collective resonances in the mid-infrared, but require stringent fabrication processes to create well-ordered structures. Here, we demonstrate how short-range-ordered Au nanoparticle multilayers on a mirror, self-assembled by a sub-nm molecular spacer, support collective plasmon-polariton resonances in the visible and infrared, continuously tunable beyond 11 μm by simply varying the nanoparticle size and number of layers. The resulting molecule-plasmon system approaches vibrational strong coupling, and displays giant Fano dip strengths, SEIRA enhancement factors ~106, light-matter coupling strengths g~100 cm−1, Purcell factors ~106, and mode volume compression factors ~108. The collective plasmon-polariton mode is highly robust to nanoparticle vacancy disorder and is sustained by the consistent gap size defined by the molecular spacer. Structural disorder efficiently couples light into the gaps between the multilayers and mirror, enabling Raman and infrared sensing of sub-picolitre sample volumes.

Description
Keywords
cond-mat.mes-hall, physics.optics, physics.optics
Journal Title
Light: Science and Applications
Conference Name
Journal ISSN
2047-7538
2047-7538
Volume Title
Publisher
Springer Nature [academic journals on nature.com]
Sponsorship
Engineering and Physical Sciences Research Council (EP/L027151/1)
Engineering and Physical Sciences Research Council (EP/L015978/1)
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/S022953/1)
European Commission Horizon 2020 (H2020) Research Infrastructures (RI) (861950)
European Commission Horizon 2020 (H2020) ERC (883703)
Engineering and Physical Sciences Research Council (EP/P024947/1)
Engineering and Physical Sciences Research Council (EP/S019367/1)
Engineering and Physical Sciences Research Council (EP/R00661X/1)