This paper reports how the interfacial engineering of plasmonic nanoparticle (NP) lattices with desired surface characteristics can control plasmon-molecule interactions for tunable nanolasing thresholds. Compared to bare Cu NP lattices, graphene-coated Cu NPs surrounded by aromatic dye molecules gain support lasing with lower thresholds and at lower dye concentrations. This lasing enhancement is attributed to favorable molecular arrangements in electromagnetic hotspots through π–π interactions between graphene and IR-140 (5,50-dichloro-11-diphenylamine-3,30-diethyl-10,12-ethylene-thiatricarbocyanine-perchlorate) and 4-(dicyanomethylene)-2-methyl-6-(4-dimethyla-minostyryl)-4H-pyran (DCM) dyes. Besides the chemical interactions mediated by few-layer graphene, nanoscale dielectric layers such as fluoropolymer and alumina can also tailor the thresholds by modifying the spatial overlap of the dye near the NP surface. Our work lays the foundation for interfacial engineering of the surface of resonator units in plasmonic metasurfaces for exquisite control of light-matter interactions.
|Original language||English (US)|
|Journal||Proceedings of the National Academy of Sciences of the United States of America|
|State||Published - May 31 2022|
- Cu plasmonics
- core-shell nanoparticles
- light-matter interactions
ASJC Scopus subject areas