4.8 Article

Interfacial engineering of plasmonic nanoparticle metasurfaces

Publisher

NATL ACAD SCIENCES
DOI: 10.1073/pnas.2202621119

Keywords

nanolasing; light-matter interactions; Cu plasmonics; graphene; core-shell nanoparticles

Funding

  1. Vannevar Bush Faculty Fellowship from the US Department of Defense [DOD N00014-17-1-3023]
  2. Cottrell Fellowship from the Research Corporation for Science Advancement [27464]
  3. National Science Foundation [CHE-2039044]
  4. Department of Energy, Office of Basic Energy Sciences [DE-SC0004752]
  5. Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF) [ECCS-1542205]
  6. Materials Research Science and Engineering Center [DMR-1720139]
  7. State of Illinois
  8. Northwestern University
  9. SHyNE Resource
  10. Materials Research Science and Engineering Center program at the Materials Research Center [NSF DMR-1121262]
  11. International Institute for Nanotechnology (IIN)
  12. Keck Foundation
  13. State of Illinois through the IIN

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This study demonstrates how interfacial engineering of plasmonic nanoparticle lattices with specific surface characteristics can control plasmon-molecule interactions for tunable nanolasing thresholds. Graphene-coated copper nanoparticles surrounded by aromatic dye molecules exhibit lower lasing thresholds and can support lasing at lower concentrations compared to bare copper nanoparticles.
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 pi-pi 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-dimethylaminostyryl)-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.

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