Correlating Nanoscopic Energy Transfer and Far-Field Emission to Unravel Lasing Dynamics in Plasmonic Nanocavity Arrays

Claire Deeb, Zhi Guo, Ankun Yang, Libai Huang, Teri W. Odom

Research output: Contribution to journalArticle

14 Citations (Scopus)

Abstract

Excited-state interactions between nanoscale cavities and photoactive molecules are critical in plasmonic nanolasing, although the underlying details are less-resolved. This paper reports direct visualization of the energy-transfer dynamics between two-dimensional arrays of plasmonic gold bowtie nanocavities and dye molecules. Transient absorption microscopy measurements of single bowties within the array surrounded by gain molecules showed fast excited-state quenching (2.6 ± 1 ps) characteristic of individual nanocavities. Upon optical pumping at powers above threshold, lasing action emerged depending on the spacing of the array. By correlating ultrafast microscopy and far-field light emission characteristics, we found that bowtie nanoparticles acted as isolated cavities when the diffractive modes of the array did not couple to the plasmonic gap mode. These results demonstrate how ultrafast microscopy can provide insight into energy relaxation pathways and, specifically, how nanocavities in arrays can show single-unit nanolaser properties.

Original languageEnglish
Pages (from-to)1454-1459
Number of pages6
JournalNano letters
Volume18
Issue number2
DOIs
Publication statusPublished - Feb 14 2018

Keywords

  • Localized surface plasmons
  • lattice plasmons
  • metal nanoparticle arrays
  • plasmon lasing
  • transient absorption microscopy

ASJC Scopus subject areas

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

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