Directional emission from dye-functionalized plasmonic DNA superlattice microcavities

Daniel J. Park, Jessie C. Ku, Lin Sun, Clotilde M. Lethiec, Nathaniel P. Stern, George C Schatz, Chad A. Mirkin

Research output: Contribution to journalArticle

15 Citations (Scopus)

Abstract

Three-dimensional plasmonic superlattice microcavities, made from programmable atom equivalents comprising gold nanoparticles functionalized with DNA, are used as a testbed to study directional light emission. DNA-guided nanoparticle colloidal crystallization allows for the formation of micrometer-scale single-crystal bodycentered cubic gold nanoparticle superlattices, with dye molecules coupled to the DNA strands that link the particles together, in the form of a rhombic dodecahedron. Encapsulation in silica allows one to create robust architectures with the plasmonically active particles and dye molecules fixed in space. At the micrometer scale, the anisotropic rhombic dodecahedron crystal habit couples with photonic modes to give directional light emission. At the nanoscale, the interaction between the dye dipoles and surface plasmons can be finely tuned by coupling the dye molecules to specific sites of the DNA particle-linker strands, thereby modulating dye-nanoparticle distance (three different positions are studied). The ability to control dye position with subnanometer precision allows one to systematically tune plasmon-excition interaction strength and decay lifetime, the results of which have been supported by electrodynamics calculations that span length scales from nanometers to micrometers. The unique ability to control surface plasmon/ exciton interactions within such superlattice microcavities will catalyze studies involving quantum optics, plasmon laser physics, strong coupling, and nonlinear phenomena.

Original languageEnglish
Pages (from-to)457-461
Number of pages5
JournalProceedings of the National Academy of Sciences of the United States of America
Volume114
Issue number3
DOIs
Publication statusPublished - Jan 17 2017

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Keywords

  • Anisotropic 3Dmicrocavity
  • Directional emission
  • DNA programmable assembly
  • Fluorescence enhancement
  • Nanoparticle surface plasmon

ASJC Scopus subject areas

  • General

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