Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 114, Issue 3, Pages 457-461Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1619802114
Keywords
DNA programmable assembly; directional emission; anisotropic 3Dmicrocavity; nanoparticle surface plasmon; fluorescence enhancement
Categories
Funding
- Air Force Office of Scientific Research Award [FA9550-12-1-0280]
- Asian Office of Aerospace Research and Development Award [FA2386-13-1-4124]
- Non-equilibrium Energy Research Center
- Center for Bio-Inspired Energy Science, Energy Frontier Research Centers - US Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences [DE-SC0000989, DE-SC0000989-0002]
- National Science Foundation (NSF) [CHE-1465045]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource [NSF NNCI-1542205]
- Materials Research Science and Engineering Center program at the Materials Research Center [NSF DMR-1121262]
- International Institute for Nanotechnology (IIN)
- Keck Foundation
- State of Illinois, through the IIN
- DOE [DE-AC02-06CH11357]
- Department of Defense
- IIN
- Direct For Mathematical & Physical Scien
- Division Of Chemistry [1465045] Funding Source: National Science Foundation
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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 body-centered 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.
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