Title: Directional emission from dye-functionalized plasmonic DNA superlattice microcavities

Abstract

Three-dimensional plasmonic superlattice microcavities, made from programmable atom equivalents comprising gold nanoparticles functionalized with DNA, are used here 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–nanopar-ticle 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 de-cay lifetime, the results of which have been supported by electro-dynamics calculations that span length scales from nanometers to micrometers. The unique ability to control surface plasmon/exciton interactions within such superlattice microcavities will cat-alyze studies involving quantum optics, plasmon laser physics, strong coupling,more » and nonlinear phenomena.« less

Authors:

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

Publication Date:

2017-01-04

Research Org.:

Northwestern Univ., Evanston, IL (United States)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); USDOD; US Air Force Office of Scientific Research (AFOSR); Asian Office of Aerospace Research and Development (AOARD); National Science Foundation (NSF); Keck Foundation; Alfred P. Sloan Foundation

OSTI Identifier:

1338230

Alternate Identifier(s):

OSTI ID: 1418600

Grant/Contract Number:  

SC0000989; AC02-06CH11357; FA9550-12-1-0280; FA2386-13-1-4124; SC0000989-0002; CHE-1465045; NNCI-1542205; DMR-1121262

Resource Type:

Published Article

Journal Name:

Proceedings of the National Academy of Sciences of the United States of America

Additional Journal Information:

Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 114 Journal Issue: 3; Journal ID: ISSN 0027-8424

Publisher:

National Academy of Sciences, Washington, DC (United States)

Country of Publication:

United States

Language:

English

Subject:

77 NANOSCIENCE AND NANOTECHNOLOGY; 59 BASIC BIOLOGICAL SCIENCES; 36 MATERIALS SCIENCE; DNA programmable assembly; directional emission; anisotropic 3D microcavity; nanoparticle; surface plasmon; fluorescence enhancement