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

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:
 [1] ;  [2] ;  [2] ;  [3] ;  [4] ;  [1] ;  [5]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry and International Inst. for Nanotechnology (IIN)
  2. Northwestern Univ., Evanston, IL (United States). International Inst. for Nanotechnology (IIN) and Dept. of Materials Science and Engineering
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  4. Northwestern Univ., Evanston, IL (United States). Dept. of Physics and Astronomy
  5. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry, Dept. of Materials Science and Engineering and International Inst. for Nanotechnology (IIN)
Publication Date:
Grant/Contract Number:
SC0000989; AC02-06CH11357; FA9550-12-1-0280; FA2386-13-1-4124; SC0000989-0002; CHE-1465045; NNCI-1542205; DMR-1121262
Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Volume: 114; Journal Issue: 3; Journal ID: ISSN 0027-8424
Publisher:
National Academy of Sciences, Washington, DC (United States)
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
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
OSTI Identifier:
1338230
Alternate Identifier(s):
OSTI ID: 1418600

Park, Daniel J., Ku, Jessie C., Sun, Lin, Lethiec, Clotilde M., Stern, Nathaniel P., Schatz, George C., and Mirkin, Chad A.. Directional emission from dye-functionalized plasmonic DNA superlattice microcavities. United States: N. p., Web. doi:10.1073/pnas.1619802114.
Park, Daniel J., Ku, Jessie C., Sun, Lin, Lethiec, Clotilde M., Stern, Nathaniel P., Schatz, George C., & Mirkin, Chad A.. Directional emission from dye-functionalized plasmonic DNA superlattice microcavities. United States. doi:10.1073/pnas.1619802114.
Park, Daniel J., Ku, Jessie C., Sun, Lin, Lethiec, Clotilde M., Stern, Nathaniel P., Schatz, George C., and Mirkin, Chad A.. 2017. "Directional emission from dye-functionalized plasmonic DNA superlattice microcavities". United States. doi:10.1073/pnas.1619802114.
@article{osti_1338230,
title = {Directional emission from dye-functionalized plasmonic DNA superlattice microcavities},
author = {Park, Daniel J. and Ku, Jessie C. and Sun, Lin and Lethiec, Clotilde M. and Stern, Nathaniel P. and Schatz, George C. and Mirkin, Chad A.},
abstractNote = {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, and nonlinear phenomena.},
doi = {10.1073/pnas.1619802114},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 3,
volume = 114,
place = {United States},
year = {2017},
month = {1}
}

Works referenced in this record:

DNA-nanoparticle superlattices formed from anisotropic building blocks
journal, October 2010
  • Jones, Matthew R.; Macfarlane, Robert J.; Lee, Byeongdu
  • Nature Materials, Vol. 9, Issue 11, p. 913-917
  • DOI: 10.1038/nmat2870

Nanoparticle Superlattice Engineering with DNA
journal, October 2011

Optical Constants of the Noble Metals
journal, December 1972