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Title: Defect tolerance and the effect of structural inhomogeneity in plasmonic DNA-nanoparticle superlattices

Bottom-up assemblies of plasmonic nanoparticles exhibit unique optical effects such as tunable reflection, optical cavity modes, and tunable photonic resonances. In this paper, we compare detailed simulations with experiment to explore the effect of structural inhomogeneity on the optical response in DNA-gold nanoparticle superlattices. In particular, we explore the effect of background environment, nanoparticle polydispersity (>10%), and variation in nanoparticle placement (~5%). At volume fractions less than 20% Au, the optical response is insensitive to particle size, defects, and inhomogeneity in the superlattice. At elevated volume fractions (20% and 25%), structures incorporating different sized nanoparticles (10-, 20-, and 40-nm diameter) each exhibit distinct far-field extinction and near-field properties. These optical properties are most pronounced in lattices with larger particles, which at fixed volume fraction have greater plasmonic coupling than those with smaller particles. Moreover, the incorporation of experimentally informed inhomogeneity leads to variation in far-field extinction and inconsistent electric-field intensities throughout the lattice, demonstrating that volume fraction is not sufficient to describe the optical properties of such structures. Finally, these data have important implications for understanding the role of particle and lattice inhomogeneity in determining the properties of plasmonic nanoparticle lattices with deliberately designed optical properties.
Authors:
 [1] ;  [2] ;  [1] ;  [3] ;  [1]
  1. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. International Inst. for Nanotechnology
  2. Northwestern Univ., Evanston, IL (United States). International Inst. for Nanotechnology. Dept. of Materials Science and Engineering
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry. International Inst. for Nanotechnology. Dept. of Materials Science and Engineering
Publication Date:
OSTI Identifier:
1235110
Grant/Contract Number:
AC02-06CH11357; FA9550-11-1-0275; 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: 112; Journal Issue: 33; 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; National Defense Science and Engineering Graduate (NDSEG) Fellowship Program (United States); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
Country of Publication:
United States
Language:
ENGLISH
Subject:
60 APPLIED LIFE SCIENCES; 59 BASIC BIOLOGICAL SCIENCES; 36 MATERIALS SCIENCE; nanoparticle; noble metal; plasmonics; DNA; disorder