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

Abstract

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:

Ross, Michael B. ^[1]; Ku, Jessie C. ^[2]; Blaber, Martin G. ^[1]; Mirkin, Chad A. ^[3]; Schatz, George C. ^[1]

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+ Show Author Affiliations

1. Department of Chemistry, Northwestern University, Evanston, IL 60208,, International Institute for Nanotechnology, Northwestern University, Evanston, IL 60208,
2. International Institute for Nanotechnology, Northwestern University, Evanston, IL 60208,, Department of Materials Science and Engineering, Northwestern University, Evanston, IL 60208
3. Department of Chemistry, Northwestern University, Evanston, IL 60208,, International Institute for Nanotechnology, Northwestern University, Evanston, IL 60208,, Department of Materials Science and Engineering, Northwestern University, Evanston, IL 60208

Publication Date:

Mon Aug 03 00:00:00 EDT 2015

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)

OSTI Identifier:

1235110

Alternate Identifier(s):

OSTI ID: 1222013

Grant/Contract Number:  

AC02-06CH11357; FA9550-11-1-0275; 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: 112 Journal Issue: 33; Journal ID: ISSN 0027-8424

Publisher:

Proceedings of the National Academy of Sciences

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