期刊
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
卷 112, 期 33, 页码 10292-10297出版社
NATL ACAD SCIENCES
DOI: 10.1073/pnas.1513058112
关键词
nanoparticle; noble metal; plasmonics; DNA; disorder
资金
- National Defense Science and Engineering Graduate (NDSEG) Fellowship Program
- Air Force Office of Scientific Research (AFOSR) Multidisciplinary University Research Initiative (MURI) [FA9550-11-1-0275]
- Northwestern Materials Research Center (MRSEC) under NSF [DMR-1121262]
- Office of the Provost
- Office for Research
- Northwestern University Information Technology
- Department of Energy [DE-AC02-06CH11357]
- MRSEC program [NSF DMR-1121262]
- International Institute for Nanotechnology (IIN)
- State of Illinois, through the IIN
Bottom-up assemblies of plasmonic nanoparticles exhibit unique optical effects such as tunable reflection, optical cavity modes, and tunable photonic resonances. Here, 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 (similar to 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. 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.
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