Structure-activity relationships in gold nanoparticle dimers and trimers for surface-enhanced raman spectroscopy

Kristin L. Wustholz, Anne Isabelle Henry, Jeffrey M. McMahon, R. Griffith Freeman, Nicholas Valley, Marcelo E. Piotti, Michael J. Natan, George C. Schatz, Richard P.Van Duyne

Research output: Contribution to journalArticle

559 Citations (Scopus)

Abstract

Understanding the detailed relationship between nanoparticle structure and activity remains a significant challenge for the field of surface-enhanced Raman spectroscopy. To this end, the structural and optical properties of individual plasmonic nanoantennas comprised of Au nanoparticle assemblies that are coated with organic reporter molecules and encapsulated by a SiO2 shell have been determined using correlated transmission electron microscopy (TEM), dark-field Rayleigh scattering microscopy, surface-enhanced Raman scattering (SERS) microscopy, and finite element method (FEM) calculations. The distribution of SERS enhancement factors (EFs) for a structurally and optically diverse set of nanoantennas is remarkably narrow. For a collection of 30 individual nanoantennas ranging from dimers to heptamers, the EFs vary by less than 2 orders of magnitude. Furthermore, the EFs for the hot-spot-containing nanoparticles are uncorrelated to aggregation state and localized surface plasmon resonance (LSPR) wavelength but are crucially dependent on the size of the interparticle gap. This study demonstrates that the creation of hot spots, where two particles are in subnanometer proximity or have coalesced to form crevices, is paramount to achieving maximum SERS enhancements.

Original languageEnglish
Pages (from-to)10903-10910
Number of pages8
JournalJournal of the American Chemical Society
Volume132
Issue number31
DOIs
Publication statusPublished - Aug 11 2010

ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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    Wustholz, K. L., Henry, A. I., McMahon, J. M., Freeman, R. G., Valley, N., Piotti, M. E., Natan, M. J., Schatz, G. C., & Duyne, R. P. V. (2010). Structure-activity relationships in gold nanoparticle dimers and trimers for surface-enhanced raman spectroscopy. Journal of the American Chemical Society, 132(31), 10903-10910. https://doi.org/10.1021/ja104174m