Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles

Sushmita Biswas, Xiaoying Liu, Jeremy W. Jarrett, Dean Brown, Vitaliy Pustovit, Augustine Urbas, Kenneth L. Knappenberger, Paul F. Nealey, Richard A. Vaia

Research output: Contribution to journalArticlepeer-review

51 Scopus citations


Metal nanoparticle assemblies are promising materials for nanophotonic applications due to novel linear and nonlinear optical properties arising from their plasmon modes. However, scalable fabrication approaches that provide both precision nano- and macroarchitectures, and performance commensurate with design and model predictions, have been limiting. Herein, we demonstrate controlled and efficient nanofocusing of the fundamental and second harmonic frequencies of incident linearly and circularly polarized light using reduced symmetry gold nanoparticle dimers formed by surface-directed assembly of colloidal nanoparticles. Large ordered arrays (>100) of these C∞v heterodimers (ratio of radii R1/R2 = 150 nm/50 nm = 3; gap distance l = 1 ± 0.5 nm) exhibit second harmonic generation and structure-dependent chiro-optic activity with the circular dichroism ratio of individual heterodimers varying less than 20% across the array, demonstrating precision and uniformity at a large scale. These nonlinear optical properties were mediated by interparticle plasmon coupling. Additionally, the versatility of the fabrication is demonstrated on a variety of substrates including flexible polymers. Numerical simulations guide architecture design as well as validating the experimental results, thus confirming the ability to optimize second harmonic yield and induce chiro-optical responses for compact sensors, optical modulators, and tunable light sources by rational design and fabrication of the nanostructures.

Original languageEnglish (US)
Pages (from-to)1836-1842
Number of pages7
JournalNano letters
Issue number3
StatePublished - Mar 11 2015

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • General Chemistry
  • General Materials Science
  • Condensed Matter Physics
  • Mechanical Engineering


Dive into the research topics of 'Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles'. Together they form a unique fingerprint.

Cite this