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 journalArticle

40 Citations (Scopus)

Abstract

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
Volume15
Issue number3
DOIs
StatePublished - Mar 11 2015

Fingerprint

Gold
Amplification
assembly
gold
Nanoparticles
Fabrication
nanoparticles
fabrication
Optical properties
harmonics
Nanophotonics
optical properties
Metal nanoparticles
Light modulators
Dichroism
optical measuring instruments
Light polarization
versatility
Harmonic generation
Dimers

All Science Journal Classification (ASJC) codes

  • Bioengineering
  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics
  • Mechanical Engineering

Cite this

Biswas, S., Liu, X., Jarrett, J. W., Brown, D., Pustovit, V., Urbas, A., ... Vaia, R. A. (2015). Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles. Nano letters, 15(3), 1836-1842. https://doi.org/10.1021/nl504613q
Biswas, Sushmita ; Liu, Xiaoying ; Jarrett, Jeremy W. ; Brown, Dean ; Pustovit, Vitaliy ; Urbas, Augustine ; Knappenberger, Kenneth L. ; Nealey, Paul F. ; Vaia, Richard A. / Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles. In: Nano letters. 2015 ; Vol. 15, No. 3. pp. 1836-1842.
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Biswas, S, Liu, X, Jarrett, JW, Brown, D, Pustovit, V, Urbas, A, Knappenberger, KL, Nealey, PF & Vaia, RA 2015, 'Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles', Nano letters, vol. 15, no. 3, pp. 1836-1842. https://doi.org/10.1021/nl504613q

Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles. / Biswas, Sushmita; Liu, Xiaoying; Jarrett, Jeremy W.; Brown, Dean; Pustovit, Vitaliy; Urbas, Augustine; Knappenberger, Kenneth L.; Nealey, Paul F.; Vaia, Richard A.

In: Nano letters, Vol. 15, No. 3, 11.03.2015, p. 1836-1842.

Research output: Contribution to journalArticle

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T1 - Nonlinear chiro-optical amplification by plasmonic nanolens arrays formed via directed assembly of gold nanoparticles

AU - Biswas, Sushmita

AU - Liu, Xiaoying

AU - Jarrett, Jeremy W.

AU - Brown, Dean

AU - Pustovit, Vitaliy

AU - Urbas, Augustine

AU - Knappenberger, Kenneth L.

AU - Nealey, Paul F.

AU - Vaia, Richard A.

PY - 2015/3/11

Y1 - 2015/3/11

N2 - 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.

AB - 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.

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