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Multipole interference in the second-harmonic optical radiation from gold nanoparticles.

Sami Kujala1, Brian K Canfield, Martti Kauranen

  • 1Optics Laboratory, Institute of Physics, Tampere University of Technology, PO Box 692, FI-33101 Tampere, Finland. sami.kujala@tut.fi

Physical Review Letters
|May 16, 2007
PubMed
Summary
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Higher multipole radiation, including magnetic dipole and electric quadrupole effects, significantly impacts second-harmonic generation in metal nanoparticle arrays. These multipole contributions influence interference patterns observed in reflected and transmitted light, depending on fundamental field polarization.

Area of Science:

  • Nanophotonics and Plasmonics
  • Nonlinear Optics

Background:

  • Second-harmonic (SH) generation is a key nonlinear optical process.
  • Understanding the contributions of different multipole moments is crucial for controlling SH emission.

Purpose of the Study:

  • To experimentally demonstrate and quantify higher multipole contributions (magnetic dipole and electric quadrupole) in SH generation from metal nanoparticle arrays.
  • To investigate the influence of these higher multipoles on interference effects in reflected and transmitted SH light.

Main Methods:

  • Fabrication of metal nanoparticle arrays.
  • Experimental measurement of SH intensities in both reflection and transmission modes.
  • Analysis of SH intensity dependence on the polarization of the fundamental incident light.

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Main Results:

  • Experimental evidence for significant magnetic dipole and electric quadrupole radiation in SH generation.
  • Observed opposite interference effects in reflected and transmitted SH intensities due to fundamental differences in radiative properties of electric dipoles versus higher multipoles.
  • Demonstrated clear dependence of interference effects on the fundamental field polarization, confirming the role of multipole effects.

Conclusions:

  • Higher multipole radiation plays a substantial role in the nonlinear optical response of metal nanoparticle arrays.
  • These multipole effects contribute up to 20% of the total emitted SH field amplitude under specific polarization conditions.
  • The findings highlight the importance of considering multipole effects for designing and optimizing nonlinear nanophotonic devices.