Third Harmonic Mechanism in Complex Plasmonic Fano Structures

We perform third harmonic spectroscopy of dolmen-type nanostructures, which exhibit plasmonic Fano resonances in the near-infrared. Strong third harmonic emission is predominantly radiated close to the low energy peak of the Fano resonance. Furthermore, we find that the third harmonic polarization of the subradiant mode interferes destructively and diminishes the nonlinear signal in the far-field. By comparing the experimental third harmonic spectra with finite element simulations and an anharmonic oscillator model, we find strong indications that the source of the third harmonic is the optical nonlinearity of the bare gold enhanced by the resonant plasmonic polarization.

[1]  Ulrich Hohenester,et al.  Tailoring spatiotemporal light confinement in single plasmonic nanoantennas. , 2012, Nano letters.

[2]  J. Aizpurua,et al.  Interference, coupling, and nonlinear control of high-order modes in single asymmetric nanoantennas. , 2012, ACS nano.

[3]  B. Metzger,et al.  High-power widely tunable sub-20 fs Gaussian laser pulses for ultrafast nonlinear spectroscopy. , 2011, Optics express.

[4]  A. Zayats,et al.  Nonlinear plasmonics , 2012, Nature Photonics.

[5]  Zhaoning Yu,et al.  Nonlinear optical spectroscopy of photonic metamaterials , 2007, 2008 Conference on Lasers and Electro-Optics and 2008 Conference on Quantum Electronics and Laser Science.

[6]  Stefan Linden,et al.  Experiments on second- and third-harmonic generation from magnetic metamaterials. , 2008, Optics express.

[7]  Germany,et al.  Lineshape of harmonic generation by metallic nanoparticles and metallic photonic crystal slabs , 2005 .

[8]  M. Hentschel,et al.  Classical analog of electromagnetically induced absorption in plasmonics , 2012, 2012 Conference on Lasers and Electro-Optics (CLEO).

[9]  A. A. Fedyanin,et al.  Contribution of the magnetic resonance to the third harmonic generation from a fishnet metamaterial , 2012 .

[10]  Nicolas Large,et al.  Near-field mediated plexcitonic coupling and giant Rabi splitting in individual metallic dimers. , 2013, Nano letters.

[11]  Y. Wang,et al.  Plasmon-induced transparency in metamaterials. , 2008, Physical review letters.

[12]  Simon Rivier,et al.  Enhanced second-harmonic generation from double resonant plasmonic antennae. , 2012, Optics express.

[13]  Carsten Rockstuhl,et al.  Towards the origin of the nonlinear response in hybrid plasmonic systems. , 2011, Physical review letters.

[14]  R. W. Christy,et al.  Optical Constants of the Noble Metals , 1972 .

[15]  Michel Orrit,et al.  Third-harmonic generation from single gold nanoparticles. , 2005, Nano letters.

[16]  Miguel Navarro-Cia,et al.  Broad-band near-infrared plasmonic nanoantennas for higher harmonic generation. , 2012, ACS nano.

[17]  Jari Turunen,et al.  Multipole interference in the second-harmonic optical radiation from gold nanoparticles. , 2007, Physical review letters.

[18]  Mohsen Rahmani,et al.  Multiresonant broadband optical antennas as efficient tunable nanosources of second harmonic light. , 2012, Nano letters.

[19]  W. K. Burns,et al.  Reflected third harmonic generated by picosecond laser pulses , 1969 .

[20]  Markku Kuittinen,et al.  Enhancement of second-harmonic generation from metal nanoparticles by passive elements. , 2013, Physical review letters.

[21]  Harald Giessen,et al.  Quantitative modeling of the third harmonic emission spectrum of plasmonic nanoantennas. , 2012, Nano letters.

[22]  Xiang Zhang,et al.  Contribution of electric quadrupole resonance in optical metamaterials , 2008, 2008 Conference on Lasers and Electro-Optics and 2008 Conference on Quantum Electronics and Laser Science.

[23]  Mark I. Stockman,et al.  Nanoscience: Dark-hot resonances , 2010, Nature.

[24]  Lukas Novotny,et al.  Enhancing the nonlinear optical response using multifrequency gold-nanowire antennas. , 2012, Physical review letters.

[25]  Yu Zhang,et al.  Coherent Fano resonances in a plasmonic nanocluster enhance optical four-wave mixing , 2013, Proceedings of the National Academy of Sciences.

[26]  B. Metzger,et al.  Third-harmonic spectroscopy and modeling of the nonlinear response of plasmonic nanoantennas. , 2012, Optics letters.

[27]  T. Meier,et al.  Collective effects in second-harmonic generation from split-ring-resonator arrays , 2012, 2012 Conference on Lasers and Electro-Optics (CLEO).

[28]  P. Nordlander,et al.  The Fano resonance in plasmonic nanostructures and metamaterials. , 2010, Nature materials.

[29]  Harald Giessen,et al.  Plasmonic analogue of electromagnetically induced transparency at the Drude damping limit. , 2009, Nature materials.

[30]  Benjamin Gallinet,et al.  Relation between near-field and far-field properties of plasmonic Fano resonances. , 2011, Optics express.

[31]  Jérémy Butet,et al.  Augmenting second harmonic generation using Fano resonances in plasmonic systems. , 2013, Nano letters.