Harmonic generation in metallic, GaAs-filled nanocavities in the enhanced transmission regime at visible and UV wavelengths.

We have conducted a theoretical study of harmonic generation from a silver grating having slits filled with GaAs. By working in the enhanced transmission regime, and by exploiting phase-locking between the pump and its harmonics, we guarantee strong field localization and enhanced harmonic generation under conditions of high absorption at visible and UV wavelengths. Silver is treated using the hydrodynamic model, which includes Coulomb and Lorentz forces, convection, electron gas pressure, plus bulk χ(3) contributions. For GaAs we use nonlinear Lorentz oscillators, with characteristic χ(2) and χ(3) and nonlinear sources that arise from symmetry breaking and Lorentz forces. We find that: (i) electron pressure in the metal contributes to linear and nonlinear processes by shifting/reshaping the band structure; (ii) TE- and TM-polarized harmonics can be generated efficiently; (iii) the χ(2) tensor of GaAs couples TE- and TM-polarized harmonics that create phase-locked pump photons having polarization orthogonal compared to incident pump photons; (iv) Fabry-Perot resonances yield more efficient harmonic generation compared to plasmonic transmission peaks, where most of the light propagates along external metal surfaces with little penetration inside its volume. We predict conversion efficiencies that range from 10(-6) for second harmonic generation to 10(-3) for the third harmonic signal, when pump power is 2 GW/cm2.

[1]  A. Zayats,et al.  Near-field distribution of optical transmission of periodic subwavelength holes in a metal film. , 2001, Physical review letters.

[2]  Sudhanshu S. Jha,et al.  OPTICAL SECOND HARMONIC GENERATION IN REFLECTION FROM MEDIA WITH INVERSION SYMMETRY. , 1968 .

[3]  F. García-Vidal,et al.  Transmission Resonances on Metallic Gratings with Very Narrow Slits , 1999, cond-mat/9904365.

[4]  Li Mei,et al.  PULSED LASER DEPOSITION OF THIN FILMS , 2000 .

[5]  S. L. Shapiro,et al.  SECOND HARMONIC GENERATION IN LiNbO3 BY PICOSECOND PULSES , 1968 .

[6]  John E. Sipe,et al.  Surface and bulk contributions to the second-order nonlinear optical response of a gold film , 2009 .

[7]  I. Sagnes,et al.  Field localization and enhancement of phase-locked second- and third-order harmonic generation in absorbing semiconductor cavities , 2009 .

[8]  E. Palik.  Handbook of Optical Constants of Solids , 1997 .

[9]  D. de Ceglia,et al.  Enhanced transmission and second harmonic generation from subwavelength slits on metal substrates , 2008, SPIE Photonics Europe.

[10]  Shuang Zhang,et al.  Second harmonic generation from patterned GaAs inside a subwavelength metallic hole array. , 2006, Optics express.

[11]  Corvi,et al.  Hydrodynamic-model calculation of second-harmonic generation at a metal surface. , 1986, Physical review. B, Condensed matter.

[12]  P. Lalanne,et al.  Negative role of surface plasmons in the transmission of metallic gratings with very narrow slits. , 2002, Physical review letters.

[13]  Reuven Gordon,et al.  Enhanced second harmonic generation from nanoscale double-hole arrays in a gold film , 2006 .

[14]  LETTER TO THE EDITOR: Strong second-harmonic radiation from a thin silver film with randomly distributed small holes , 2003 .

[15]  H. Lezec,et al.  Extraordinary optical transmission through sub-wavelength hole arrays , 1998, Nature.

[16]  W. Glenn,et al.  Second-harmonic generation by picosecond optical pulses , 1969 .

[17]  S Enoch,et al.  Strong modification of the nonlinear optical response of metallic subwavelength hole arrays. , 2006, Physical review letters.

[18]  Harry A. Atwater,et al.  Quantitative determination of optical transmission through subwavelength slit arrays in Ag films: Role of surface wave interference and local coupling between adjacent slits , 2008 .

[19]  J. Manassah,et al.  Induced phase modulation of a generated second-harmonic signal. , 1987, Optics letters.

[20]  Charles T. Rogers,et al.  Optical surface second harmonic measurements of isotropic thin-film metals: Gold, silver, copper, aluminum, and tantalum , 2004 .

[21]  H J Bakker,et al.  Second-harmonic generation of femtosecond pulses: observation of phase-mismatch effects. , 1991, Optics letters.

[22]  Jose Requejo-Isidro,et al.  Large Enhancement of the Third-order Optical Susceptibility in Cu-silica Composites Produced by Low-Energy High-Current Ion Implantation , 2001 .

[23]  Masud Mansuripur,et al.  Transmission of light through a periodic array of slits in a thick metallic film. , 2005, Optics express.

[24]  Fadi Issam Baida,et al.  Light transmission by subwavelength annular aperture arrays in metallic films , 2002 .

[25]  Pierre Chavel,et al.  Perturbative approach for surface plasmon effects on flat interfaces periodically corrugated by subwavelength apertures , 2003 .

[26]  Steve Blair,et al.  Fluorescence enhancement from an array of subwavelength metal apertures. , 2003, Optics letters.

[27]  Steve Blair,et al.  Third-harmonic generation from arrays of sub-wavelength metal apertures. , 2009, Optics express.

[28]  N. Kothari,et al.  Transient second-harmonic generation: influence of effective group-velocity dispersion , 1988 .

[29]  R. Boyd,et al.  Accessing the optical nonlinearity of metals with metal- dielectric photonic bandgap structures. , 1999, Optics letters.

[30]  John E. Sipe,et al.  Analysis of second-harmonic generation at metal surfaces , 1980 .

[31]  V. Agranovich,et al.  Surface polaritons : electromagnetic waves at surfaces and interfaces , 1982 .

[32]  Kevin J. Malloy,et al.  Second harmonic generation from a nanopatterned isotropic nonlinear material , 2006 .

[33]  A. Moreau,et al.  Origin of the super-enhanced light transmission through a 2-D metallic annular aperture array: a study of photonic bands , 2004 .

[34]  Michael Scalora,et al.  Inhibition of linear absorption in opaque materials using phase-locked harmonic generation. , 2008, Physical review letters.

[35]  Bernard Kippelen,et al.  A comprehensive analysis of the contributions to the nonlinear optical properties of thin Ag films , 2010 .

[36]  Generation Efficiency of the Second Harmonic Inhomogeneous Component , 2010, 1010.4693.

[37]  Michael Scalora,et al.  Anomalous momentum states, non-specular reflections, and negative refraction of phase-locked, second-harmonic pulses , 2008 .

[38]  Robert W Boyd,et al.  Enhanced nonlinear optical response of one-dimensional metal-dielectric photonic crystals. , 2004, Physical review letters.

[39]  E. Barakat,et al.  Second harmonic generation enhancement by use of annular aperture arrays embedded into silver and filled by lithium niobate. , 2010, Optics express.

[40]  F Rotermund,et al.  Terahertz near-field enhancement in narrow rectangular apertures on metal film. , 2009, Optics express.

[41]  Olga G. Kosareva,et al.  Role of phase matching in pulsed second-harmonic generation: Walk-off and phase-locked twin pulses in negative-index media , 2007 .

[42]  Jennifer J. Quinn,et al.  Hydrodynamic model for surface plasmons in metals and degenerate semiconductors , 1976 .

[43]  Ajay Nahata,et al.  Enhanced nonlinear optical conversion from a periodically nanostructured metal film. , 2003, Optics letters.

[44]  M. Neviere,et al.  Nonlinear polarisation inside metals: A mathematical study of the free-electron model , 1986 .

[45]  Nicolaas Bloembergen,et al.  Light waves at the boundary of nonlinear media , 1962 .

[46]  M. Centini,et al.  Second- and third-harmonic generation in metal-based structures , 2010 .

[47]  M. Scalora,et al.  Third harmonic generation at 223 nm in the metallic regime of GaP , 2011 .

[48]  隆夫 国府田,et al.  V. M. Agranovich and D. L. Mills 編: Surface Polaritons, Electromagnetic Waves at Surfaces and Interfaces, North-Holland, Amsterdam and New York, 1982, xvi+717ページ, 24.5×17cm, 38,350円 (Modern Problems in Condensed Matter Sciences, Vol. 1). , 1983 .

[49]  Michael Scalora,et al.  Second harmonic generation from nanoslits in metal substrates: applications to palladium-based H2 sensor , 2008 .

[50]  Steve Blair,et al.  Second-harmonic generation from an array of sub-wavelength metal apertures , 2005 .

[51]  Steve Blair,et al.  Second-harmonic generation from an array of subwavelength metal apertures , 2005, SPIE OPTO.

[52]  Yaochun Shen.  Principles of nonlinear optics , 1984 .