Theory of second harmonic generation at a metal surface with surface plasmon excitation

Agarwal, G. S.; Jha, Sudhanshu S.

doi:10.1016/0038-1098(82)90534-8

Cited by 113 publications

(99 citation statements)

References 15 publications

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“…Returning to the excitation profile for silver, available theory by Agarwal and Jha [28] supports the notion that 2-photon plasmon-resonance enhancement effects should exist. (More recent theoretical studies by Hua and Gersten [29], Bennemann and co-workers [30], and Dadap and co-workers [31] also predict 2-photon resonance enhancement.)…”

Section: Nonlinear Spectral Behaviormentioning

confidence: 74%

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Johnson

Hupp

et al. 2002

Chemical Physics Letters

142

109

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The optical frequency doubling properties of silver, copper, and platinum nanoparticles in aqueous solution are studied via hyper-Rayleigh scattering (HRS) spectroscopy. Substantial HRS responses are observed for silver and copper particles. The response is attributed to enhancement due to resonance of the nonlinearly scattered light with the particles' surface plasmon absorption band. Platinum particles, which lack visible-region plasmon absorption, do not display detectable HRS signals. The largest signals from silver particles are observed under conditions of two-photon resonance, qualitatively consistent with the predictions of available theory; smaller yet still impressive signals are observed under pre-and post-resonant conditions. Ó

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Section: Nonlinear Spectral Behaviormentioning

confidence: 74%

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Johnson

Hupp

et al. 2002

Chemical Physics Letters

142

109

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“…More recently, it has been demonstrated that the origin of the SHG process in gold and silver metallic particles is electric-dipole allowed due to the breaking of symmetry at the particle surface and the deviation of the shape of the particles from perfect spheres [10,11]. As a consequence, the origin of the second harmonic response for these small particles is not due to the quadrupole moment, as expected for perfect nanospheres, but rather it is of a dipolar nature [12,13]. This conclusion was obtained from hyper Rayleigh scattering experiments performed in an homogeneous liquid phase.…”

Section: Introductionmentioning

confidence: 98%

Second harmonic generation response by gold nanoparticles at the polarized water/2-octanone interface: from dispersed to aggregated particles

Galletto

Gomis-Bas

Schiffrin

et al. 2007

J. Phys.: Condens. Matter

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Gold nanoparticles with a diameter of approximately 20 nm have been observed at the polarized water/2-octanone interface by the nonlinear optical technique of second harmonic generation. Electric field induced adsorption of the gold particles at this liquid/liquid interface is clearly observed and confirms that these are negatively charged. The process is quasi-reversible at high potential sweep rates, but aggregation at the interface is observed at slower sweep rates through the loss of the nonlinear optical signal. The time evolution of the second harmonic signal is also reported during potential step experiments. After a rapid increase due to adsorption, a continuous decrease in the nonlinear optical signal intensity is observed due to aggregation of the particles into large islands at the interface. Diffusion of these large islands at the interface was observed for a longer timescale through large signal fluctuations.

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“…This 4th-order dependence gives rise to a large enhancement in the SHG emission even with a moderate enhancement of the electric field in the core region, which is a much stronger effect than the ''twophoton resonance'' [18,28,29]. The internal field is often evaluated through the electrostatic approximation [25], which elegantly explains the resonance behavior of the core-shell nanostructures.…”

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confidence: 99%

Nonlinear Optical Properties of Core-Shell Nanocavities for Enhanced Second-Harmonic Generation

et al. 2010

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A nonlinear optical plasmonic core-shell nanocavity is demonstrated as an efficient, subwavelength coherent light source through second-harmonic generation. The nonlinear optical plasmonic nanocavity incorporates a noncentrosymmetric medium, which utilizes the entire mode volume for even-order nonlinear optical processes. In previous plasmonic nanocavities, enhancement of such processes was only possible at the interface but symmetry prohibited in the body. We measured an enhancement of over 500 times in the second-harmonic radiation power. Calculations show that an enhancement of over 3500 times is achievable. DOI: 10.1103/PhysRevLett.104.207402 PACS numbers: 78.67.Bf, 42.65.Ky, 73.20.Mf, 81.16.Dn Nonlinear optical (NLO) harmonic generation [1] is important in a broad range of technologies and has become of increasing interest in photonics [2][3][4], chemistry [5,6], material science [7], and biosensing [8,9]. The interest was recently renewed [10][11][12][13][14][15][16][17] by the increasing demands for subwavelength coherent light sources, a critical component in the sciences of physics, information, and biology involving nanometer length scale. As one of the most important means for this purpose, second-harmonic generation (SHG) is prohibited in bulk centrosymmetric materials, though nanoscale SHG was often achieved by breaking the symmetry through interfaces [18], imperfect spheres [19], and asymmetric shapes [20]. Nanoscale SHG is also achieved though the used of noncentrosymmetric nanocrystals [11,[13][14][15][16]21], asymmetric geometric arrangements [22], and coating of NLO material over nanospheres [23]. Practically, however, NLO harmonic generation is generally inefficient at such a small scale. Plasmonic nanocavities are thus intriguing for the construction of more efficient coherent NLO light sources because of their compact mode volume [24] resulting in a highly concentrated local field at resonance [25]. We have synthesized plasmonic core-shell nanocavities using a noncentrosymmetric NLO cavity medium, which enables the entire mode volume of the cavity to harness the enhanced local field. This results in an intrinsically NLO plasmonic nanocavity that is fundamentally different from previous dielectric core plasmonic nanoshells [26], where intracavity SHG is symmetry prohibited, and the plasmonic enhancement in NLO harmonic generation is so far limited to the interface [23,27]. Our calculations show that a geometry-tunable enhancement factor of up to several thousands in the SHG efficiency is theoretically achievable in these NLO plasmonic nanocavities. We experimentally demonstrate enhancements of 500 and 70 times under resonant and off-resonance conditions, respectively, using 100 nm BaTiO 3 =Au core-shell structures. The results agree well with the theoretical prediction.The principle of intracavity SHG enhancement in a plasmonic nanocavity is illustrated in Fig. 1(a). The structure consists of a noncentrosymmetric crystalline core (tetragonal BaTiO 3 as an example) of radius r 1 enclosed i...

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Theory of second harmonic generation at a metal surface with surface plasmon excitation

Cited by 113 publications

References 15 publications

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Hyper-Rayleigh scattering studies of silver, copper, and platinum nanoparticle suspensions

Second harmonic generation response by gold nanoparticles at the polarized water/2-octanone interface: from dispersed to aggregated particles

Nonlinear Optical Properties of Core-Shell Nanocavities for Enhanced Second-Harmonic Generation

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