Second-harmonic generation in arrays of spherical particles

Mochán, W. Luis; Maytorena, Jesús A.; Mendoza, Bernardo S.; Brudny, Vera L.

doi:10.1103/physrevb.68.085318

Cited by 62 publications

(64 citation statements)

References 28 publications

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“…[13] for the nonlinear response of a single sphere of nanoscopic dimensions made up of a centrosymmetric material. Although the centrosymmetry is locally lost close to the surface of each sphere, opposite sides acquire different polarizations according to their orientation with respect to the applied field.…”

Section: Nonlinear Response Of a Single Spherementioning

confidence: 99%

“…Under these assumptions expressions for the nonlinear polarizabilities g n , n ¼ e; m; q;q q of a single sphere may be obtained [13] in terms of the dipolarly allowed surface response functions (namely, the dimensionless functions aðwÞ, bðwÞ and f ðwÞ which are commonly used to parametrize the response of a flat, homogeneous surface [14,15]), and the quadrupolarly allowed bulk response (gðwÞ and d 0 ðwÞ) of a flat semiinfinite homogeneous isotropic material [16]. Thus, we may take advandtage of various models and measurements of those intrinsic response functions to obtain the non linear susceptibility of small particles.…”

Section: Nonlinear Response Of a Single Spherementioning

confidence: 99%

“…For example, within a composite, the electric field has longitudinal short range spatial fluctuations [12] besides the transverse macroscopic field, and the latter is not necessarily a plane wave. A general theory for the quadratic nonlinear response of a single small nonmagnetic centrosymmetric sphere illuminated by an arbitrary non-homogeneous electromagnetic field was developed by Mochn et al in [13], from where the results in both [8,11] can be derived.…”

Section: Introductionmentioning

confidence: 99%

“…In this paper we use the hyperpolarizabilities obtained in [13] to calculate the macroscopic second order susceptibilities of a composite made up of a random distribution of these spheres. We calculate the second-harmonic radiation from a thin homogeneous slab of this composite illuminated by a focused gaussian beam, and from an inhomogeneous composite with a density gradient.…”

Section: Introductionmentioning

confidence: 99%

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Second harmonic generation from a collection of nanoparticles

Brudny

Mochán

Maytorena

et al. 2003

Physica Status Solidi (b)

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In this paper we discuss the SH radiation produced by a composite film made up of nanosized spherical centrosymmetric homogeneous particles. Although each individual sphere is unable to radiate in the forward direction when illuminated by a plane wave, our results show that for a thin composite film illuminated by a focused gaussian linearly polarized beam the radiation pattern presents two narrow lobes displaced along the polarization direction by a small angle of the order of the diffraction-induced angular divergence of the linear far field. The SH radiation produced by a non-homogeneous film, on the other hand presents non-trivial patterns which depend on the fundamental frequency, the waist of the illuminating beam, the sharpness of the edge, the density profile and both the incoming and outgoing polarizations. We hope that these results can be extended to develop characterization techniques for composite films based on surface SHG or SFG.

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Section: Nonlinear Response Of a Single Spherementioning

confidence: 99%

Section: Nonlinear Response Of a Single Spherementioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Second harmonic generation from a collection of nanoparticles

Brudny

Mochán

Maytorena

et al. 2003

Physica Status Solidi (b)

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“…The response of small particles can be modeled by Second-Harmonic Rayleigh Scattering [43][44][45][46]. For small particles of low refractive index contrast, which do not significantly perturb the incident field, also the Rayleigh-Gans-Debye approximation can be used [47][48][49][50][51].…”

Section: Introductionmentioning

confidence: 99%

Plasmonic enhancement of second harmonic generation on metal coated nanoparticles

Wunderlich¹,

Peschel²

2013

Opt. Express

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Second Harmonic Generation (SHG) is a widely used tool to study surfaces. Here we investigate SHG from spherical nanoparticles consisting of a dielectric core (radius 100 nm) and a metallic shell of variable thickness. Plasmonic resonances occur that depend on the thickness of the nanoshells and boost the intensity of the Second Harmonic (SH) signal. The origin of the resonances is studied for the fundamental harmonic and the second harmonic frequencies. Mie resonances at the fundamental harmonic frequency dominate resonant effects of the SHsignal at low shell thickness. Resonances excited by a dipole emitting at SH frequency close to the surface explain the enhancement of the SHG-process at a larger shell thickness. All resonances are caused by surface plasmon polaritons, which run on the surface of the spherical particle and are in resonance with the circumference of the sphere. Because their wavelength critically depends on the properties of the metallic layer SHG resonances of core-shell nanoparticles can be easily tuned by varying the thickness of the shell. References and links1. Y. Shen, "Surface 2nd harmonic-generation -a new technique for surface studies," Annu. Rev. Mater. Sci. 16(1), 69-86 (1986). 2. H. Wang, E. C. Y. Yan, E. Borguet, and K. B. Eisenthal, "Second harmonic generation from the surface of centrosymmetric particles in bulk solution," Chem. Phys. Lett. 259(1-2), 15-20 (1996). 3. E. C. Y. Yan, Y. Liu, and K. B. Eisenthal, "New method for determination of surface potential of microscopic particles by second harmonic generation," J. Chem. Phys. B 102(33), 6331-6336 (1998 11-14 (2011). 14. J. Griffin, A. K. Singh, D. Senapati, E. Lee, K. Gaylor, J. Jones-Boone, and P. C. Ray, "Sequence-Specific HCV RNA Quantification Using the Size-Dependent Nonlinear Optical Properties of Gold Nanoparticles," Small 5 (

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Trade‐Off between Second‐ and Third‐Order Nonlinearities, Ultrafast Free Carrier Absorption and Material Damage in Silicon Nanoparticles

Rudenko

Han

Moloney

2022

Advanced Optical Materials

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that different mechanisms are involved in SHG from non-centrosymmetric and centrosymmetric semiconductor materials. The latter ones inherit the inversion symmetry that forbids electric dipole secondorder susceptibility. Nevertheless, the symmetry is broken by bulk quadrupole and surface dipole contributions. [17,18] In order to describe the nonlinear optical response of centrosymmetric materials such as silicon (Si), a phenomenological model was proposed by Bloembergen et al. [9] and applied to specific nanostructures in the recent studies. [3,19] In the pioneering work, [9] the correspondence between pheno menological and a hydrodynamic model for free electrons, commonly applied to describe second-order nonlinear response from metals, [13] was demonstrated. These two approaches, originally designed for bound and free electrons and coupled to Maxwell equations by the nonlinear polarization, form the basis to describe the perturbative nonlinear response of arbitrary nanostructures.Upon ultrashort laser excitation of all-dielectric materials, optical properties swiftly change due to photo-ionization processes, while free carrier absorption may lead to the local material damage. On the one hand, these effects are commonly considered as the limiting factors for the operating frequency conversion nanodevices. [1,2,[20][21][22][23] On the other hand, inhomogeneous free carriers can serve as an additional source for symmetry breaking [24,25] and for high-order harmonics generation in non-perturbative regimes, [7,8,26,27] and participate in ultrafast self-action, all-optical switching, and modulation at the nanoscale. [20,[28][29][30][31][32] While the applicability of the perturbative approaches is limited to describe weak intensity regimes, the extended hydrodynamic model for electron-hole plasma kinetics and electron-ion transfer gives a reliable estimate for the inhomogeneous absorption and heating processes inside the laser-excited nanostructures and describes the non-perturbative mechanism of harmonic generation due to direct electron transitions from valence to conduction band. To date, a self-consistent approach, considering both nonlinear sources and laser-induced electron-hole dynamics has not been proposed and applied in the context of SHG and THG.In the current work, a multi-physical approach is developed in order to explore the natural material limitations for nonlinear conversion efficiency achievable by ultrashort laser irradiation of Reaching the optimal second-and third-order nonlinear conversion efficiencies while avoiding undesirable free carrier absorption losses and material damage in ultrashort laser-excited nanostructures is a challenging obstacle in all-dielectric ultrafast nanophotonics. In order to elucidate the main aspects of this problem, a multi-physical model is developed, coupling nonlinear Maxwell equations supplied by surface and bulk nonlinearities with free carrier hydrodynamic equations for electron-hole plasma kinetics and electron-ion transfer for silicon. The maximum feasible effic...

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Second-harmonic generation in arrays of spherical particles

Cited by 62 publications

References 28 publications

Second harmonic generation from a collection of nanoparticles

Second harmonic generation from a collection of nanoparticles

Plasmonic enhancement of second harmonic generation on metal coated nanoparticles

Trade‐Off between Second‐ and Third‐Order Nonlinearities, Ultrafast Free Carrier Absorption and Material Damage in Silicon Nanoparticles

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