Single-Beam and Enhanced Two-Beam Second-Harmonic Generation from Silicon Nanocrystals by Use of Spatially Inhomogeneous Femtosecond Pulses

Figliozzi, P.; Sun, Lixing; Jiang, Yongqiang; Matlis, Nicholas H.; Mattern, B.; Downer, M. C.; Withrow, S. P.; White, C. W.; Mochán, W. Luis; Mendoza, Bernardo S.

doi:10.1103/physrevlett.94.047401

Cited by 74 publications

(54 citation statements)

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“…The FHG work, done with the objective of interpreting data obtained by the Downer group on surfaces of varying roughness [28], showed that interface angles were not always those of the bulk, a result also found by Kwon et al [5] Our most recent application, to amorphous (a-) SiO 2 [14], was intended as a first step toward understanding the data of Figliozzi et al [29] on crystalline Si nanoparticles embedded in SiO 2 . Among other results, this work showed that the Liénard-Wiechert expression for radiation from an accelerated charge, although valid for linear optics, did not incorporate the relativistic contribution and hence could not be used for NLO.…”

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confidence: 85%

“…This lateral gradient can determine among other phenomena the spatial pattern of the emerging radiation, for example, the 2-lobed pattern reported in Ref. [29] for SHG from amorphous material under Gaussian-beam excitation [14]. Since lateral gradients can be engineered, for example through the use of crossedbeam excitation, this may be of considerable importance in the future.…”

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confidence: 97%

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Bond models in linear and nonlinear optics

Aspnes

2010

Physica Status Solidi (b)

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Atomic-scale descriptions of linear-optical properties such as reflection are nearly a century old, but surprisingly, analogous models describing nonlinear-optical (NLO) properties as the natural dynamic response of bond charges driven by an external field are a recent development. These bond-charge models have proven to be particularly useful in describing the relevant physics of second-, third-, and fourth-harmonic generation, identifying previously unrecognized contributions to NLO responses, and uncovering well-disguised correlations in tensor parameters determined phenomenologically from symmetry conditions. Current capabilities are discussed, and opportunities for improved understanding noted. 1 Introduction The availability of continuum sources of radiation covering wide spectral ranges has not only made linear-optical spectroscopy possible, but also linear-optical techniques indispensable for determining information nondestructively about materials, interfaces, and structures. Owing to the higher-order tensors involved, in principle nonlinear-optical (NLO) probes are much more powerful, but spectroscopic data [1-5] have been difficult to acquire. However, commercial femtosecond systems that can tune over wide wavelength ranges are becoming available, and we are rapidly reaching the point where NLO spectroscopy will be routine.The potentially greater diagnostic power of NLO comes at a price, specifically the need to use more complex models and methods to interpret these more complex data. For most linear-optical applications, measurements can be analyzed using macroscopic parameters such as the dielectric function e, which for isotropic materials is a scalar and anisotropic materials a second-rank tensor. Here a return to fundamentals is generally unnecessary, and the last contact most linear-optical spectroscopists have had with atomic scale properties is the textbook derivation of the ClausiusMossotti relation [6], which relates the dielectric constant to local polarizabilities in the static limit.For NLO, quantities equivalent to e are the susceptibility tensors x ijk , x ijkl , etc. [7]. Symmetry-allowed NLO tensor components have been determined for all crystal classes, and

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confidence: 85%

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confidence: 97%

Bond models in linear and nonlinear optics

Aspnes

2010

Physica Status Solidi (b)

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“…Dispersion of both the ordinary and extraordinary refractive indices of ZnO are taken from reference (Figliozzi et al, 2005).…”

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confidence: 99%

Nonlinear Ellipsometry by Second Harmonic Generation

Bovino¹,

Larciprete²,

Sibilia³

et al. 2012

Nonlinear Optics

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“…Dipolar SHG is allowed through a surface contribution arising at the interface between centrosymmetric materials where centrosymmetry is broken [1,2]. However, when higher-order multipole interactions [3,4], such as magnetic-dipole and electric-quadrupole interactions, are taken into account, SHG can occur even inside bulk centrosymmetric materials, which was observed in several experiments [5][6][7][8]. When SHG is used as a surface or interface probe, it is essential to separate bulk contributions from the measured SH signal and verify that such multipolar contributions are actually negligible [9].…”

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Direct observation of bulk second-harmonic generation inside a glass slide with tightly focused optical fields

et al. 2016

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Bulk second-harmonic generation (SHG) inside glass slides is directly detected unambiguously without interference from surface contributions. This is enabled by tightly focused and highly localized ultrashort laser pulses. The theoretical calculations based on vector diffraction theory and the phenomenological model of SHG inside centrosymmetric materials agree well with the measured far-field SHG radiation patterns for different polarization states of the fundamental beam. The results indicate that the observed bulk SHG is predominantly related to the bulk parameter δ and originates from the three-dimensional field gradient in the focal region. DOI: 10.1103/PhysRevB.93.161109 Under the electric dipole approximation of light-matter interaction, second-harmonic generation (SHG) is usually considered forbidden in bulk centrosymmetric materials. Dipolar SHG is allowed through a surface contribution arising at the interface between centrosymmetric materials where centrosymmetry is broken [1,2]. However, when higher-order multipole interactions [3,4], such as magnetic-dipole and electric-quadrupole interactions, are taken into account, SHG can occur even inside bulk centrosymmetric materials, which was observed in several experiments [5][6][7][8]. When SHG is used as a surface or interface probe, it is essential to separate bulk contributions from the measured SH signal and verify that such multipolar contributions are actually negligible [9]. In addition, as suggested recently, strong multipole interactions may bypass the noncentrosymmetry requirement and promote applications of new nonlinear materials [10,11]. Therefore, a thorough understanding of the physical mechanisms behind bulk SHG from bulk centrosymmetric materials is fundamental for many practical applications utilizing SHG [12].Various attempts have been made to characterize surface and bulk contributions to SHG [7,8,13,14]. For example, the SHG based on two noncollinear fundamental beams [7,8] has been widely used to study surface and bulk contributions in a quantitative way. However, up to now, the separation of surface and bulk contributions is still known to be a fundamental difficulty in the field of SHG from centrosymmetric materials. Since two-beam overlap in a spatial region is usually several millimeters long [8], the excitation field is not highly localized. Furthermore, as the SH signal is often too weak to detect when the interaction volume is deep inside the bulk material, the excitation region is often chosen to be near the surface in order to maximize signal intensity [15]. Thus the surface dipolar response cannot be completely avoided, which often perturbs the bulk response. This contributes to the wide variation of results reported in the literature. So far, the mechanism of bulk SHG inside centrosymmetric materials still remains unclear.Bulk SHG has been previously observed in centrosymmetric gaseous materials [16,17] with focused laser pulses, where * Corresponding author: rhui@ku.edu SHG was attributed to the ponderomotive force cau...

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Single-Beam and Enhanced Two-Beam Second-Harmonic Generation from Silicon Nanocrystals by Use of Spatially Inhomogeneous Femtosecond Pulses

Cited by 74 publications

References 17 publications

Bond models in linear and nonlinear optics

Bond models in linear and nonlinear optics

Nonlinear Ellipsometry by Second Harmonic Generation

Direct observation of bulk second-harmonic generation inside a glass slide with tightly focused optical fields

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