Suppression of nonlinear optical signals in finite interaction volumes of bulk materials

Cattaneo, Stefano; Siltanen, Mikael; Wang, Fu Xiang; Kauranen, Martti

doi:10.1364/opex.13.009714

Cited by 11 publications

(13 citation statements)

References 16 publications

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“…Our results indicate that the reflected SHG signal originates almost entirely from surface contributions, whereas the transmitted signal is dominated by bulk contributions. We also show that, even when the nonlinear response is of bulk origin, the SHG signal vanishes when the interaction is localized deep in the bulk medium [13]. On the contrary, bulk signals are maximized when the interaction is localized in the proximity of an interface.…”

Section: Introductionmentioning

confidence: 70%

“…We have also made the intriguing observation that, even though the transmitted SHG signal originates essentially from bulk contributions, it vanishes when the input beams intersect deep in the bulk of the sample [13]. Figure 3 (left) shows the signal obtained by translating the glass plate through the overlap of the fundamental beams.…”

Section: Resultsmentioning

confidence: 95%

“…Naively, this could be interpreted as an indication that the true bulk contributions to the measured signal are negligible and we are still addressing some type of a surface response. This surprising result can be explained by considering the growth of the SHG signal over the interaction region [13,15]. For infinite plane waves and undepleted input beams, the amplitude exiting the nonlinear medium is proportional to the integral…”

Section: Resultsmentioning

confidence: 99%

“…In the case of intersecting beams of finite size, however, the source polarization needs to be weighed by a function ( ) g z to account for the overlap of the input beams (Fig. 3, right) [13]. The function ( ) g z is assumed to be nonvanishing only within the interval a z b < < and need not be specified in detail except for general properties of continuity and smoothness.…”

Section: Resultsmentioning

confidence: 99%

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Bulk versus surface contributions in nonlinear optics of isotropic centrosymmetric media

Cattaneo

Kauranen

2005

Physica Status Solidi (b)

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The relative importance of bulk and surface contributions to the second-harmonic response of isotropic surfaces is addressed by studying the polarization properties of second-harmonic signals generated by two noncollinear input beams. Measurements on an air-glass interface reveal that the bulk contributions dominate in transmission but are negligible in reflection. Even when the nonlinear response has a bulk origin, it is strongly suppressed when the interaction volume is localized deep inside the bulk medium. Conversely, bulk contributions are maximized when the interaction volume is localized near the surface.

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Section: Introductionmentioning

confidence: 70%

Section: Resultsmentioning

confidence: 95%

Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

See 2 more Smart Citations

Bulk versus surface contributions in nonlinear optics of isotropic centrosymmetric media

Cattaneo

Kauranen

2005

Physica Status Solidi (b)

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“…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.…”

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confidence: 99%

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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Second‐harmonic spectroscopy of nano‐interfaces

Sun

Figliozzi

Jiang

et al. 2005

phys. stat. sol. (c)

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Optical second-harmonic is shown to be a noninvasive, interface-sensitive probe of silicon nanocrystals. The TEM 01 spatial mode of SHG radiation from a silicon nanocrystal composite indicates there is nonlocal dipolar (quadrupolar) polarization source which is proportional to the gradient of the incoming electric field. With two orthogonally polarized laser beams, we enhanced the SHG from nanocrystals by creating wavelength-scale, forward-radiating gradient in the second-harmonic polarization. The quantitative features of two-beam SHG were also studied with a fused silica slide. We demonstrate several techniques for isolating the nano-interface signal from the (bulk-quadrupolar) substrate signal in our samples.

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Suppression of nonlinear optical signals in finite interaction volumes of bulk materials

Cited by 11 publications

References 16 publications

Bulk versus surface contributions in nonlinear optics of isotropic centrosymmetric media

Bulk versus surface contributions in nonlinear optics of isotropic centrosymmetric media

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

Second‐harmonic spectroscopy of nano‐interfaces

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