Multipolar second-harmonic generation in noble metal nanoparticles

Bachelier, Guillaume; Russier‐Antoine, Isabelle; Bénichou, Emmanuel; Jonin, Christian; Brevet, Pierre‐François

doi:10.1364/josab.25.000955

Cited by 142 publications

(156 citation statements)

References 27 publications

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“…The presence of this very sharp resonance near 800 nm suggests that the second harmonic light is most likely generated from the regions of high charge accumulation or in the places of strong field-enhancement due to the lightning-rod effect. Its sensitivity to chirality can then be attributed to enantiomerically sensitive plasmon modes, which were already observed in linear optics [30], and which could be related to the SHG response through recent theoretical studies [31][32][33].…”

Section: Resultsmentioning

confidence: 82%

Linearly polarized second harmonic generation microscopy reveals chirality

Valev¹,

Silhanek²,

Smisdom³

et al. 2010

Opt. Express

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Abstract:In optics, chirality is typically associated with circularly polarized light. Here we present a novel way to detect the handedness of chiral materials with linearly polarized light. We performed Second Harmonic Generation (SHG) microscopy on G-shaped planar chiral nanostructures made of gold. The SHG response originates in distinctive hotspots, whose arrangement is dependent of the handedness. These results uncover new directions for studying chirality in artificial materials.

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Section: Resultsmentioning

confidence: 82%

Linearly polarized second harmonic generation microscopy reveals chirality

Valev¹,

Silhanek²,

Smisdom³

et al. 2010

Opt. Express

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“…54 The results show that the impact on the SH far-field is higher in the case of a defect on the lateral arm side than in the case of a defect in the gap, despite the strong fundamental field enhancement in the gap. This somewhat counterintuitive result is easily understood having in mind that SHG from the nanogap is not efficiently radiated to the far-field due to destructive interferences (see the case of the perfect antenna, Figure 4).…”

Section: Etallic Nanostructures Supporting Surface Plasmon Resonancmentioning

confidence: 85%

Ultrasensitive Optical Shape Characterization of Gold Nanoantennas Using Second Harmonic Generation

2013

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Second harmonic generation from plasmonic nanoantennas is investigated numerically using a surface integral formulation for the calculation of both the fundamental and the second harmonic electric field. The comparison between a realistic and an idealized gold nanoantenna shows that second harmonic generation is extremely sensitive to asymmetry in the nanostructure shape even in cases where the linear response is barely modified. Interestingly, minute geometry asymmetry and surface roughness are clearly revealed by far-field analysis, demonstrating that second harmonic generation is a promising tool for the sensitive optical characterization of plasmonic nanostructures. Furthermore, defects located where the linear field is strong (e.g., in the antenna gap) do not necessarily have the strongest impact on the second harmonic signal. KEYWORDS: Plasmonics, nonlinear optics, surface integral formulation, realistic nanostructures Furthermore, the coupling between several substructures is a convenient way to control SPR properties.2,3 In particular, bringing two nanostructures in close proximity results in an enhancement by several orders of magnitude of the electric field in the hot spot. This geometry is called a nanoantenna, or an optical antenna, since it represents the optical analogous of microwave and radiowave antennas.4−6 The electromagnetic properties of nanoantennas can be tuned by modifying their geometric parameters (length, shape, and gap dimension) and tailored for specific applications.7 For instance, optical antennas have been designed for studying quantum systems at the single emitter level, Optical antennas are also promising for the observation of nonlinear optical effects that require a high electric field such as that observed in the hot spots.19 Several studies have reported the observation of multiphoton excited luminescence, 20−22 second harmonic generation (SHG), 23,24 third harmonic generation, 25,26 high harmonic generation, 27 and four-wave mixing, 28 as well as ultrafast spectroscopy. 29,30 Recently, a new approach has been proposed to enhance nonlinear conversion in nanoantennas, using structures that are resonant at the several wavelengths involved in the frequency conversion. 31−33Among the different nonlinear parametric optical processes, SHG is the simplest one and has the advantage of being sensitive to the symmetry of the plasmonic nanostructures as well as their spatial arrangement. 34−40 Contrary to the other nonlinear optical processes, it was observed that SHG can be significantly suppressed in centrosymmetric gaps, although the fundamental electric field is strongly enhanced. 41 On the other hand, efficient SHG is observed in asymmetric gaps, such as the one formed in noncentrosymmetric T-shaped gold dimers.42 A clear insight into the impact of the nanoantenna shape on their SHG properties, particularly in the far-field, is therefore required to guide further the development of SHG from nanoantennas for practical applications like nonlinear plasmonics sensing. 4...

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“…In fact, the SHG dependency of material symmetry and the nanostructure shape open up a series of technique development of in situ ultrasensitive nonlinear optical characterization, including the detection of very slight deviations from perfectly symmetric shapes [131,132] as well as minute surface roughness [133,134]. Because SHG can point out defects that linear responses cannot, it is attractive in some specific nanoparticle geometries such as the nonlinear optical characterization of gold nanotips by incident beams with azimuthal and radial polarizations [135].…”

Section: Inherent Harmonic Generationsmentioning

confidence: 99%

Nonlinear plasmonic imaging techniques and their biological applications

et al. 2016

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Nonlinear optics, when combined with microscopy, is known to provide advantages including novel contrast, deep tissue observation, and minimal invasiveness. In addition, special nonlinearities, such as switch on/off and saturation, can enhance the spatial resolution below the diffraction limit, revolutionizing the field of optical microscopy. These nonlinear imaging techniques are extremely useful for biological studies on various scales from molecules to cells to tissues. Nevertheless, in most cases, nonlinear optical interaction requires strong illumination, typically at least gigawatts per square centimeter intensity. Such strong illumination can cause significant phototoxicity or even photodamage to fragile biological samples. Therefore, it is highly desirable to find mechanisms that allow the reduction of illumination intensity. Surface plasmon, which is the collective oscillation of electrons in metal under light excitation, is capable of significantly enhancing the local field around the metal nanostructures and thus boosting up the efficiency of nonlinear optical interactions of the surrounding materials or of the metal itself. In this mini-review, we discuss the recent progress of plasmonics in nonlinear optical microscopy with a special focus on biological applications. The advancement of nonlinear imaging modalities (including incoherent/ coherent Raman scattering, two/three-photon luminescence, and second/third harmonic generations that have been amalgamated with plasmonics), as well as the novel subdiffraction limit imaging techniques based on nonlinear behaviors of plasmonic scattering, is addressed.

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Multipolar second-harmonic generation in noble metal nanoparticles

Cited by 142 publications

References 27 publications

Linearly polarized second harmonic generation microscopy reveals chirality

Linearly polarized second harmonic generation microscopy reveals chirality

Ultrasensitive Optical Shape Characterization of Gold Nanoantennas Using Second Harmonic Generation

Nonlinear plasmonic imaging techniques and their biological applications

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