Enhancement of the second harmonic signal of nonlinear crystals by a single metal nanoantenna

Gürdal, Emre; Horneber, Anke; Meixner, Alfred J.; Kern, D. P.; Zhang, Dai; Fleischer, Monika

doi:10.1039/d0nr05696k

Cited by 7 publications

(5 citation statements)

References 48 publications

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“…In the second function, radiative plasmons tuned to the up- or down-converted frequency enhance the out-coupling of light by extracting energy from the NLO material through near-field interactions and then quickly scattering it to the far-field, i.e., via the Purcell effect 19 , 38 . Carefully designed nanostructures can make use of both strategies 22 , and antenna effects can be significant whether or not the NLO material itself is optically resonant 21 .…”

Section: Resultsmentioning

confidence: 99%

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Near-field enhancement of optical second harmonic generation in hybrid gold–lithium niobate nanostructures

et al. 2023

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Nanophotonics research has focused recently on the ability of nonlinear optical processes to mediate and transform optical signals in a myriad of novel devices, including optical modulators, transducers, color filters, photodetectors, photon sources, and ultrafast optical switches. The inherent weakness of optical nonlinearities at smaller scales has, however, hindered the realization of efficient miniaturized devices, and strategies for enhancing both device efficiencies and synthesis throughput via nanoengineering remain limited. Here, we demonstrate a novel mechanism by which second harmonic generation, a prototypical nonlinear optical phenomenon, from individual lithium niobate particles can be significantly enhanced through nonradiative coupling to the localized surface plasmon resonances of embedded gold nanoparticles. A joint experimental and theoretical investigation of single mesoporous lithium niobate particles coated with a dispersed layer of ~10 nm diameter gold nanoparticles shows that a ~32-fold enhancement of second harmonic generation can be achieved without introducing finely tailored radiative nanoantennas to mediate photon transfer to or from the nonlinear material. This work highlights the limitations of current strategies for enhancing nonlinear optical phenomena and proposes a route through which a new class of subwavelength nonlinear optical platforms can be designed to maximize nonlinear efficiencies through near-field energy exchange.

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Section: Resultsmentioning

confidence: 99%

“…In stark contrast, many past investigations [18][19][20][21][22][23] have achieved enhancement factors between 5 and 20 by employing carefully tailored hybrid nanostructures. The manufacture of such structures is technically challenging, causing difficulties with the reproduction of large enhancement ratios between samples 22 .…”

Section: Introductionmentioning

confidence: 86%

Near-field enhancement of optical second harmonic generation in hybrid gold–lithium niobate nanostructures

et al. 2023

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“…Herein, lithium niobate (LiNbO 3 , LN) is selected as the core material to grow a raspberry-like Au shell. Due to its noncentrosymmetric crystalline structure, LN, which is a mixed-metal oxide exhibiting piezoelectricity, electro-optics, and second-order nonlinear optical properties at the nanoscale, is utilized for both multimodal imaging and phototriggered release of chemotherapeutics. − Combining the intrinsic nonlinear optical properties of noncentrosymmetric oxide materials with plasmonic resonances is an effective way to enhance several nonlinear processes, as already demonstrated for mesoporous LN microspheres, for LN bulk crystals combined with various Au (Au) nanostructures, , and for another dielectric core composed of barium titanate (BaTiO 3 ). − Note that, in the bulk form, hybrid plasmonic waveguides are able to produce giant second harmonic (SH) signals, thanks to the influence of plasmonic resonances on the confined modes. , The encapsulation of LN NPs in a raspberry-like Au nanoshell by a wet chemistry approach has several noticeable advantages. First, it avoids the difficulties related to the nanofabrication of precisely positioned nanostructures and provides a scalable elaboration route .…”

Section: Introductionmentioning

confidence: 99%

Black Gold Plasmon Response of a Raspberry Shell Grown on Lithium Niobate Nonlinear Nanoparticles

Bredillet,

Behel,

Taitt

et al. 2023

J. Phys. Chem. C

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Lithium niobate nanoparticles (LN NPs) coated with a raspberry-like gold (Au) shell are synthesized herein. The strong plasmon resonance coupling between Au NPs in raspberry nanostructures is expected to modify the surface and cavity optical fields and thus significantly alter the second harmonic (SH) signal generated by the noncentrosymmetric crystalline core of LN. Plasmonic properties of the core−shell NPs are first modeled using the discrete-dipole approximation method. The influence of the size and filling fraction of Au NPs on the extinction cross section is correlated with the experimental responses. Comparison at 800 nm of the first hyperpolarizability of individual Au NPs, bare LN cores, and hybrid nanostructures demonstrates no enhancement. It reveals instead an octupolar response in the polarization-resolved data, consistent with a dominant surface contribution of the raspberry-like Au shell. The wavelength-dependent SH emission of the hybrid nanostructures is finally determined in the 700−1300 nm excitation range, and a continuous increase that reaches a factor up to 20 is only evidenced at the longest excitation wavelength of 1300 nm.

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“…LiNbO 3 is one of the most widely employed dielectrics for advanced photonics and optoelectronics due to its remarkable acousto-optic, electro-optic, and nonlinear coefficients [ 25 , 26 , 27 ]. The association of LiNbO 3 with noble metal plasmonic nanostructures has shown to be a useful route to provide solid-state platforms for boosting nonlinear processes at the nanoscale [ 17 , 19 , 21 , 28 ]. SHG enhancement factors as high as 400 have been reported by using hexagonal plasmonic necklaces of silver nanoparticles formed on the LiNbO 3 crystal surface [ 21 ].…”

Section: Introductionmentioning

confidence: 99%

Giant Second Harmonic Generation Enhancement by Ag Nanoparticles Compactly Distributed on Hexagonal Arrangements

2021

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The association of plasmonic nanostructures with nonlinear dielectric systems has been shown to provide useful platforms for boosting frequency conversion processes at metal-dielectric interfaces. Here, we report on an efficient route for engineering light–matter interaction processes in hybrid plasmonic-χ(2) dielectric systems to enhance second harmonic generation (SHG) processes confined in small spatial regions. By means of ferroelectric lithography, we have fabricated scalable micrometric arrangements of interacting silver nanoparticles compactly distributed on hexagonal regions. The fabricated polygonal microstructures support both localized and extended plasmonic modes, providing large spatial regions of field enhancement at the optical frequencies involved in the SHG process. We experimentally demonstrate that the resonant excitation of the plasmonic modes supported by the Ag nanoparticle-filled hexagons in the near infrared region produces an extraordinary 104-fold enhancement of the blue second harmonic intensity generated in the surface of a LiNbO3 crystal. The results open new perspectives for the design of efficient hybrid plasmonic frequency converters in miniaturized devices.

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Enhancement of the second harmonic signal of nonlinear crystals by a single metal nanoantenna

Abstract: This work fundamentally investigates how the second harmonic generation (SHG) from commercial nonlinear crystals can be boosted by the addition of individual optical nanoantennas.

Cited by 7 publications

References 48 publications

Near-field enhancement of optical second harmonic generation in hybrid gold–lithium niobate nanostructures

Near-field enhancement of optical second harmonic generation in hybrid gold–lithium niobate nanostructures

Black Gold Plasmon Response of a Raspberry Shell Grown on Lithium Niobate Nonlinear Nanoparticles

Giant Second Harmonic Generation Enhancement by Ag Nanoparticles Compactly Distributed on Hexagonal Arrangements

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