Three-Dimensional Nanostructures as Highly Efficient Generators of Second Harmonic Light

Yu, Zhang; Grady, Nathaniel K.; Ayala-Orozco, Ciceron; Halas, Naomi J.

doi:10.1021/nl2033602

Cited by 283 publications

(289 citation statements)

References 34 publications

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“…It has recently been shown that certain plasmonic nanostructures can produce an enhanced nonlinear response when excited at their resonant frequency (1,2). Phase-matching requirements (3)(4)(5) for nonlinear optics in macroscopic media are usually optimally fulfilled at nanoscale dimensions [sinc 2 (Δk z/2) ∼1 for small z, where z is the propagation distance through the medium]. For plasmonic nanostructures, the most important property for the enhancement of nonlinear properties is their increased local fields at resonance, which can provide larger effective susceptibilities than their intrinsic material susceptibility.…”

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confidence: 99%

Coherent Fano resonances in a plasmonic nanocluster enhance optical four-wave mixing

Wen

Zhen

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

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Plasmonic nanoclusters, an ordered assembly of coupled metallic nanoparticles, support unique spectral features known as Fano resonances due to the coupling between their subradiant and superradiant plasmon modes. Within the Fano resonance, absorption is significantly enhanced, giving rise to highly localized, intense near fields with the potential to enhance nonlinear optical processes. Here, we report a structure supporting the coherent oscillation of two distinct Fano resonances within an individual plasmonic nanocluster. We show how this coherence enhances the optical four-wave mixing process in comparison with other doubleresonant plasmonic clusters that lack this property. A model that explains the observed four-wave mixing features is proposed, which is generally applicable to any third-order process in plasmonic nanostructures. With a larger effective susceptibility χ (3) relative to existing nonlinear optical materials, this coherent double-resonant nanocluster offers a strategy for designing high-performance thirdorder nonlinear optical media.nanostructured materials | nonlinear optics | phase matching T raditionally, nonlinear optical phenomena have relied on crystalline media that combine material susceptibilities and phase matching to optimize nonlinear optical processes. It has recently been shown that certain plasmonic nanostructures can produce an enhanced nonlinear response when excited at their resonant frequency (1, 2). Phase-matching requirements (3-5) for nonlinear optics in macroscopic media are usually optimally fulfilled at nanoscale dimensions [sinc 2 (Δk z/2) ∼1 for small z, where z is the propagation distance through the medium]. For plasmonic nanostructures, the most important property for the enhancement of nonlinear properties is their increased local fields at resonance, which can provide larger effective susceptibilities than their intrinsic material susceptibility.In the third-order nonlinear process of four-wave mixing (FWM), two external fields E 0 (ω 1 ) and E 0 (ω 2 ) are simultaneously incident on the nanostructure, inducing local fields E(ω 1 ) and E(ω 2 ); absorbing two ω 2 and one ω 1 photons and emitting a photon at ω FWM = 2ω 2 − ω 1 (Fig. 1A) (3). The electromagnetic FWM enhancement G FWM = jE(ω 2 )/E 0 (ω 2 )j 4 · jE(ω 1 )/E 0 (ω 1 )j 2 thus depends on the field enhancements at the input frequencies. Fanoresonant structures can exhibit very large local field enhancements (6, 7), making these structures prime candidates for nonlinear frequency generation. Although previous studies of nonlinear plasmonics used nanostructures with a single dipolar resonance (8, 9), in a multiinput process such as FWM, the conversion efficiency is expected to be further enhanced if the plasmon modes of the nanostructure are resonant with both input frequencies (10).In this study, we demonstrate highly efficient FWM from a plasmonic nanocluster that supports two distinct Fano resonances (FRs) (6,7,(11)(12)(13)(14). When excited by a coherent source, the two spatially coherent FRs oscillate...

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confidence: 99%

Coherent Fano resonances in a plasmonic nanocluster enhance optical four-wave mixing

Wen

Zhen

et al. 2013

Proc. Natl. Acad. Sci. U.S.A.

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190

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“…The localized surface plasmon resonance enhances efficiency and can be designed by selecting the nanoparticle shape for a given wavelength; selective polarization response can also be designed into the nanoparticle. A number of asymmetric plasmonic geometries have been used for harmonic generation, including L-and V-shaped nanoparticles, nanocups, and asymmetric trimers [3][4][5][6][7]. Larger plasmonic structures-such as the ratchet wheel-have also been shown to affect the polarization of harmonic emission [8][9][10][11][12].…”

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confidence: 99%

“…These characteristics make the nanospiral a strong candidate for nonlinear optical applications where a broadband plasmonic element is necessary. Unlike plasmonic structures with globally broken symmetry created by modifying or arranging nanoparticles with some inherent local symmetry, [3,4,7,14] the nanospiral has no local axis of symmetry at all so that the nanospiral can generate secondharmonic light from any polarization state. This inherent lack of symmetry therefore makes the nanospiral an attractive candidate for nonlinear metasurface elements.…”

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confidence: 99%

“…After deformation, the nanoparticles exhibit neither second-harmonic response nor the other properties of the nanospirals. If the nanospirals were coated in a protective silicon layer as shown in references [3] and [7], the power threshold could almost certainly be increased beyond an incident power of 280 µW per nanoparticle in order to create even higher harmonicgeneration efficiencies.…”

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Efficient forward second-harmonic generation from planar archimedean nanospirals

et al. 2015

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Abstract:The enhanced electric field at plasmonic resonances in nanoscale antennas can lead to efficient harmonic generation, especially when the plasmonic geometry is asymmetric on either inter-particle or intra-particle levels. The planar Archimedean nanospiral offers a unique geometrical asymmetry for second-harmonic generation (SHG) because the SHG results neither from arranging centrosymmetric nanoparticles in asymmetric groupings, nor from non-centrosymmetric nanoparticles that retain a local axis of symmetry. Here, we report forward SHG from planar arrays of Archimedean nanospirals using 15 fs pulses from a Ti:sapphire oscillator tuned to 800 nm wavelength. The measured harmonic-generation efficiencies are 2.6·10 −9 , 8·10 −9 and 1.3·10 −8 for left-handed circular, linear, and right-handed circular polarizations, respectively. The uncoated nanospirals are stable under average power loading of as much as 300 µW per nanoparticle. The nanospirals also exhibit selective conversion between polarization states. These experiments show that the intrinsic asymmetry of the nanospirals results in a highly efficient, two-dimensional harmonic generator that can be incorporated into metasurface optics.Keywords: nonlinear plasmonics, asymmetric nanoparticles, polarization conversion, metasurfaces, near-field enhancement, Archimedean nanospirals The second-order susceptibility governs a host of important nonlinear optical phenomena, including frequency mixing, sum-frequency and harmonic generation, and optical rectification. In crystalline and molecular materials, second-order nonlinearities are nonvanishing only at surfaces or in materials with a noncentrosymmetric crystal structure; moreover, the efficient generation of a second-order nonlinear effect requires that the fundamental incident and the nonlinear outgoing waves be phase matched through a macroscopic volume of material, typically on the order of cubic millimeters [1].Plasmonic nanostructures and nanostructure arrays also exhibit second-order nonlinearities, and can generate forward second harmonics if their geometries are not centrosymmetric. Such structures are inherently planar, and therefore compatible with thin-film optical and optoelectronic technologies and with metasurface optics. With advances in nanofabrication, the symmetry of the structures can be exquisitely controlled at the level of a few nanometers [2]. Combining these effects with ultrafast, high-intensity laser pulses yields massive electricfield enhancements and correspondingly greater secondharmonic yield. The localized surface plasmon resonance enhances efficiency and can be designed by selecting the nanoparticle shape for a given wavelength; selective polarization response can also be designed into the nanoparticle. A number of asymmetric plasmonic geometries have been used for harmonic generation, including L-and V-shaped nanoparticles, nanocups, and asymmetric trimers [3][4][5][6][7]. Larger plasmonic structures-such as the ratchet wheel-have also been shown to affect the polarization o...

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“…Recently, advances of nanofabrication techniques [7,8] have enabled control of the sizes, shapes, and alignment of nanostructures of a wide range of materials, and their SHG responses have been investigated. For example, the reports for SHG responses from the GaAs nanoneedles grown by the chemical vapor deposition method [9], the nanocups deposited Au by electron-beam evaporation on to silica nanoparticles [10], the ZnO nanorods grown on glass substrates by means of the low-temperature chemical bath method [11], the Pt nanowires created by the physical vapor deposition method [12], and the Au nanoholes fabricated by the focused ion beam method [13] attracted most researchers. These SHG processes are used in a wide range of applications, such as developing devices for optical processing [14], nonlinear imaging [4], and phase-sensitive amplification [15].…”

Section: Introductionmentioning

confidence: 99%

Nonlinear optics on nano/micro-hierarchical structures on metals: focus on symmetric and plasmonic effects

Ogata

Guo

2017

Nano Reviews & Experiments

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In this review, the authors study their creation of nano/micro-hierarchical structures on Ag and Ni substrates by femtosecond laser treatment and their investigation of their optical second-harmonic generation (SHG) signal intensities by SHG spectroscopy. The authors obtained the nanostructure-covered microgroove and microcube structures. These hierarchical surface structures were found to modify significantly the optical nonlinearity of the metal surfaces. The macroscopic symmetry of the surface’s shapes influenced SHG, and the excitation of surface plasmons enhanced SHG. On the other hand, the nanostructures on the microstructures had an additional effect on the generated SHG. For the microcube structures, the additional SHG emission was suppressed by removing a large amount of nanostructures. Left SHG was discussed by the effect of the propagating delay.

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Three-Dimensional Nanostructures as Highly Efficient Generators of Second Harmonic Light

Cited by 283 publications

References 34 publications

Coherent Fano resonances in a plasmonic nanocluster enhance optical four-wave mixing

Coherent Fano resonances in a plasmonic nanocluster enhance optical four-wave mixing

Efficient forward second-harmonic generation from planar archimedean nanospirals

Nonlinear optics on nano/micro-hierarchical structures on metals: focus on symmetric and plasmonic effects

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