Ultrafast Optical Modulation of Second- and Third-Harmonic Generation from Cut-Disk-Based Metasurfaces

Sartorello, Giovanni; Olivier, Nicolas; Zhang, Jingjing; Yue, Weisheng; Gosztola, David J.; Wiederrecht, Gary P.; Wurtz, Gregory A.; Zayats, Anatoly V.

doi:10.1021/acsphotonics.6b00108

Cited by 75 publications

(59 citation statements)

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“…In fact, THG benefits from the resonantlyenhanced volume currents in plasmonic nanoantennas at visible wavelengths, a process typically modeled by considering the bulk χ (3) material nonlinear susceptibility. [12][13][14][15][16] On the contrary, SHG is strictly forbidden in the bulk of centrosymmetric materials, such as those usually employed in plasmonics (Au, Ag, Al), where SHG is due to surface-related processes stemming from the removal of inversion symmetry associated with the metal/environment interface [17][18][19][20][21][22][23][24] or due to strong field gradients and nonlocal effects. 17,18 Such SHG mechanisms are typically described by an effective surface χ (2) nonlinear susceptibility, 4 The mechanisms at the basis of THG in metal nanostructures are still largely debated, [25][26][27] since the driving fields are strongly nonuniform within the skin depth inside the material and retardation effects might play a fundamental role.…”

Section: Textmentioning

confidence: 99%

“…49,50 The presence of cascaded effects in THG seeded by SFG in plasmonic nanoantennas has been neglected in the literature thus far because of the large difference often reported between the SHG and THG emission yields. However, sizeable SFG has been recently reported for some specific plasmonic nanostructures 15 and the optimization of SFG through intrapulse phase engineering has been exploited to maximize SHG in plasmonic nanoantennas. 47 Here we tentatively consider a surface Fig.…”

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Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas

et al. 2019

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The optimization of nonlinear optical processes at the nanoscale is a crucial step for the integration of complex functionalities into compact photonic devices and metasurfaces. In such systems, photon upconversion can be achieved with high efficiencies via third-order processes, such as third harmonic generation (THG), thanks to the resonantly enhanced volume currents. Conversely, second-order processes, such as second harmonic generation (SHG), are often inhibited by the symmetry of metal lattices and of common nanoantenna geometries. SHG and THG processes in plasmonic nanostructures are generally treated independently, since they typically represent small perturbations in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold for plasmon-enhanced nonlinear optics, by providing evidence of a sum frequency generation process seeded by SHG, which sizably contributes to the overall THG yield.We address this mechanism by unveiling a characteristic fingerprint in the polarization state of the THG emission from non-centrosymmetric gold nanoantennas, which directly reflects the asymmetric distribution of second harmonic fields within the structure and does not depend on the model one employ to describe photon upconversion. We suggest that such cascaded processes may also appear for structures that exhibit only moderate SHG yields. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows gaining further insight on the physics of plasmon-enhanced nonlinear optical processes. This could be crucial in the realization of nanoscale elements for photon conversion and manipulation operating at room-temperature.

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Section: Textmentioning

confidence: 99%

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Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas

et al. 2019

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“…Finally, not only linear, but also nonlinear properties of plasmonic nanostructures can be controlled via Kerr nonlinearity in metal on an ultra‐fast timescale. The all‐optical control of SHG and THG from cut‐disk‐based metasurfaces was experimentally realised showing significant variation of SHG intensity (up to 20%) with control light illumination ( Figure ) …”

Section: Kerr‐type Nonlinearity and Ultrafast Nonlinear Plasmonicsmentioning

confidence: 99%

Section: Kerr‐type Nonlinearity and Ultrafast Nonlinear Plasmonicsmentioning

confidence: 99%

Free‐electron Optical Nonlinearities in Plasmonic Nanostructures: A Review of the Hydrodynamic Description

Krasavin

Ginzburg

Zayats

2017

Laser & Photonics Reviews

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Requirements of integrated photonics and miniaturisation of optical devices demand efficient nonlinear components not constrained by conventional macroscopic nonlinear crystals. Intrinsic nonlinear response of free carriers in plasmonic materials provides opportunities to design both second-and third-order nonlinear optical properties of plasmonic nanostructures and control light with light using Kerr-type nonlinearities as well as achieve harmonic generation. This review summarises principles of free-carrier nonlinearities in the hydrodynamic description in both perturbative and non-perturbative regimes, considering also contribution of nonlocal effects. Engineering of harmonic generation, solitons, nonlinear refraction and ultrafast all-optical switching in plasmonic nanostructures and metamaterials are discussed. The full hydrodynamic consideration of nonlinear dynamics of free carriers reveals key contributions to the nonlinear effects defined by the interplay between a topology of the nanostructure and nonlinear response of the fermionic gas at the nanoscale, allowing design of high effective nonlinearities in a desired spectral range. Flexibility and unique features of free-electron nonlinearities are important for nonlinear plasmonic applications in free-space as well as integrated and quantum nanophotonic technologies.

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“…The recent burgeoning topological metasurfaces provide another optical dimension, which take advantage of topology to realize robust optical transmission, and other novel phenomena in energy band . Moreover, instantaneous, ultrafast, and active manipulation of optical field in nanosecond or femtosecond is another dimension that characterizes time evolution instead of the steady states to explore the light–matter interaction . Due to the development of nanofabrication techniques, quantum entanglement realized by metasurfaces has drawn much attention of researchers, which may greatly boost the exploitation of the quantum photonics.…”

Section: Discussionmentioning

confidence: 99%

From Single‐Dimensional to Multidimensional Manipulation of Optical Waves with Metasurfaces

et al. 2019

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given refractive indices. The limited refractive indices of natural materials prevent the generation of new optical phenomena. The size and weight of traditional optical devices also prevent optical system miniaturization and integration. Nowadays, there is an everincreasing demand for new approaches to implement the effective manipulation of optical waves in different dimensions and to get the novel optical devices on demand.With the development of nanofabrication technology, artificial nanostructures become approachable which offer a promising solution to the achievement of efficient manipulation of optical waves in different dimensions. Metamaterials, which attain their optical functionalities from the subwavelength structures rather than their constitutive materials, provided intriguing possibilities for the evolution of modern optics and have attracted great interest from the scientific community over the past twenty years. [1][2][3] By judiciously modulating their subwavelength structure parameters, the effective values of the permeability and permittivity of the metamaterials can be designed on purpose to realize the manipulation of optical waves in a spectific dimension and to get the desirable optical functionalities, which are even not achievable with natural materials. Previous works have demonstrated that metamaterials can be widely applied in realizing negative refractive index, [4][5][6] electromagnetic invisibility cloaks, [7,8] optical black holes, [9] chiral media, [10,11] and so on. However, the commercialization of metamaterial-based optical devices in real applications is still challenging, which we ascribe to the strong dispersion and high losses associated with typically used metallic structures, and also the difficult and costly fabrication for 3D designs.Recently, planar metamaterials or metasurfaces have received great attention for their advantages to meet these challenges. [12][13][14] Compared to metamaterials, metasurfaces, as artificial planar designs, have dramatically reduced the fabrication complexity. Moreover, the thickness of metasurfaces is less than or similar to the wavelength of operating waves, which results in the reduction of the undesirable losses and offers an effective manner for implementing tunable and reconfigurable optical devices. Overall, metasurfaces provide an effective way to overcome the challenges in metamaterials, and it has been successfully proven that metasurfaces are more feasible for the engineering of the fundamental dimensions of optical Metasurfaces, 2D artificial arrays of subwavelength elements, have attracted great interest from the optical scientific community in recent years because they provide versatile possibilities for the manipulation of optical waves and promise an effective way for miniaturization and integration of optical devices. In the past decade, the main efforts were focused on the realization of single-dimensional (amplitude, frequency, polarization, or phase) manipulation of optical waves. Compared to the metasurfaces with sing...

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Ultrafast Optical Modulation of Second- and Third-Harmonic Generation from Cut-Disk-Based Metasurfaces

Cited by 75 publications

References 42 publications

Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas

Evidence of Cascaded Third-Harmonic Generation in Noncentrosymmetric Gold Nanoantennas

Free‐electron Optical Nonlinearities in Plasmonic Nanostructures: A Review of the Hydrodynamic Description

From Single‐Dimensional to Multidimensional Manipulation of Optical Waves with Metasurfaces

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