Optical Second Harmonic Generation in Plasmonic Nanostructures: From Fundamental Principles to Advanced Applications

Butet, Jérémy; Brevet, Pierre‐François; Martin, Olivier J. F.

doi:10.1021/acsnano.5b04373

Cited by 496 publications

(487 citation statements)

References 211 publications

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“…Plasmon excitations in conducting nanostructures concentrate electromagnetic energy into spatial regions commensurate with the structure size, enabling control over light-matter interactions on the nanoscale for diverse applications including optical sensing [1,2], photovoltaics [3,4], and nonlinear optics [5,6]. In this context, highly doped graphene has emerged as an attractive plasmonic material capable of supporting long-lived and electrically tunable collective excitations that can boost light absorption well beyond the intrinsic broadband 2.3% level in pristine samples [7,8].…”

Section: Introductionmentioning

confidence: 99%

Transient nonlinear plasmonics in nanostructured graphene

Cox¹,

Abajo²

2018

Optica

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Plasmons in highly doped graphene offer the means to dramatically enhance light absorption in the atomically thin material. Ultimately the absorbed light energy induces an increase in electron temperature, accompanied by large shifts in the chemical potential. This intrinsically incoherent effect leads to strong intensity-dependent modifications of the optical response, complementing the remarkable coherent nonlinearities arising in graphene due to interband transitions and anharmonic intraband electron motion. Through rigorous time-domain quantum-mechanical simulations of graphene nanoribbons, we show that the incoherent mechanism dominates over the coherent response for the high levels of intensity required to trigger nonperturbative optical phenomena such as saturable absorption. We anticipate that these findings will elucidate the role of coherent and incoherent nonlinearities for future studies and applications of plasmon-assisted nonlinear optics.

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Section: Introductionmentioning

confidence: 99%

Transient nonlinear plasmonics in nanostructured graphene

Cox¹,

Abajo²

2018

Optica

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“…[10][11][12] Bulk metals, thin metal layers, and plasmonic metamaterials have been investigated in the nonlinear regime. [13][14][15] The nonlinear propagation of surface plasmon polaritons (SPPs) in plasmonic waveguides can be studied in terms of either the second-order nonlinearity, 16,17 or the third-order nonlinearity. 18,19 The latter is particularly important because it is present in all materials.…”

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confidence: 99%

Nonlinear Dynamics of Ultrashort Long-Range Surface Plasmon Polariton Pulses in Gold Strip Waveguides

et al. 2016

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We study experimentally and theoretically nonlinear propagation of ultrashort long-range surface plasmon polaritons in gold strip waveguides. The nonlinear absorption of the plasmonic modes in the waveguides is measured with femtosecond pulses revealing a strong dependence of the third-order nonlinear susceptibility of the gold core on the pulse duration and layer thickness. A comprehensive model for the pulse duration dependence of the third-order nonlinear susceptibility is developed on the basis of the nonlinear Schrödinger equation for plasmonic mode propagation in the waveguides. The model accounts for the intrinsic delayed (noninstantaneous) nonlinearity of free electrons of gold as well as the thickness of the gold film, and is experimentally verified. The obtained results are important for the development of active plasmonic and nanophotonic components. 2Plasmonic nanostructures represent a unique platform for many linear and nonlinear optical applications. 1 A great variety of plasmonic waveguides for integrated optics, 2,3 nanofocusing, 4,5 sensing, 6,7 lasing and amplification of light 8,9 has been proposed. In particular, special attention has recently been paid to the nonlinear optical properties of plasmonic waveguides, hybrid plasmonic waveguides, and other elements important for future nanophotonic communication approaches. [10][11][12] Bulk metals, thin metal layers, and plasmonic metamaterials have been investigated in the nonlinear regime. [13][14][15] The nonlinear propagation of surface plasmon polaritons (SPPs) in plasmonic waveguides can be studied in terms of either the second-order nonlinearity, 16,17 or the third-order nonlinearity. 18,19 The latter is particularly important because it is present in all materials. In metals, it mainly arises due to hot-electron contributions from changes of the intrinsic electronic temperature after absorption of the incident light. Typically, the electron relaxation time in noble metals is on the few-picosecond scale, 18,19 implying that their nonlinear susceptibility can depend on the laser pulse duration if it is shorter than or comparable with the electron relaxation time. 20 The majority of the experimental data on the third-order nonlinear susceptibility of gold were collected near the interband transitions in a wavelength range of 532-630 nm for pulse durations between 100 fs and 1 ns. 20 Most results were obtained with the z-scan method, reporting very high values of the third-order susceptibility in the range of 10 -16 -10 -15 m 2 /V 2 . [21][22][23][24] However, the linear propagation losses of SPPs in Au-based waveguides, which are also related to the same interband transitions, are very high (~30-40 dB/mm) in this wavelength range. 25 On the other hand, nanophotonic and plasmonic devices are extensively exploited in the infrared (IR) wavelength range. 2,3 The propagation losses of long-range SPPs (LRSPPs) in Au-based waveguides can be ~2-5 dB/mm at the telecommunication wavelengths. 25 Meanwhile, the third-3 order susceptibility of...

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“…They therefore provide efficient means to control of the nanoscale optical response, enabling efficient tuning of directional scattering, 14 Fano interferences, 65 molecular sensing 66 and multiple bright resonances for broadband fluorescence enhancement, 67 as well as second harmonic generation. 68 …”

Section: Discussionmentioning

confidence: 99%

Mode Coupling in Plasmonic Heterodimers Probed with Electron Energy Loss Spectroscopy

et al. 2017

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While plasmonic antennas composed of building blocks made of the same material have been thoroughly studied, recent investigations have highlighted the unique opportunities enabled by making compositionally asymmetric plasmonic systems. So far, mainly heterostructures composed of nanospheres and nanodiscs have been investigated, revealing opportunities for the design of Fano resonant nanostructures, directional scattering, sensing and catalytic applications. In this article, an improved fabrication method is reported that enables precise tuning of the heterodimer geometry, with interparticle distances made down to a few nanometers between Au−Ag and Au−Al nanoparticles. A wide range of mode energy detuning and coupling conditions are observed by near field hyperspectral imaging performed with electron energy loss spectroscopy, supported by full wave analysis numerical simulations. These results provide direct insights into the mode hybridization of plasmonic heterodimers, pointing out the influence of each dimer constituent in the overall electromagnetic response. By relating the coupling of nondipolar modes and plasmon−interband interaction with the dimer geometry, this work facilitates the development of plasmonic heterostructures with tailored responses, beyond the possibilities offered by homodimers. KEYWORDS: optical nanoantennas, plasmonic heterostructures, bimetallic antennas, electron energy loss spectroscopy, electron beam lithography, eigenmodes C ollective oscillations of the conduction electrons in metal nanostructures, known as localized surface plasmon resonances, 1 have been intensively studied and designed by manipulating both the nanostructures size and geometry, as well as their dielectric environment.2 These investigations, carried out over the entire visible light spectrum, including the near-UV and near-IR, have demonstrated the control of both nanoscale optical fields and far field radiation, 1 leading to the concept of optical nanoantennas.2,3 The electromagnetic properties of these structures are governed by their eigenmodes, ranging from dipoles to high order multipoles. 4,5 When the nanoparticles are arranged in pairs or multimers, these modes couple to each other and hybridize, producing further optical properties. 6−8 In the simplest and most common geometry, involving the coupling of two selfsimilar spherical nanoparticles separated by a nanogap, a wellknown dipole−dipole interaction along the dimer axis is produced. 6 This coupling generates an intense and confined near field in the gap region, which can enable large nanoscale fluorescence enhancement 9 and surface enhanced Raman scattering down to the single molecule level. 10,11 Thanks to a complete description of the plasmonic coupling for spherical self-similar nanoparticle dimers, Nordlander and coauthors 7 have shown that the gap dependent hybridization in such nanostructures stems from the interaction of the uncoupled eigenmodes. Specifically, the uncoupled modes hybridize with bonding and antibonding interactions a...

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Optical Second Harmonic Generation in Plasmonic Nanostructures: From Fundamental Principles to Advanced Applications

Cited by 496 publications

References 211 publications

Transient nonlinear plasmonics in nanostructured graphene

Transient nonlinear plasmonics in nanostructured graphene

Nonlinear Dynamics of Ultrashort Long-Range Surface Plasmon Polariton Pulses in Gold Strip Waveguides

Mode Coupling in Plasmonic Heterodimers Probed with Electron Energy Loss Spectroscopy

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