Enhanced optical Kerr effect method for a detailed characterization of the third-order nonlinearity of two-dimensional materials applied to graphene

Dremetsika, Evdokia; Kockaert, Pascal

doi:10.1103/physrevb.96.235422

Cited by 21 publications

(18 citation statements)

References 33 publications

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“…These early works have greatly promoted the exploration of graphene-based nonlinear optics. [99][100][101][102][103][104] Based on the successful exploration of the nonlinear properties of graphene and its derivatives, researchers began to study other 2D materials, such as topological insulators, layered TMDCs, black phosphorus, and MXenes. Among them, topological insulators including Bi 2 Se 3 , Bi 2 Te 3 , and Sb 2 Te 3 , characterized by a robust metallic edge or surface state and a narrow band-gap bulk insulating state, have gained great attention in the field of physics, chemistry, and material.…”

Section: Third-order Optical Propertiesmentioning

confidence: 99%

2D Layered Materials: Synthesis, Nonlinear Optical Properties, and Device Applications

Guo

Xiao

Wang

et al. 2019

Laser & Photonics Reviews

421

197

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In recent years, 2D layered materials, including graphene, topological insulators, transition metal dichalcogenides, black phosphorus, MXenes, graphitic carbon nitride, and metal‐organic frameworks, have attracted considerable interest due to their potential applications in the fields of physics, chemistry, biology, and energy. Their rise in the field of nonlinear photonics began around 2009 and has become an important research direction. Here, the synthesis techniques, nonlinear optical properties, integration strategies, and device applications of layered materials are reviewed. In terms of nonlinear optical properties, the focus is on saturable absorption and Kerr nonlinearity. On this basis, their applications in various pulsed lasers, including fiber lasers, solid‐state lasers, waveguide lasers, and related nonlinear optical phenomenon, are summarized. In addition, novel optical devices using layered materials, such as optical modulators, optical polarizers, optical switchers, and even all‐optical device, are also involved. It is believed that the development of 2D layered materials in the field of photonics will continue to deepen, thus laying a good foundation for its practical application.

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Section: Third-order Optical Propertiesmentioning

confidence: 99%

2D Layered Materials: Synthesis, Nonlinear Optical Properties, and Device Applications

Guo

Xiao

Wang

et al. 2019

Laser & Photonics Reviews

421

197

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“…Experimentally demonstrated third‐order susceptibilities from the NIR to the THz range. Susceptibilities from the following references are plotted over the wavelength of the exciting light pulses: [a] Dremetsika and Kockaert, [b] Kumar et al, [c] Soavi et al, [d] Hendry et al, [e] Kundys et al, [f] König‐Otto et al (Landau‐quantized graphene in a magnetic field), and [g] Hafez et al Whereas in the NIR (left), the nonlinearity mechanism is typically associated with coherent electron dynamics, in the THz (right) the mechanism is noncoherent and thermal. For intermediate wavelengths, different mechanisms have been proposed, such as plasmon nonlocal effects [e], and thermally induced plasmon shifts (no susceptibility quoted).…”

Section: Terahertz Nonlinear Interactions In Graphenementioning

confidence: 99%

Terahertz Nonlinear Optics of Graphene: From Saturable Absorption to High‐Harmonics Generation

Hafez

Kovalev

Tielrooij

et al. 2019

Advanced Optical Materials

126

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visible light frequencies, corresponding to interband transitions leading to electron-hole pair generation. [5,6,12] In the case of doped graphene, that is, graphene containing a certain concentration of free electrons or holes, Drude-like conductivity was observed at far-infrared and terahertz (THz) frequencies, corresponding to intraband free-carrier absorption. [8,9,[12][13][14][15] Further, theoretical studies predicted strong nonlinear interaction of graphene with intense light fields, in particular at the technologically important THz frequencies (typically, in the range 0.1-10 THz), [16][17][18][19][20][21][22][23][24][25] as originating from both interband and intraband electron dynamics. These predictions were inspired by the unique band structure of graphene: absence of a bandgap and linear energy-momentum dispersion for its electrons. [2,3,[26][27][28] A plethora of strong nonlinear effects in graphene in the IR and optical frequency ranges, originating from interband electron dynamics, was successfully demonstrated, including saturable absorption and nonlinear refraction, [29][30][31][32][33][34][35][36][37][38][39] higherharmonic generation, [40][41][42][43][44][45][46][47] and wave-mixing processes [48][49][50] (see also reviews [51][52][53] ). At THz frequencies, however, until recently only saturable absorption effects in doped graphene, [54][55][56][57][58][59][60][61] and induced multiphoton-like absorption in multilayer near-intrinsic graphene were successfully demonstrated. [62] At the same time, the observation of the long sought-after effect of THz higher-order harmonics generation, Graphene has long been predicted to show exceptional nonlinear optical properties, especially in the technologically important terahertz (THz) frequency range. Recent experiments have shown that this atomically thin material indeed exhibits possibly the largest nonlinear coefficients of any material known to date, paving the way for practical graphene-based applications in ultrafast (opto-)electronics operating at THz rates. Here the advances in the booming field of nonlinear THz optics of graphene are reported, and the state-of-the-art understanding of the nature of the nonlinear interaction of graphene with the THz fields based on the thermodynamic model of electron transport in graphene is described. A comparison between different mechanisms of nonlinear interaction of graphene with light fields in THz, infrared, and visible frequency ranges is also provided. Finally, the perspectives for the expected technological applications of graphene based on its extraordinary THz nonlinear properties are summarized. This report covers the evolution of the field of THz nonlinear optics of graphene from the very pioneering to the state-of-the-art works. It also serves as a concise overview of the current understanding of THz nonlinear optics of graphene and as a compact reference for researchers entering the field, as well as for the technology developers.

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“…Over the past several years numerous experiments have been carried out to study the response of graphene in parametric nonlinear-optical processes like four-wave mixing 1 – 5 , third-harmonic generation 6 , 7 , self-(de)focusing 8 – 12 , and self-phase modulation (SPM) 13 – 15 . These measurements mostly pointed at an extremely high effective third-order susceptibility in the 2D material, much higher than what theory predicts for graphene’s electronic third-order susceptibility 16 – 19 in the density-matrix framework at the single-particle level 20 , 21 .…”

Section: Introductionmentioning

confidence: 99%

Graphene’s nonlinear-optical physics revealed through exponentially growing self-phase modulation

Vermeulen¹,

Castelló‐Lurbe²,

Khoder³

et al. 2018

Nat Commun

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Graphene is considered a record-performance nonlinear-optical material on the basis of numerous experiments. The observed strong nonlinear response ascribed to the refractive part of graphene’s electronic third-order susceptibility χ(3) cannot, however, be explained using the relatively modest χ(3) value theoretically predicted for the 2D material. Here we solve this long-standing paradox and demonstrate that, rather than χ(3)-based refraction, a complex phenomenon which we call saturable photoexcited-carrier refraction is at the heart of nonlinear-optical interactions in graphene such as self-phase modulation. Saturable photoexcited-carrier refraction is found to enable self-phase modulation of picosecond optical pulses with exponential-like bandwidth growth along graphene-covered waveguides. Our theory allows explanation of these extraordinary experimental results both qualitatively and quantitatively. It also supports the graphene nonlinearities measured in previous self-phase modulation and self-(de)focusing (Z-scan) experiments. This work signifies a paradigm shift in the understanding of 2D-material nonlinearities and finally enables their full exploitation in next-generation nonlinear-optical devices.

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Enhanced optical Kerr effect method for a detailed characterization of the third-order nonlinearity of two-dimensional materials applied to graphene

Cited by 21 publications

References 33 publications

2D Layered Materials: Synthesis, Nonlinear Optical Properties, and Device Applications

2D Layered Materials: Synthesis, Nonlinear Optical Properties, and Device Applications

Terahertz Nonlinear Optics of Graphene: From Saturable Absorption to High‐Harmonics Generation

Graphene’s nonlinear-optical physics revealed through exponentially growing self-phase modulation

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