Giant Nonlinearity Research Articles

Giant nonlinear optical wave mixing in a van der Waals correlated insulator.

Optical nonlinearities are one of the most fascinating properties of two-dimensional (2D) materials. While tremendous efforts have been made to find and optimize the second-order optical nonlinearity in enormous 2D materials, opportunities to explore higher-order ones are elusive because of the much lower efficiency. Here, we report the giant high odd-order optical nonlinearities in centrosymmetric correlated van der Waals insulator manganese phosphorus triselenide. When illuminated by two near-infrared femtosecond lasers, the sample generates a series of profound four- and six-wave mixing outputs. The near-infrared third-order nonlinear susceptibility reaches near the highest record values of 2D materials. Comparative measurements to other prototypical nonlinear optical materials [lithium niobate, gallium(II) selenide, and tungsten disulfide] reveal its extraordinary wave mixing efficiency. The wave mixing processes are further used for nonlinear optical waveguide with multicolor emission. Our work highlights the promising prospect for future research of the nonlinear light-matter interactions in the correlated 2D system and for potential nonlinear photonic applications.

Tunable Intracavity Coherent Up-Conversion with Giant Nonlinearity in a Polar Fluidic Medium.

The study has demonstrated a novel microcavity-based flexible photon up-conversion system using second harmonic generation (SHG) from a polar nematic fluidic medium doped with a laser dye. The idea is based on coherent light generation via stimulated emission (lasing) and simultaneous frequency doubling inside a microcavity. The polar nematic fluid equips very high even-order optical nonlinearity due to its polar symmetry and large dipole moment along the molecular long axis. At the same time, its inherent fluidic nature allows to easily functionalize the media just by doping, in the present case, with an emissive laser dye. The demonstrated system exhibits a giant nonlinear optical response to input light, while enabling spectral narrowing and multiple-signal output of up-converted light, which is not attainable through the simple SH-conversion of input light. Furthermore, the susceptibility of the liquid crystal offers dynamic modulation capabilities by an external stimulus, such as signal switching by the application of electric field or wavelength tuning through temperature variation. Such a brand-new type of simple coherent flexible up-conversion system must be promising as a new principle for easily accessible and down-scalable wavelength conversion devices.

Unlocking Giant Third-Order Optical Nonlinearity in (MA)2CuX4 through Introducing Jahn-Teller Distortion.

Nonlinear absorption coefficient and modulation depth stand as pivotal properties of nonlinear optical (NLO) materials, while the existing NLO materials exhibit limitations such as low nonlinear absorption coefficients and/or small modulation depths, thereby severely impeding their practical application. Here we unveil that introducing Jahn-Teller distortion in a Mott-Hubbard system, (MA)2CuX4 (MA=methylammonium; X=Cl, Br) affords the simultaneous attainment of a giant nonlinear absorption coefficient and substantial modulation depth. The optimized compound, (MA)2CuCl4, demonstrates a nonlinear absorption coefficient of (1.5±0.08)×105 cm GW-1, a modulation depth of 60 %, and a relatively low optical limiting threshold of 1.22×10-5 J cm-2. These outstanding attributes surpass those of most reported NLO materials. Our investigation reveals that a more pronounced distortion of the [CuX6]4- octahedron emerges as a crucial factor in augmenting optical nonlinearity. Mechanism study involving structural and spectral characterization along with theoretical calculations indicates a correlation between the compelling performance and the Mott-Hubbard band structure of the materials, coupled with the Jahn-Teller distortion-induced d-d transition. This study not only introduces a promising category of high-performance NLO materials but also provides novel insights into enhancing the performance of such materials.

Giant Optical Nonlinear Response up to 60th‐Order Induced by the Ytterbium Energy Relay Mediated Photon Avalanches

AbstractThe exploration of photon avalanching (PA) luminescence in different lanthanide emitters has profound implications in plentiful frontier applications. However, studies for universal mechanisms at the nanoscale to exhibit giant nonlinear responses in various avalanching emitters are limited. Here, record‐breaking nonlinear responses up to 60th‐order in high‐lying emitting levels of various emitters at room temperature are generated by proposing a universal mechanism named energy relay‐mediated photon avalanche (enrePA). By harnessing energy from the avalanching nano‐engine through the energy relay of Yb3+ ions, the brightness of blue emissions from Tm3+ and Ho3+ can be enhanced with giant optical nonlinearity up to 60th and 38th order, respectively. Further incorporating gadolinium‐based systems, more emitters (Tb3+, Eu3+, Dy3+, Nd3+) can be activated with extreme optical nonlinearities up to 48th‐order. By expanding PA into the full‐spectrum range, the enrePA mechanism opens exciting avenues for flexible and high‐efficiency PA modulation in multilayer nanostructures, enabling the applicability of PA in more technologies such as super‐resolution imaging, lithography, and optical detection.

High-Order Nonlinear Electrophoresis in a Nematic Liquid Crystal.

Electrophoresis is the motion of particles relative to a surrounding fluid driven by a uniform electric field. In conventional electrophoresis, the electrophoretic velocity grows linearly with the applied field. Nonlinear effects with a quadratic speed vs field dependence are gaining research interest since an alternating current field could drive them. Here, we report on the giant nonlinearity of electrophoresis in a nematic liquid crystal in which the speed grows with the fourth and sixth powers of the electric field. The mechanism is attributed to the shear thinning of the nematic environment induced by the moving colloid. The observed giant nonlinear effect dramatically enhances the efficiency of electrophoretic transport.

2D Memory Selectors with Giant Nonlinearity Enabled by Van der Waals Heterostructures.

The integration of one-selector-one-resistor crossbar arrays requires the selectors featured with high nonlinearity and bipolarity to prevent leakage currents and any crosstalk among distinct cells. However, a selector with sufficient nonlinearity especially in the frame of device miniaturization remains scarce, restricting the advance of high-density storage devices. Herein, a high-performance memory selector is reported by constructing a graphene/hBN/WSe2 heterostructure. Within the temperature range of 300-80K, the nonlinearity of this selector varies from ≈103-≈104 under forward bias, and increases from ≈300-≈105 under reverse bias, the highest reported nonlinearity among 2D selectors. This improvement is ascribed to direct tunneling at low bias and Fowler-Nordheim tunneling at high bias. The tunneling current versus voltage curves exhibit excellent bipolarity behavior because of the comparable hole and electron tunneling barriers, and the charge transport polarity can be effectively tuned from N-type or P-type to bipolar by simply changing source-drain bias. In addition, the conceptual memory selector exhibits no sign of deterioration after 70000 switching cycles, paving the way for assembling 2D selectors into modern memory devices.

Colossal Kerr nonlinearity without absorption in a five-level atomic medium

In this work, we present an analytical method to achieve giant Kerr nonlinearity without absorption in a five-level atomic medium. By using iterative perturbation technique on density matrix equations, we have derived the analytical expressions of nonlinear susceptibility and Kerr nonlinear coefficient in the presence of spontaneously generated coherence (SGC) and relative phase between applied laser fields. It shows that, this five-level atomic medium exhibits multiple electromagnetically induced transparency (EIT) at three different frequencies, at the same time, the Kerr nonlinear coefficient is enhanced around three transparent spectral regions; in each such EIT region appears a pair of positive–negative peaks of Kerr nonlinear coefficient. In particular, these nonlinear peaks are moved to the center of the EIT windows via SGC. This means that the Kerr nonlinear coefficient is enhanced with completely suppressed absorption at different transparency frequencies. Furthermore, the magnitude and the sign of the Kerr nonlinear coefficient are easily controlled according to the SGC strength, the coupling laser intensity, and the relative phase between applied laser fields. Such a giant nonlinear medium can be useful for photonic devices working in the resonant frequency region without absorption. As a typical application, this giant Kerr nonlinear material has been applied to an interferometer for the formation of optical bistability, and showed the appearance of OB at the resonant frequency with significantly reduced threshold intensity and OB width.

Lanthanide-Doped KMgF3 Upconversion Nanoparticles for Photon Avalanche Luminescence with Giant Nonlinearities.

Lanthanide (Ln3+)-doped photon avalanche (PA) upconversion nanoparticles (UCNPs) have great prospects in many advanced technologies; however, realizing efficient PA luminescence in Ln3+-doped UCNPs remains challenging due to the deleterious surface and lattice quenching effect. Herein, we report a unique strategy based on the pyrolysis of KHF2 for the controlled synthesis of aliovalent Ln3+-doped KMgF3 UCNPs, which can effectively protect Ln3+ from luminescence quenching by surface and internal OH- defects and thereby boost upconversion luminescence. This enables us to realize efficient PA luminescence from Tm3+ at 802 nm in KMgF3: Tm3+ UCNPs upon 1064 nm excitation, with a giant nonlinearity of ∼27, a PA response time of 281 ms, and an excitation threshold of 16.6 kW cm-2. This work may open up a new avenue for exploring highly nonlinear PA luminescence through aliovalent Ln3+ doping and crystal lattice engineering toward diverse emerging applications.

Giant room-temperature nonlinearities in a monolayer Janus topological semiconductor

Nonlinear optical materials possess wide applications, ranging from terahertz and mid-infrared detection to energy harvesting. Recently, the correlations between nonlinear optical responses and certain topological properties, such as the Berry curvature and the quantum metric tensor, have attracted considerable interest. Here, we report giant room-temperature nonlinearities in non-centrosymmetric two-dimensional topological materials—the Janus transition metal dichalcogenides in the 1 T’ phase, synthesized by an advanced atomic-layer substitution method. High harmonic generation, terahertz emission spectroscopy, and second harmonic generation measurements consistently show orders-of-the-magnitude enhancement in terahertz-frequency nonlinearities in 1 T’ MoSSe (e.g., > 50 times higher than 2H MoS2 for 18th order harmonic generation; > 20 times higher than 2H MoS2 for terahertz emission). We link this giant nonlinear optical response to topological band mixing and strong inversion symmetry breaking due to the Janus structure. Our work defines general protocols for designing materials with large nonlinearities and heralds the applications of topological materials in optoelectronics down to the monolayer limit.

Investigation of Giant Nonlinearity in a Plasmonic Metasurface with Epsilon-Near-Zero Film

Plasmonic metamaterials can exhibit a variety of physical optical properties that offer extraordinary nonlinear conversion efficiency for ultra-compact nanodevice applications. Furthermore, the optical-rectification effect from the plasmonic nonlinear metasurfaces (NLMSs) can be used as a compact source of deep-subwavelength thickness to radiate broadband terahertz (THz) signals. Meanwhile, a novel dual-mode metasurface consisting of a split-ring resonator (SRR) array and an epsilon-near-zero (ENZ) layer was presented to boost the THz conversion efficiency further. In this paper, to explore the mechanism of THz generation from plasmonic NLMSs, the Maxwell-hydrodynamic multiphysics model is adopted to investigate complex linear and intrinsic nonlinear dynamics in plasmonics. We solve the multiphysics model using the finite-difference time-domain (FDTD) method, and the numerical results demonstrate the physical mechanism of the THz generation processes which cannot be observed in our previous experiments directly. The proposed method reveals a new approach for developing new types of high-conversion-efficiency nonlinear nanodevices.

Giant cross-Kerr nonlinearity in the metal nanoparticles-graphene nanodisks-quantum dots hybrid system with low light intensity for photovoltaic devices

Giant cross-Kerr nonlinearity in the metal nanoparticles-graphene nanodisks-quantum dots hybrid system with low light intensity for photovoltaic devices

Controlling water giant low-inertia nonlinear refractive index in the THz frequency range via temperature variation.

To create self-controlled radiation photonics systems, it is necessary to have complete information about the nonlinear properties of the materials used. In this Letter, the vibrational mechanism of the giant low-inertia cubic nonlinearity of the refractive index of water in the terahertz (THz) frequency range is experimentally proven. Its dominance, which manifests itself when the temperature of the liquid changes, is demonstrated. The measured nonlinear refractive index in the THz frequency range for a water jet at temperatures from 14°C to 21°C demonstrates a correlation with the theoretical approach, varies in the range 4-10 × 10-10 cm2/W, and is characterized by an inertial time constant of less than 1 ps.

Enhanced terahertz third harmonic generation with high-order guided-mode resonance of graphene plasmonic gratings

We present a unique scheme to efficiently enhance terahertz third harmonic generation (THG). By exploiting the high-order guided-mode resonance of graphene plasmonic grating, the off-plane transverse localized field can be suppressed, which enables the electromagnetic energy to be tightly concentrated and significantly enhanced in the monolayer graphene. Meanwhile, high density of in-plane hot spots can be excited to form a quasi-continuous enhanced-field profile called as hot surface. This can bring about the giant nonlinearity enhancement of terahertz field-graphene interaction, greatly pushing forward the enhanced THG in monolayer graphene to breakout the limitation of various patterned metamaterials. It is anticipated that the graphene plasmonic grating has promising application for nonlinear terahertz spectroscopy, imaging and communication.

Gain-Assisted Giant Third-Order Nonlinearity of Epsilon-Near-Zero Multilayered Metamaterials.

We investigate the third-order nonlinear optical properties of epsilon-near-zero (ENZ) Au/dye-doped fused silica multilayered metamaterials in the visible spectral range for TM incident by using nonlocal effective medium theory at different incidence angles. The nonlocal response affects the permittivity of anisotropic metamaterials when the thickness of the layer cannot be much smaller than the incident wavelength. By doping pump dye gain material within the dielectric layer to compensate for the metal loss, the imaginary part of the effective permittivity is reduced to 10−4, and the optical nonlinear refractive index and nonlinear absorption coefficient are enhanced. The real and imaginary parts of the permittivity are simultaneously minimized when the central emission wavelength of the gain material is close to the ENZ wavelength, and the nonlinear refraction coefficient reaches the order of 10−5 cm2/W, which is five orders of magnitude larger than that of the nonlinear response of the metamaterial without the gain medium. Our results demonstrate that a smaller imaginary part of the permittivity can be obtained by doping gain materials within the dielectric layer; it offers the promise of designing metamaterials with large nonlinearity at arbitrary wavelengths.

Two-photon IR pumped UV–Vis transient absorption spectroscopy of Dirac fermions in the topological insulator Bi2Se3

It is often taken for granted that in pump-probe experiments on the topological insulator (TI) Bi2Se3 using IR pumping with a commercial Ti:sapphire laser [∼800 nm (1.55 eV photon energy)], the electrons are excited in the one-photon absorption regime, even when pumped with absorbed fluences in the mJ cm−2 range. Here, using UV–Vis transient absorption (TA) spectroscopy, we show that even at low-power Infrared (IR) pumping with absorbed fluences in the μJ cm−2 range, the TA spectra of the TI Bi2Se3 extend across a part of the UV and the entire visible region. This observation suggests unambiguously that the two-photon pumping regime accompanies the usual one-photon pumping regime even at low laser powers applied. We attribute the high efficiency of two-photon pumping to the giant nonlinearity of Dirac fermions in the Dirac surface states (SS). On the contrary, one-photon pumping is associated with the excitation of bound valence electrons in the bulk into the conduction band. Two mechanisms of absorption bleaching were also revealed since they manifest themselves in different spectral regions of probing and cause the appearance of three different relaxation dynamics. These two mechanisms were attributed to the filling of the phase-space in the Dirac SS and bulk states, followed by the corresponding Pauli blocking.

A giant self-Kerr nonlinearity using phase-sensitive excitation in a closed three-level atomic system

A third-order nonlinear response is investigated theoretically using a closed lambda system. In this scheme, a pair of optical fields and a microwave field connect three hyperfine levels in a cyclic fashion, rendering the atomic response sensitive to the relative phase of all three fields. Changing the relative phase, we can suppress the linear response of the probe field and enhance its third order self-Kerr nonlinear response using the underlying electromagnetically induced transparency (EIT) effect. The resultant giant self-Kerr nonlinear response is comparable to or exceeding that found in atomic systems at room temperature. Most importantly, we show that the self-Kerr nonlinear response at an optical frequency can be controlled using the phase and amplitude of a frequency-separated microwave field.

Giant nonlinearity in upconversion nanoparticles

Giant nonlinearity in upconversion nanoparticles

Inertia of the oscillatory mechanisms of giant nonlinearities of optical materials in the terahertz spectral range

Subject of study. The inertia of the oscillatory mechanisms of the nonlinearities of isotropic dielectric media in the field of the terahertz-frequency electromagnetic waves was investigated for resonant and nonresonant interactions between radiation and matter. The purpose of this work was to construct a dynamic model of the nonlinear polarization responses of optical media with oscillatory nature in the field of terahertz pulses and to estimate the time constants characterizing the inertia of such responses during resonant and nonresonant interactions between radiation and media molecular vibrations. Method. The model of anharmonic vibrations of the atoms of each molecule as an oscillator in the general case for an isotropic medium, with both quadratic and cubic nonlinearities, was reduced for a macroscopic optical characteristic—its polarization—to a model as a system of parametrically coupled equations with only cubic nonlinearities. The system parameters were determined from well-known characteristics of a medium, such as its thermal expansion coefficient, stretching molecular vibration frequency, and refractive index. Main results. Expressions were obtained for the inertial time constants of the cubic susceptibilities of optical media with nonlinear vibrations in two- and one-photon resonant interactions with quasi-monochromatic terahertz pulses as well as in nonresonant interactions with broadband terahertz pulsed radiation through the thermal, spectral, and optical characteristics of materials known in the literature. Numerical estimates were obtained for the inertial time constants of the nonlinear susceptibilities of media with particularly high vibrational nonlinearities in the refractive indices, namely, α-pinene and water, as well as silicon dioxide. For these materials, the inertial time constants of the resonant oscillatory mechanisms of the nonlinearities for radiation in the terahertz spectral range were shown to be of the order of hundreds of femtoseconds; for the nonresonant interactions, the time constants decreased to ten femtoseconds or less. Practical significance. The obtained inertial time constant estimations of the polarization responses of materials indicate that their giant nonlinearities in the far infrared spectral range could be used to develop ultrafast photonic devices for pulsed terahertz radiation parameter control.

Giant Nonlinear Optical Response of Graphene Oxide Thin Films Under the Photochemical and Photothermal Reduction

AbstractThin graphene oxide (GO) films have been widely explored for their outstanding optical properties, especially their large optical nonlinear coefficients, and high tunability of optical nonlinear coefficients under photoreduction. In this work, an experimental observation of giant nonlinear optical response in GO films under two different photoreduction mechanisms is reported. After ultraviolet (UV) light‐induced photochemical reduction and continuous wave (CW) laser‐induced photothermal reduction, the nonlinear optical response of reduced graphene oxide (rGO) via the Z‐scan method using a femtosecond laser beam at a wavelength of 800 nm is characterized. The rGO exhibits a giant optical nonlinearity, especially two‐photon absorption (TPA). A giant TPA coefficient of rGO on the order of ≈105 cm GW−1 is obtained under two photoreduction mechanisms (photochemistry and photothermal). This is the first time that a large enhancement effect of TPA has been observed in graphene‐based materials, and the TPA coefficient is an order of magnitude higher than the highest value previously reported. The versatile optical nonlinear properties imply a huge potential of the GO film in advanced photonic and optoelectronic devices such as broadband ultrafast optical switching and optical limiting.

Optical nonlinearity goes ultrafast in 2D semiconductor-based nanocavities.

Hybrid systems of silver nanodisks strongly coupled to monolayer tungsten-disulfide (WS2) show giant room-temperature nonlinearity due to their deeply sub-wavelength localized nature, resulting in ultrafast modifications of nonlinear absorption in a solid-state system.