A purely artificial mechanism for optical nonlinearity is proposed based on a metamaterial route. The mechanism is derived from classical electromagnetic interaction in a meta-molecule consisting of a cut-wire meta-atom nested within a split-ring meta-atom. Induced by the localized magnetic field in the split-ring meta-atom, the magnetic force drives an anharmonic oscillation of free electrons in the cut-wire meta-atom, generating an intrinsically nonlinear electromagnetic response. An explicit physical process of a second-order nonlinear behavior is adequately described, which is perfectly demonstrated with a series of numerical simulations. Instead of "borrowing" from natural nonlinear materials, this novel mechanism of optical nonlinearity is artificially dominated by the meta-molecule geometry and possesses unprecedented design freedom, offering fascinating possibilities to the research and application of nonlinear optics.
We have derived the local electric field inside graded metal-dielectric composite films with weak nonlinearity analytically, which further yields the effective linear dielectric constant and third-order nonlinear susceptibility of the graded structures. As a result, the composition-dependent gradation can produce a broad resonant plasmon band in the optical region, resulting in a large enhancement of the optical nonlinearity and hence a large figure of merit.
A nonrelativistic Hamiltonian describing interaction between a mechanical degree of freedom and radiation pressure is commonly used as an ultimate tool for studying system behavior in opto-mechanics. This Hamiltonian is derived from the equation of motion of a mechanical degree of freedom and the optical wave equation with time-varying boundary conditions. We show that this approach is deficient for studying higher order nonlinear effects in an open resonant opto-mechanical system. Opto-mechanical interaction induces a large mechanical nonlinearity resulting from a strong dependence of the pow…
The effective linear and third-order nonlinear susceptibility of graded metallic films with weak nonlinearity have been investigated. Due to the simple geometry, we were able to derive exactly the local field inside the graded structures having a Drude dielectric gradation profile. We calculated the effective linear dielectric constant and third-order nonlinear susceptibility. We investigated the surface plasmon resonant effect on the optical absorption, optical nonlinearity enhancement, and figure of merit of graded metallic films. It is found that the presence of gradation in metallic films …
Epsilon-near-zero (ENZ) materials have shown significant potential for nonlinear optical applications due to their ultrafast hot carriers and consequent optical nonlinearity enhancement. Modified poly(3,4-ethylenedioxythiophene) (PEDOT) films show metallic characteristics and a resultant ENZ wavelength near 1550nm through polar solvent treatment and annealing. The metallic PEDOT film exhibits an intrinsic optical nonlinear response that is comparable to gold and 100-fold higher than typical inorganic semiconductor ENZ materials due to π-conjugated delocalized electrons. Hot carriers generate a…
Metals typically have very large nonlinear susceptibilities, whose origin is mainly of thermal character. We model the cubic nonlinearity of thin metal films by means of a delayed response derived \textit{ab initio} from an improved version of the classic two temperature model. We validate our model by comparison with ultrafast pump-probe experiments on gold films.
Within a decade of fruitful developments, metamaterials became a prominent area of research, bridging theoretical and applied electrodynamics, electrical engineering and material science. Being man-made structures, metamaterials offer a particularly useful playground to develop novel interdisciplinary concepts. Here we demonstrate a novel principle in metamaterial assembly which integrates electromagnetic, mechanical, and thermal responses within their elements. Through these mechanisms, the conformation of the meta-molecules changes, providing a dual mechanism for nonlinearity and offering no…
Over the last three decades, plasmonics using metallic nanostructures has become central to nanophotonics research. Recently, its targets have been extended to nonlinear optical phenomena. In a nonlinear regime, quantum mechanical effects, as exemplified by electron spill-out on the surface of nanostructures, significantly influence the optical response. Quantum hydrodynamic theory (QHT) is a promising basis for the analysis of nonlinear optical responses involving such quantum mechanical effects. Herein, QHT was applied to calculate the third-order optical nonlinearity of a spherical metallic…
We present a theoretical analysis of the nonlinear response of a metamaterial consisting of an array of split ring resonators coupled to a two level atomic system (2LS) without inversion. We calculated the total complex susceptibility and the linear, third and fifth-order nonlinear solution of the Maxwell Bloch equations that describe the coupled system. We analyzed the impact of the nonlinear effects on the dynamics of an active metamaterial/2LS compound in dependence of the magnitude of the external electric field when the 2LS is pumped by an external pump source and population inversion is …
Nonlinear processes are at the core of many optical technologies including lasers, information processing, sensing, and security, and require optimised materials suitable for nanoscale integration. Here we demonstrate the emergence of a strong bulk second-order nonlinear response in a composite plasmonic nanorod material comprised of centrosymmetric materials. The metamaterial provides equally strong generation of the p-polarized second harmonic light in response to both s- and p-polarized excitation. We develop an effective-medium description of the underlying physics, compare its predictions…
We demonstrate a nonlinear metamaterial that can be switched between low and high transmission by controlling the power level of the incident beam. The origin of this nonlinear response is the superconducting Nb thin film employed in the metamaterial structure. We show that with moderate RF power of about 22 dBm it is possible to quench the superconducting state as a result of extremely strong current densities at the corners of the metamaterial's split-ring resonators. We measure a transmission contrast of 10 dB and a change in group delay of 70 ns between the low and high power states.
We demonstrate that the effective third-order nonlinear susceptibility of a graphene sheet can be enhanced by more than two orders of magnitude by patterning it into a graphene metasurface. In addition, in order to gain deeper physical insights into this phenomenon, we introduce a novel homogenization method, which is subsequently used to characterize quantitatively this nonlinearity enhancement effect by calculating the effective linear and nonlinear susceptibility of graphene metasurfaces. The accuracy of the proposed homogenization method is demonstrated by comparing its predictions with th…
From the demonstration of saturable absorption by Vavilow and Levshin in 1926, and with invention of the laser, unavailability of strongly nonlinear materials was a key obstacle for developing optical signal processing, in particular in transparent telecommunication networks. Today, most advanced photonic switching materials exploit gain dynamics and near-band and excitonic effects in semiconductors, nonlinearities in organic media with weakly-localized electrons and nonlinearities enhanced by hybridization with metamaterials. Here we report on a new type of artificial nonlinearity that is nan…
We find the analytical expression for the threshold intensity necessary to launch ultra-slow light pulses in a metamaterial with simultaneous cubic electric and magnetic nonlinearity. The role played respectively by the permittivity, the permeability, the electric cubic nonlinearity, the magnetic cubic nonlinearity and the pulse duration is clearly identified and discussed.
The development of nanomaterials with a large nonlinear susceptibility is essential for nonlinear nanophotonics. We show that transition-metal-dichalcogenide (TMD) nanotriangles have a large effective second-order susceptibility [$χ^{(2)}$] at mid-infrared to near-infrared frequencies owing to their broken centrosymmetry. $χ^{(2)}$ is calculated within the density-matrix formalism that accounts for dissipation and screening. $χ^{(2)}$ peaks in the vicinity of both two-photon resonances (specified by the geometry) and plasmon resonances (tunable via the carrier density). Aligning the resonances…
We report on the linear and nonlinear optical response of metamaterials evoked by first and second order multipoles. The analytical ground on which our approach bases permits for new insights into the functionality of metamaterials. For the sake of clarity we focus here on a key geometry, namely the split-ring resonator, although the introduced formalism can be applied to arbitrary structures. We derive the equations that describe linear and nonlinear light propagation where special emphasis is put on second harmonic generation. This contribution basically aims at stretching versatile and exis…
A theoretical study of wave propagation in 1D metamaterial is presented. A system of nonlinear evolution equation for electromagnetic waves with both polarizations account is derived by means of projection operators method for general nonlinearity and dispersion. The system describes interaction of opposite directed waves with a given polarization. The particular case of Kerr nonlinearity and Drude dispersion is considered. In such approximation it results in the correspondent systems of nonlinear equations that generalizes the Schäfer-Wayne one. Particular solutions in case of slow-varying en…
Metasurfaces have attracted a great deal of attention from researchers due to their prominent optical properties. In particular, metasurfaces may consist of structures possessing optical anapole resonances with strong field confinement and substantially suppressed scattering. As a result, such nanostructures display enhanced nonlinear optical properties. In this paper by means of three-dimensional finite-difference time-domain simulations, the ability of anapole modes in high-index dielectric metasurfaces with circular nanopores is shown. In the vicinity of the anapole state, the effective opt…
We study the main nonlinear solutions of plasmonic slot waveguides made from an anisotropic metamaterial core with a positive Kerr-type nonlinearity surrounded by two semi-infinite metal regions. First, we demonstrate that for a highly anisotropic diagonal elliptical core, the bifurcation threshold of the asymmetric mode is reduced from GW/m threshold for the isotropic case to 50 MW/m one indicating a strong enhancement of the spatial nonlinear effects, and that the slope of the dispersion curve of the asymmetric mode stays positive, at least near the bifurcation, suggesting a stable mode. Sec…
We develop a quantum theory of electron confinement in metal nanofilms. The theory is used to compute the nonlinear response of the film to a static or low-frequency external electric field and to investigate the role of boundary conditions imposed on the metal surface. We find that the sign and magnitude of the nonlinear polarizability depends dramatically on the type of boundary condition used.
The optical Kerr effect of material with negative refraction is estimated for the first time. This is done via three-dimensional finite-difference time-domain (FDTD) simulations of disordered bidisperse metasurfaces consisting of high index (GaP) spheres at the wavelength of 532~nm. The metasurfaces comprise spherical particles randomly arranged on plane having two sizes close to the magnetic and electric dipole Mie resonances. The real part of the effective nonlinear refractive index of the metasurfaces is computed in the vicinity of the Mie resonances where the metasurface possesses the nega…
All-optical switching based on optical nonlinearity must undergo complex processes of light-mater interaction in atom and electron scale, so a relative high power and long response time is required, that construct main bottlenecks in all-optical technology. In this paper, we propose a new mechanism for building all-optical switching based on a change resonance modes of meta-atoms in metamaterials, not involved optical nonlinearity of materials. A metamaterial composed of cubic dielectric meta-atoms periodically embedded in a background matrix is designed and constructed. All-optical switch fun…
We analyze an inherent nonlinearity of Surface Plasmon Polaritons at the interface of Fermi-Dirac metal plasma, stemming from the depletion of electron density in high-field intensity regions. The derived optical nonlinear coefficients are comparable to the experimental values for metals. We calculate the dispersion relations for the nonlinear propagation of high-intensity Surface Plasmon Polaritons, predicting a nonlinear induced cutoff and vanishing group velocity.
Over the last few decades, extensive previous studies of the nonlinear response of metal nanoparticles report a wide variation of nonlinear coefficients, thus, revealing a highly confused picture of the underlying physics. This naturally prevents rational design of these systems for practical devices. Here, we provide a systematic study of the nonlinear response of metal spheres under continuous wave illumination within a purely thermal model. We characterize the strong dependence of the temperature rise and overall thermo-optic nonlinear response on the particle size and permittivity, on the …
High index dielectric nanoantennas excited at Mie-type resonances have exhibited enormous enhancement of optical nonlinearity. Such nanostructures have been actively studied by researchers in the last years. The present work provides the first numerical analysis study of the optical Kerr effect of nanocomposites consisting of high refractive index (GaP) spheres at the wavelength of 532~nm. This is done by means of three-dimensional finite-difference time-domain (FDTD) simulations. The effective nonlinear refractive index of $0.8$~$μ$m thick nanocomposites and metasurfaces is evaluated. It is s…
We investigate the effect of anomalous field enhancement in metamaterials where the effective refractive index gradually changes from positive to negative values, i.e. transition metamaterials. We demonstrate that considerable field enhancement can be achieved in lossy optical transition metamaterials that have electromagnetic material properties obtained from experimental data. The field enhancement factor is found to be polarization-dependent and largely determined by the material parameters and the width of the transition layer.
The nonlinear optical properties of the high index nanoparticles are boosted at the anapole state. Researchers intensively study this phenomenon as promising for various applications. In this work, the nonlinear optical Kerr effect of disordered and square lattice metasurfaces of GaP nanodisks is investigated as a function of the disk size in the vicinity of the anapole state at the wavelength of 532 nm. When the sizes of the nanodisks are close to the anapole state, the effective second order refractive index of the metasurface increases exponentially. On approaching the anapole state, the si…
The vacuum is expected to exhibit electromagnetic nonlinearity. We demonstrate the properties of nonlinear electromagnetic wave in a two-dimensional rectangular cavity by calculating the nonlinear correction for two classical standing waves. We apply the linear approximation in a short timescale. A part of the nonlinear correction increases with time. In particular, a one-dimensional second harmonic grows if the cavity size satisfies a specific condition. We also analyze the nonlinear electromagnetic wave in a timescale longer than the applicable limit of the linear approximation. We formulate…
We theoretically investigate the electromagnetic response of a novel class of multi-layered metamaterials obtained by alternating graphene sheets and dielectric layers, the whole structure not exhibiting a plane of reflection symmetry along the stacking direction. We show that the electromagnetic response of the structure is characterized by a magneto-electric coupling described by an effective chiral parameter. Exploiting the intrinsic tunability of the graphene-light coupling, we prove that one can tune both the dielectric and the chiral electromagnetic response by varying the graphene chemi…
We investigate the storage and retrieval of electromagnetic waves using a nonlinear metamaterial, analogous to the electromagnetically induced transparency (EIT) observed in atomic systems. We experimentally demonstrate the storage of the electromagnetic wave by reducing an auxiliary "control" wave; the stored wave is then released by recovering the control wave. We also confirm that the metamaterial can store and reproduce the phase distribution of the original input wave. These effects confirm a remarkable analogy between the metamaterial and an atomic EIT medium.
An analytical method of electromagnetic wave interactions with a general radially anisotropic cloak is established. It is able to deal with arbitrary parameters ($ε_r(r)$, $μ_r(r)$, $ε_t(r)$ and $μ_t(r)$) of a radially anisotropic inhomogeneous shell. The general cloaking condition is proposed from the wave relations for the first time. We derive the parameters of a novel class of spherical nonlinear cloaks and examine its invisibility performance by the proposed method at various nonlinear situations. Spherical metamaterial cloaks with improved invisibility performance is achieved with optima…
The quantum confiment of Rydberg excitons (REs) in quantum structures opens the way towards considering nonlinear interactions in such systems. We present a theoretical calculation of optical functions in the case of a nonlinear coupling between REs in a quantum well with an electromagnetic wave. Using the Real Density Matrix Approach (RDMA), the analytical expressions for a linear and nonlinear absorption are derived and numerical calculations for Cu$_2$0 quantum wells are performed. The results indicate the conditions in which quantum well confinement states can be observed in linear and non…
In this paper, we carry out a theoretical investigation on the propagation of spatio-temporal solitons (light bullets) in the nonlinear metamaterial waveguides. Our theoretical study is based on the formulation of Lagrangian variational analysis with a suitable ansatz followed by a split-step Fourier method in confirming the outcomes former numerically. A particular emphasis is given to obtain the conditions on the system parameters for stable dynamics in negative as well as positive index regimes of metamaterial waveguides. Similar to the conventional medium, the three-dimensional (3D) light …
The specific optical nonlinearities inherent in aggregates of metal nanoparticles under pico- and nanosecond pulsed laser irradiation are studied in nanoparticle aggregates formed in silver hydrosols. The results of experimental studies of the correlation between the degree of aggregation of silver hydrosols and their nonlinear refraction index at the wavelengths 0.532 and 1.064 microns are discussed. The experiments revealed that nonlinear refraction index changes its sign at 1.064 microns as the degree of the hydrosol aggregation grows. The role of various processes occurring in resonant dom…
Metasurfaces have attracted significant research interest owing to their unprecedented control over the spatial distributions of electromagnetic fields. Herein we propose the concept of metasurface tessellation to achieve reconfigurable scattering functions. Square meta-tiles, composed of identical structures, are arranged to fill a surface. The electromagnetic scattering of the tiled surface is determined by the orientation distribution of the meta-tiles. We present three typical cases of meta-tiles consisting of binary elements to realize several distinct scattering patterns. This study prov…
We propose a scheme for realizing subwavelength electromagnetic diode by employing cascading nonlinear meta-atoms. One-way response is demonstrated on a microwave transmission line comprising of three metallic ring resonators acting as meta-atoms and a varactor as the nonlinear medium inclusion. Experiments show that our implementation can operate simultaneously as forward diode and backward diode at different frequencies. A transmission contrast of up to 14.7dB was achieved between forward and backward transmission. Subwavelength size of our diode should be useful for miniaturization of integ…
Electromagnetic waves impinging on three-dimensional helical metallic metamaterials have been shown to exhibit chiral effects of large magnitude both theoretically and in experimental realizations. Chirality here describes different responses of scatterers, materials, or metamaterials to left and right circularly polarized electromagnetic waves. These differences can be quantified in terms of electromagnetic chirality measures. In this work we consider the optimal design of thin metallic free-form nanowires that possess measures of electromagnetic chirality as large as fundamentally possible. …
Simultaneous measurements of the intensity and phase of a probe wave reflected from an interface between silica and elemental alpha-gallium reveal its very strong optical nonlinearity, affecting both these parameters of the reflected wave. The data corroborate with a non-thermal mechanism of optical response which assumes appearance of a homogeneous highly metallic layer, only a few nanometer thick, between the silica and bulk alpha-gallium.
We develop, from first principles, a general and compact formalism for predicting the electromagnetic response of a metamaterial with non-magnetic inclusions in the long wavelength limit, including spatial dispersion up to the second order. Specifically, by resorting to a suitable multiscale technique, we show that medium effective permittivity tensor and the first and second order tensors describing spatial dispersion can be evaluated by averaging suitable spatially rapidly-varying fields each satysifing electrostatic-like equations within the metamaterial unit cell. For metamaterials with ne…
Optical devices with metastable states controlled with light (optical flip-flops) are needed in data storage, signal processing and displays. Although non-volatile optical memory relying on structural phase transitions in chalcogenide glasses has been widely used for optical data storage, beyond that, weak optical nonlinearities have hindered the development of low-power bistable devices. Here we report on a new type of volatile optical bistability in a resonant hybrid nano-optomechanical device, comprising of a pair of anchored nanowires decorated with plasmonic metamolecules. The nonlinearit…
A possibility of tuning the phase of the third-order Kerr-type nonlinear susceptibility in a system consisting of two interacting metal nanospheres and a nonlinearly polarizable molecule is investigated theoretically and numerically. It is shown that by varying the relative inter-sphere separation, it is possible to tune the phase of the effective nonlinear susceptibility χ^{(3)}(ω;ω,ω,-ω)$ in the whole range from 0 to $2π$.
Plasmonic metamaterials and metasurfaces offer new opportunities in developing high performance terahertz emitters and detectors beyond the limitations of conventional nonlinear materials. However, simple meta-atoms for second-order nonlinear applications encounter fundamental trade-offs in the necessary symmetry breaking and local-field enhancement due to radiation damping that is inherent to the operating resonant mode and cannot be controlled separately. Here we present a novel concept that eliminates this restriction obstructing the improvement of terahertz generation efficiency in nonline…
We address the propagation of laser beams in Si02-VO2 nanocomposite waveguides with thermo-optical nonlinearity. We show that the large modifications of the absorption coefficient as well as notable changes of refractive index of VO2 nanoparticles embedded into the SiO2 host media that accompany the semiconductor-to-metal phase transition may lead to optical limiting in the near-infrared wave range.
Local electromagnetic field enhancement in resonant metamaterials is useful for efficient generation of nonlinear phenomena; however, the field enhancement is suppressed by losses of nonlinear elements in metamaterials. For overcoming this issue, we investigate the nonlinear response of an electromagnetically induced transparency like metasurface loaded with gas as the nonlinear element. To induce nonlinearity in the gas associated with discharges, an electromagnetic wave with a modulated amplitude is incident on the metasurface. The measured waveform and spectrum of the transmitted electromag…
We report the experimental observation of strong two-color optical nonlinearity in an ultracold gas of $^{85}\mathrm{Rb}$-$^{87}\mathrm{Rb}$ atom mixture. By simultaneously coupling two probe transitions of $^{85}$Rb and $^{87}$Rb atoms to Rydberg states in electromagnetically induced transparency (EIT) configurations, we observe significant suppression of the transparency resonance for one probe field when the second probe field is detuned at $\sim1~\mathrm{GHz}$ and hitting the EIT resonance of the other isotope. Such a cross-absorption modulation to the beam propagation dynamics can be desc…
Applications of metallic metamaterials have generated significant interest in recent years. Electromagnetic behavior of metamaterials in the optical range is usually characterized by a local-linear response. In this article, we develop a finite-difference time-domain (FDTD) solution of the hydrodynamic model that describes a free electron gas in metals. Extending beyond the local-linear response, the hydrodynamic model enables numerical investigation of nonlocal and nonlinear interactions between electromagnetic waves and metallic metamaterials. By explicitly imposing the current continuity co…
Two distinct models are developed to investigate the transverse magnetic stationary solutions propagating in one-dimensional anisotropic nonlinear plasmonic structures made from a nonlinear metamaterial core of Kerr-type embedded between two semi-infinite metal claddings. The first model is semi-analytical, in which we assumed that the anisotropic nonlinearity depends only on the transverse component of the electric field and that the nonlinear refractive index modification is small compared to the linear one. This method allows us to derive analytically the field profiles and the nonlinear di…
