We theoretically investigate the spectral caustics of high-order harmonics in solids. We analyze the 1-dimension model of solids HHG and find that, apart from the caustics originated from the van Hove singularities in the energy-band structure, another kind of catastrophe singularities also emerge when the different branches of electron-hole trajectories generating high-order harmonics coalesce into a single branch. We solve time-dependent Schrödinger equation in periodic potential and demonstrate the control of this kind of singularities in HHG with the aids of two-color laser fields. The diffraction patterns of the harmonic spectrum near the caustics agree well with the inter-band electron-hole recombination trajectories predicted by the semiconductor semi-classical equation. This work is expected to help to understand the HHG dynamics in solids and manipulate the harmonic spectrum by adjusting driving field parameters.
The high-order harmonic spectrum generated in two-color intense laser field under certain conditions has a pronounced maximum caused by the so called spectral caustic. Using a numerical solution of the 3D time-dependent Schrödinger equation we study the width of the maximum and the degree of the generation enhancement due to the caustic as a function of the fundamental intensity, wavelength, and atomic ionization potential. It is shown that the degree of this enhancement can be well quantitatively characterized by a single parameter: the ratio of the radius of the free electronic oscillation i…
We report the observation of arbitrary accelerating beams designed using a non-paraxial description of optical caustics. We use a spatial light modulator-based setup and techniques of Fourier optics to generate circular and Weber beams subtending over 95 degrees of arc. Applying a complementary binary mask also allows the generation of periodic accelerating beams taking the forms of snake-like trajectories, and the application of a rotation to the caustic allows the first experimental synthesis of optical accelerating beams upon the surface of a sphere in three dimensions.
Strong field driven electric currents in condensed matter systems open new frontiers in petahertz electronics. In this regime new challenges arise as the role of the band structure and the quantum nature of electron-hole dynamics have yet to be resolved. Here we reveal the underlying attosecond dynamics that dictates the temporal evolution of carriers in multi-band solid state systems, via high harmonic generation (HHG) spectroscopy. We demonstrate that when the electron-hole relative velocity approaches zero, enhanced quantum interference leads to the appearance of spectral caustics in the HH…
Geometrical optics (GO) is often used to model wave propagation in weakly inhomogeneous media and quantum-particle motion in the semiclassical limit. However, GO predicts spurious singularities of the wavefield near reflection points and, more generally, at caustics. We present a new formulation of GO, called metaplectic geometrical optics (MGO), that is free from these singularities and can be applied to any linear wave equation. MGO uses sequenced metaplectic transforms of the wavefield, corresponding to symplectic transformations of the ray phase space, such that caustics disappear in the n…
We report an application of the tri-dimensional pseudo-spectral time domain algorithm, that solves with accuracy the nonlinear Maxwell's equations, to predict second harmonic generation in lithium niobate ridge-type waveguides with high index contrast. Characteristics of the nonlinear process such as conversion efficiency as well as impact of the multimode character of the waveguide are investigated as a function of the waveguide geometry in uniformly and periodically poled medium.
The effect of slow light on second harmonic generation in a periodically poled $χ^{(2)}$ nonlinear medium is investigated theoretically. A linear $π$ phase shifted grating is used to slow the group velocity of the fundamental frequency and the resulting field enhancement greatly increases the second harmonic conversion efficiency. A second linear grating at the input end ensures that all output is in the forward direction. We show that almost 100\% conversion efficiency can be achieved for continuous wave pumping at low intensities that generate negligible conversion in the absence of the slow…
Optical waveguides made from periodically poled materials provide high confinement of light and enable the generation of new wavelengths via quasi-phase-matching, making them a key platform for nonlinear optics and photonics. However, such devices are not typically employed for high-harmonic generation. Here, using 200-fs, 10-nJ-level pulses of 4100 nm light at 1 MHz, we generate high harmonics up to the 13th harmonic (315 nm) in a chirped, periodically poled lithium niobate (PPLN) waveguide. Total conversion efficiencies into the visible--ultraviolet region are as high as 10 percent. We find …
We studied the high-order harmonic generation (HHG) from 2D solid materials in circularly and bichromatic circularly polarized laser fields numerically by simulating the dynamics of single-active-electron processes in 2D periodic potentials. Contrary to the absence of HHG in the atomic case, circular HHGs below the bandgap with different helicities are produced from intraband transitions in solids with $C_4$ symmetry driven by circularly polarized lasers. Harmonics above the bandgap are elliptically polarized due to the interband transitions. High-order elliptically polarized harmonics can be …
Second-order optical nonlinear effects (second-harmonic and sum-frequency generation) are demonstrated in the telecommunication band by periodic poling of thin films of lithium niobate wafer-bonded on silicon substrates and rib-loaded with silicon nitride channels to attain ridge waveguide with cross-sections of ~ 2 μm2. The compactness of the waveguides results in efficient second-order nonlinear devices. A nonlinear conversion of 8% is obtained with a pulsed input in 4 mm long waveguides. The choice of silicon substrate makes the platform potentially compatible with silicon photonics, and th…
Optical second-harmonic generation (SHG) is studied for the confined geometry of a circular cylindrical waveguide or optical fiber. A model situation of high symmetry is considered where the material with nonlinear susceptibility is isotropic and distributed in radially symmetric manner about the axis. In addition it is assumed that the material of high second-order nonlinearity consists of a thin circular layer, with periodic variation in the axial direction - similar to a usual quasi-phasematched configuration. One can optimize the efficiency of SHG by choosing the period of the array such t…
We study theoretically the effect of the giant resonance in Xe on the phase difference between the consecutive high order resonantly-enhanced harmonics and calculate the duration of the attosecond pulses produced by these harmonics. For certain conditions resonantly-induced dephasing compensates the phase difference which is intrinsic for the off-resonance harmonics. We find these conditions analytically and compare them with the numerical results. This harmonic synchronization allows attosecond pulse shortening in conjunction with the resonance-induced intensity increase by more than an order…
High harmonic generation (HHG) from crystals in strong laser fields has been understood by the band theory of solid, which is based on the periodic boundary condition (PBC) of translational invariant. For systems having PBC of rotational invariant, in principles an analogous Bloch theorem can be developed and applied. Taking a ring-type cluster of cyclo[18]carbon as a representative, we theoretically suggest a quasi-band model and study its HHG by solving time-dependent Liouville-von Neumann equation. Under the irradiation of circularly polarized laser, explicit selection rules for left-handed…
Conventional photonic lattices, such as metamaterials and photonic crystals, exhibit various interesting physical properties that are attributed to periodic modulations in lattice parameters. In this study, we introduce novel types of photonic lattices, namely Fourier-component-engineered metasurfaces, that do not possess the first Fourier harmonic component in the lattice parameters. We demonstrate that these metasurfaces support the continuous high-$Q$ bound states near second stop bands. The concept of engineering Fourier harmonic components in periodic modulations provides a new method to …
The high harmonic generation in periodically corrugated submicrometer waveguides is studied numerically. Plasmonic field enhancement in the vicinity of the corrugations allows to use low pump intensities. Simultaneously, periodic placement of the corrugations leads to quasi-phase-matching and corresponding increase of the high harmonic efficiency. The optimization of waveguide geometry is performed, and the resulting spectra are analyzed by the means of (1+1)D numerical model.
We study the propagation of light in a three-dimensional double-periodic Ag/TiO2 multilayer metamaterial composed of coupled plasmonic waveguides operating in the visible and UV spectral range. For these frequencies, light propagation in the plane of the waveguides is described by a negative phase velocity, while for the orthogonal direction light propagation is described by a Bloch wave composed of a large number of harmonics. As a result, the material cannot generally be described by a single phase index: decomposing the Bloch wave into different harmonics we show that for the wavelength ran…
A simple and flexible technique for achieving quasi-phase-matching in integrated photonic waveguides without periodic poling is proposed and experimentally demonstrated, referred to as mode-shape-modulation (MSM). It employs a periodic variation of waveguide width to modulate the intensity of the pump wave, effectively suppressing out-of-phase light generation. This technique is applied to the case of second-harmonic generation in thin-film lithium niobate ridge waveguides. MSM waveguides are fabricated and characterized with pulsed-pumping in the near-infrared, showing harmonic generation at …
High-order harmonic generation (HHG) in isolated atoms and molecules has been widely utilized in extreme ultraviolet (XUV) photonics and attosecond pulse metrology. Recently, HHG has also been observed in solids, which could lead to important applications such as all-optical methods to image valance charge density and reconstruction of electronic band structures, as well as compact XUV light sources. Previous HHG studies are confined on crystalline solids; therefore decoupling the respective roles of long-range periodicity and high density has been challenging. Here, we report the first observ…
Remarkable optical and electrical properties of two-dimensional (2D) materials, such as graphene and transition-metal dichalcogenide (TMDC) monolayers, offer vast technological potential for novel and improved optoelectronic nanodevices, many of which relying on nonlinear optical effects in these 2D materials. This article introduces a highly effective numerical method for efficient and accurate description of linear and nonlinear optical effects in nanostructured 2D materials embedded in periodic photonic structures containing regular three-dimensional (3D) optical materials, such as diffract…
We study theoretically optical response of WS2 monolayer located near periodic metal nanostructured arrays in two and three dimensions. The emphasis of simulations is on the strong coupling regime of excitons supported by WS2 and surface plasmon-polaritons supported by various periodic plasmonic interfaces. It is demonstrated that a monolayer of WS2 placed in a close proximity of periodic arrays of either slits or holes results in a Rabi splitting of the corresponding surface plasmon-polariton resonance as revealed in calculated transmission and reflection spectra. The nonlinear regime, at whi…
Optical properties of periodic arrays of nanoholes of a triangular shape with experimentally realizable parameters are examined in both linear and nonlinear regimes. Utilizing fully vectorial three-dimensional approach based on the nonlinear hydrodynamic Drude model describing metal coupled to Maxwells equations and Bloch equations for molecular emitters we analyze linear transmission, reflection, and nonlinear power spectra. Rigorous numerical calculations demonstrating second and third harmonic generation by the triangular hole arrays are performed. It is shown that both the Coulomb interact…
In a one-dimensional periodic nonlinear $χ^{(2)}$ medium, by choosing a proper material and geometrical parameters of the structure, it is possible to obtain two matching conditions for simultaneous generation of second and third harmonics. This leads to new diversity of the processes of the resonant three-wave interactions, which are discussed within the framework of slowly varying envelope approach. In particular, we concentrate on the fractional conversion of the frequency $ω\to (2/3) ω$. This phenomenon occurs by means of intermediate energy transfer to the first harmonic at the frequency …
We study numerically the Bloch electron wave-packet dynamics in periodic potentials to simulate laser-solid interactions. We introduce a quasi-classical model in the \emph{k} space combined with the energy band structure to understand the high-order harmonic generation (HHG) process occurring in a subcycle timescale. This model interprets the multiple plateau structure in HHG spectra well and the linear dependence of cutoff energies on the amplitude of vector potential of the laser fields. It also predicts the emission time of HHG, which agrees well with the results by solving the time-depende…
Nonlinear optical processes of spatially structured light, including optical vortex and vector optical fields, have stimulated a lot of interesting physical effects and found a variety of important applications ranging from optical imaging to quantum information processing. However, high harmonic generation of vector optical fields with space-varying polarization states is still a challenge. Here we demonstrate third harmonic generation of spatially structured light including vector optical fields, in a nonlinear Sagnac interferometer containing a carefully designed quasi-periodically poled po…
We theoretically study high-order harmonic generation (HHG) from solid-phase systems in spatially inhomogeneous strong laser fields originated by resonant plasmons within a metallic nanostructure. The intensity of the second plateau in HHG may be enhanced by two-three orders and be comparable with the intensity of the first plateau. This is due to bigger transition probabilities to higher conduction bands. It provides us a practical way to increase the yields of HHG with laser intensity below the damage threshold. It presents a promising way to triple the range of HHG spectra in experimental m…
Ptychographic Coherent Diffractive Imaging enables diffraction-limited imaging of nanoscale structures at extreme ultraviolet and x-ray wavelengths, where high-quality image-forming optics are not available. However, its reliance on a set of diverse diffraction patterns makes it challenging to use ptychography to image highly periodic samples, limiting its application to defect inspection for electronic and photonic devices. Here, we use a vortex high harmonic light beam driven by a laser carrying orbital angular momentum to implement extreme ultraviolet ptychographic imaging of highly periodi…
We investigate the multielectron effects on high-harmonic generation from solid-state materials using the time-dependent Hartree-Fock theory. We find qualitative change in harmonic spectra, in particular, multiple-plateau formation at significantly lower laser intensities than within the independent-electron approximation. We reveal its origin in terms of interband polarization, i.e, electron-hole polarization, enabling interband excitation at remote crystal momenta via Coulomb potential.
Optical orbital angular momentum (OAM), as an important degree of freedom of light, has been attracted extensive attention, due to its intrinsic feature of natural discrete infinite dimension. Manipulation of OAM spectra is crucial for many impressive applications from classical to quantum realms, in particular, nonlinear manipulation of OAM spectra. Here we realized the nonlinear manipulation of OAM spectra by using the simultaneous second- and third-harmonic generation in a single nonlinear crystal of quasi-periodically poled potassium titanyl phosphate, for fundamental waves with a variety …
Spatial and spectral properties of the pulsed second harmonic generation in a periodically-poled KTP waveguide exploiting simultaneously the first, second, and third harmonics of periodic nonlinear modulation are analyzed. Experimental results are interpreted using a model based on finite elements method. Correlations between spatial and spectral properties of the fundamental and second-harmonic fields are revealed. Individual nonlinear processes can be exploited combining spatial and spectral filtering. Also the influence of waveguide parameters to the second-harmonic spectra is addressed.
We formulate a theory of bulk optical current for a periodically driven system, which accounts for the mixing of external drive and laser field frequencies and, therefore, the broadening of the harmonic spectrum compared to the undriven system. We express the current in terms of Floquet-Bloch bands and their non-adiabatic Berry connection and curvature. Using this expression, we relate spatio-temporal symmetries of the driven model to selection rules for current harmonics. We illustrate the application of this theory by studying high harmonic generation in the periodically driven Su-Schrieffer…
Exponential localization of wavefunctions in lattices, whether in real or synthetic dimensions, is a fundamental wave interference phenomenon. Localization of Bloch-type functions in space-periodic lattice, triggered by spatial disorder, is known as Anderson localization and arrests diffusion of classical particles in disordered potentials. In time-periodic Floquet lattices, exponential localization in a periodically driven quantum system similarly arrests diffusion of its classically chaotic counterpart in the action-angle space. Here we demonstrate that nonlinear optical response allows for …
