Optical Harmonic Generation Research Articles

Ultrafast Optical Modulation of Harmonic Generation in Two-Dimensional Materials.

The modulation of optical harmonic generation in two-dimensional (2D) materials is of paramount importance in nanophotonic and nano-optoelectronic devices for their applications in optical switching and communication. However, an effective route with ultrafast modulation speed, ultrahigh modulation depth, and broad operation wavelength range is awaiting a full exploration. Here, we report that an optical pump can dynamically modulate the third harmonic generation (THG) of a graphene monolayer with a relative modulation depth above 90% at a time scale of 2.5 ps for a broad frequency ranging from near-infrared to ultraviolet. Our observation, together with the real-time, time-dependent density functional theory (TDDFT) simulations, reveals that this modulation process stems from nonlinear dynamics of the photoexcited carriers in graphene. The superior performance of the nonlinear all-optical modulator based on 2D materials paves the way for its potential applications including nanolasers and optical communication circuits.

Giant enhancement of harmonic generation in all-dielectric resonant waveguide gratings of quasi-bound states in the continuum.

We report the giant enhanced optical harmonic generation in all-dielectric silicon nitride (SiN) based resonant waveguide gratings (RWGs) of quasi-bound states in the continuum (BICs) of ultra-high Q factor and localized field. The BICs are realized by tuning the excitation of the guided modes modulated by geometry parameters of four-part grating layer. At a feasible structure of quasi-BIC for nanofabrication, the SHG and THG are enhanced by 103 and 106, compared with those from the RWGs of traditional two-part grating layer, respectively, and even up to 108 and 1010 compared with those from the planar SiN film, respectively. The resonance wavelength of quasi-BICs can be effectively tuned by the angle of incidence, while almost not affect the enhancement of SHG and THG response. Our results show that the efficiency harmonic generation from all-nonlinear-dielectric RWGs of quasi-BICs has potential applications for the integrated nonlinear photonic devices.

Spatiotemporally resolved optical emission spectroscopy and harmonic generation in Cu plasmas

Laser-induced ablation plasmas of Cu generated by nanosecond 1064 nm pulses have been examined as media for third harmonic generation of a nanosecond driving pulse. A narrow window of ablation fluences where third harmonic generation is optimized has been identified in a region around twice the ablation threshold. A detailed analysis of the features of the Cu plasma across this critical fluence window, through spatially and temporally resolved optical emission spectroscopy, has been used to assess critical plasma parameters such as temperature, electron density, and abundance of Cu species in different ionization stages. This description has been correlated with the conditions for optimum low-order harmonic generation in the Cu plasma.

Effect of isovalent substitution on the crystal structure and properties of two-slab indates BaLa2−xSmxIn2O7

AbstractExploring the effect of isomorphic substitution of atoms on crystal structure and features of oxide compounds is one of the main tasks of modern materials science. This paper deals with the La/Sm isovalent substitution in a two-slab perovskite-like BaLa2In2O7 structure and its effect on the structural features and magnetic properties of BaLa2−xSmxIn2O7 indates synthesized. A complete characterization including data of scanning electron microscopy (SEM), energy-dispersive X-ray spectroscopy (EDS), X-ray diffraction (XRD), structural calculations (Rietveld method), second optical harmonic generation of the laser radiation, calculations of valence bond sums (VBS), and magnetic susceptibility data of phases obtained is presented. The existence region of BaLa2−xSmxIn2O7 solid solutions with a two-slab perovskite-like structure (0 ≤ x ≤ 1.8) was established, and their coordinate parameters were refined. The character of barium and RE atoms distribution in BaLa2−xSmxIn2O7 structure has determined, and the correlation between substitution degree of lanthanum atoms and the length of Ln–O2 interblock distance has revealed. The magnetic properties of BaLa2−xSmxIn2O7 were considered in terms of the crystal field effect.

Exploiting interband transitions in graphene for optical harmonic generation

Researchers show that the nonlinear optical properties of graphene produce a different tuning mechanism.

Quantum interference between the optical Stark effect and resonant harmonic generation in WS2

An applied field can modulate optical signals by resonance shifting via the Stark effect. The optical Stark effect (OSE) uses ultrafast light in the transparency region of a material to shift resonances with speeds limited by the pulse duration or system coherence. In this Letter we investigate the OSE in resonant optical harmonic generation (OHG) using the ground state exciton transition of WS2 with a variety of morphologies. Multidimensional pump-harmonic-probe measurements, in which the probe is second- or third-harmonic emission, reveal not only large Stark shifts that are commensurate with the large optical susceptibilities common to WS2 excitons, but also behaviors more complex than simple OSE treatments predict. We show how a new manifestation of the Stark Effect, brought forth by coherent photon exchange between the pump and OHG fundamental fields, can strongly enhance or suppress OHG.

Optical second- and third-harmonic generation on excitons in ZnSe/BeTe quantum wells

Optical harmonic generation on excitons is found in ZnSe/BeTe quantum wells with type-II band alignment. Two experimental approaches with spectrally-broad femtosecond laser pulses and spectrally-narrow picosecond pulses are used for spectroscopic studies by means of second and third harmonic generation (SHG and THG). The SHG signal is symmetry-forbidden for light propagation along the structure's growth axis, which is the [001] crystal axis, but can be induced by an external magnetic field. The THG signal is detected at zero magnetic field and its intensity is field independent. A group theory analysis of SHG and THG rotational anisotropy diagrams allows us to identify the involved excitation mechanisms.

Linear and non-linear optical properties of gelatin membranes doped with photoresponsive berries extracts

Natural extracts were successfully used as doping agents for the preparation of solutions, thin films and membranes in order to improve the optical properties of various polymers. The purpose of the present research is to develop polymeric membranes made of photoresponsive natural extracts and lithium perchlorate (LiClO4) by solution casting method. To achieve this, bilberry and blackcurrant extracts were successfully incorporated into gelatin/glycerine/lithium perchlorate (GEL/GLY/LiClO4) mixtures at different concentrations. The prepared membranes were characterized from structural point of view using Fourier transform infrared (FT-IR) and UV–Vis spectroscopy. Moreover, their hydrophilic/hydrophobic character was evaluated by the contact angle measurement. Their nonlinear optical properties were investigated by the optical third harmonic generation technique, and the results showed a potential use of membranes as integral part for the manufacture of optoelectronic devices such as light-emitting diodes (LEDs).

Magnetic Field Effects in Optical Harmonics Generation by Excitons

Mechanisms that are responsible for the optical harmonics generation at exciton transitions are analyzed in several classes of materials. In the cubic GaAs semiconductor, the magneto-induced optical second-harmonic generation second optical harmonic is observed in the region of orbital quantization of the valence and conduction bands. An unusually strong amplitude of the optical third-harmonic generation in an external magnetic field in the region of 1s exciton due to exciton–polariton resonance is found. The optical second-harmonic generation due to 1s, 2s, and 2p exciton resonances in a magnetic field is revealed in a hexagonal wide band-gap ZnO semiconductor. Depending on the symmetry of the exciton states, the mechanisms of the optical second-harmonic generation involve the spin and orbital Zeeman effects, and the magneto-Stark effect. The magneto-induced contribution to second harmonic generation (SHG) in the region of exciton transitions in the Cr2O3 antiferromagnet placed in an external magnetic field is studied.

Optical harmonic generation on the exciton-polariton in ZnSe

We study optical harmonic generation on the 1S exciton-polariton in the semiconductor ZnSe. Intense and spectrally narrow exciton resonances are found in optical second (SHG), third (THG), and fourth (FHG) harmonic generation spectra. The resonances are shifted to higher energy by 3.2 meV from the exciton energy in the linear reflectivity spectrum. Additional resonances are observed in the THG and FHG spectra and assigned to combinations of incident and backscattered photons in the crystal. Rotational anisotropy diagrams are measured and further information on the origin of the optical harmonic generation and the involved exciton states is obtained by a symmetry analysis using group theory in combination with a microscopic consideration.

Relativistic Nonlinear Optical Phenomena in the Field of Subterawatt Laser Pulses

Experiments on the generation of high optical harmonics demonstrating that relativistic regimes of interaction of radiation with matter can be implemented in the field of mid-infrared laser pulses with a peak power of 0.3 TW have been reported. The observation of relativistic phenomena at such extraordinary low peak powers of the laser field becomes possible because of the formation of a high-quality space-time mode of the laser field with an exactly specified polarization state. Such a field structure ensures a high intensity of radiation in the focus of the beam and the effective acceleration of electrons by a low-frequency electromagnetic field of a high-contrast laser pulse with an exactly specified polarization at the extremely sharp vacuum-solid interface.

Efficient and highly tunable second-harmonic generation in Z-cut periodically poled lithium niobate nanowaveguides.

Thin-film lithium-niobate-on-insulator (LNOI) has emerged as a superior integrated-photonics platform for linear, nonlinear, and electro-optics. Here we combine quasi-phase-matching, dispersion engineering, and tight mode confinement to realize nonlinear parametric processes with both high efficiency and wide wavelength tunability. On a millimeter-long, Z-cut LNOI waveguide, we demonstrate efficient (1900±500%W-1cm-2) and highly tunable (-1.71nm/K) second-harmonic generation from 1530 to 1583 nm by type-0 quasi-phase-matching. Our technique is applicable to optical harmonic generation, quantum light sources, frequency conversion, and many other photonic information processes across visible to mid-IR spectral bands.

Nanocomposite for photonics — Nickel pyrophosphate nanocrystals synthesised in silica nanoreactors

Abstract Nanophotonics is one of the most important branches of electronics. The search for and design of novel and more efficient laser-operated materials seems to be fully justified. Therefore, here, we show how to fabricate materials that have an enhanced non-linear optical response using a procedure of synthesis in a silica nanoreactor. We obtained the initial material through the precise functionalisation of SBA-15 silica using nickel phosphonate units that were anchored inside the silica channels by propyl chains, which was then transformed into an optically active nanocomposite after thermal processing. Using thermogravimetry, transmission electron microscopy (TEM), Raman vibrational analysis, and N 2 sorption analysis, we analysed the thermal behaviour of the initial functional material. All research that is connected with second- and third-order optical harmonic generation enables the structural changes in these materials and their influence on their optical properties to be explored. Nonlinear optical measurements confirmed our assumption that material that is prepared using silica nanoreactors can have precisely tailored properties, in this case, nonlinear optical properties.

Enhanced third harmonic generation from sinusoidal graphene gratings

We investigate the nonlinear optical third harmonic generation of sinusoidal curved graphene which is placed on the dielectric substrate. Under transverse magnetic polarization, the third harmonic generation (THG) from graphene is dramatically enhanced at fundamental-mode and several higher-order modes of surface plasmon of graphene. The enhancement factor of THG is up to106 compared to that from graphene on a planar dielectric. We study in detail THG intensity affected by the Fermi level of graphene, grating period and amplitude, and the angle of incidence of light. The tunable and enhanced THG response at multiple wavelengths show that the sinusoidal-shaped graphene grating has potential applications for graphene based broadband nonlinear photonics.

Structural Features of Phosphates Ca9 – xMxDy(PO4)7 (M = Zn2+ or Mg2+)

Phosphate solid solutions based on the whitlockite family Ca9 – xMxDy(PO4)7 (M = Zn2+ or Mg2+) have been obtained. The samples have been investigated by a combination of the methods, such as X‑ray diffraction analysis, second optical harmonic generation, and luminescence spectroscopy. It is established that the unit-cell symmetry change (R3c → $$R\bar {3}c$$) in the solid-solution series with an increase in the degree of substitution Ca2+ → M2+; the concentration dependence is determined. Phase transitions of the ferro- and antiferroelectric types, as well as their temperature positions, have been determined by dielectric spectroscopy. The synthesized samples exhibit strong luminescence under 350-nm excitation with the resulting radiation in the white region in color coordinates.

Co-doping effect of Amaranth and EDTA on bulk growth, optical, structural properties and second harmonic generation of KDP crystals grown by Sankaranarayanan-Ramasamy (SR) technique

KDP (Potassium dihydrogen phosphate) single crystals co-doped with Amaranth dye and EDTA (Ethylenediaminetetraacetic acid disodium salt) with concentrations of 0.005 mol% and 1 mol% respectively in the solution were grown from seeds by the method of temperature reduction and Sankaranarayanan-Ramasamy (SR) technique. The seeds were mounted vertically and in a direction of 59° from the vertical. The latter orientation of the seed made second harmonic generation (SHG) efficiency of KDP crystal with the 1064 nm laser reach its maximum value. Bulk growth, optical, and structural properties of the crystals were assessed by UV–Vis spectroscopy, X-ray diffraction (XRD) analysis, and photoluminescence. The elemental composition of crystals was also determined by Energy-dispersive X-ray (EDX) spectroscopy. Amaranth and EDTA additives have improved the SHG performance of pure KDP crystals by up to 168%, which probably could not be achieved by doping either with Amaranth or EDTA. Finally, three different parts of the crystal rods grown by SR technique were not homogeneous in the optical, structural properties and the degree of being dyed.

Optical high-order harmonic generation as a structural characterization tool

Structural characterization is essential to material engineering, but few tools can detect structural properties in the time domain. High harmonic generation (HHG) emerges as a new frontier that touches the heart of condensed-matter physics from the symmetry to quantum geometrical nature of electrons, but its capability in structural characterization has not been materialized. Here, we establish a crucial connection between the symmetry of a material and the helicity of light. We employ monolayer ${\mathrm{MoS}}_{2}$ as an example. We show that a linearly polarized laser pulse used in experiments is not ideal for structural characterization because it only generates in-plane anisotropy. It is the circularly polarized laser field that is capable of producing four distinctive HHG signals from the four phases of ${\mathrm{MoS}}_{2}$. This finally links the laser helicity to the crystal structure. The results are generic and are not affected by the Berry curvature, the interband or intraband contribution. Our study unleashes the power of HHG as a structural characterization tool for technologically important materials.

Generation of an Attosecond Pulse in Helium Excited by Half-Cycle X-Ray Pulses

Conventionally, attosecond pulses are obtained using generation of high-order optical harmonics upon excitation of various media by femtosecond laser pulses with the central frequency in the infrared range. Here, we consider theoretically an alternative possibility of obtaining an isolated extreme ultraviolet (XUV) attosecond pulse in a thin layer of helium atoms excited by a pair of half-cycle (quasi-unipolar) X-ray pulses. The approach is based on the free polarization decay of an atomic medium. An analogy of the processes under consideration with the phenomenon of superradiance is discussed.

Сегнетоэлектрические фазовые переходы в Sr-=SUB=-9-=/SUB=-Tm(VO_4)-=SUB=-7-=/SUB=- при замещении стронция на кальций и свинец

By solid-phase synthesis at 1373 K in Sr9-xMexTm (VO4)7 systems the solid solutions with Me = Ca (0≤ x≤2) and Me = Pb (0≤ x≤1) were obtained. Single-phase samples at room temperature are isostructural to the Ca3(VO4)2 ferroelectric (space group (sp.gr.) R3c, Z = 6). Substances are characterized by X-ray phase analysis (XRD), second optical harmonic generation (SHG), and dielectric spectroscopy. The intensity of the SHG signal change depending on the substitution cation and its concentration varies in the range of 30-50 units relative to the quartz standard. A reversible ferroelectric phase transition was found in the temperature range 850–960 K. The transition is accompanied by a sharp maximum in the temperature dependence of the dielectric constant. The absence of a SHG signal above the transition temperature indicates the centrosymmetry of the paraelectric phase.

Эффекты магнитного поля в экситонной генерации оптических гармоник

Mechanisms responsible for the optical harmonics generation in several classes of materials at excitonic transitions are considered. In the cubic semiconductor GaAs, magnetically induced second harmonic generation (SHG) was observed in the region of orbital quantization for the valence and conduction bands. An unusually strong third harmonic generation was detected in the region of the 1s exciton in an external magnetic field due to the exciton-polariton resonance. Magnetic field induced SHG was revealed in the hexagonal wide bandgap semiconductor ZnO at exciton resonances 1s, 2s, and 2p. Depending on the symmetry of the exciton states, the SHG mechanisms are determined by the spin and orbital Zeeman effects, and the magneto-Stark effect. Magnetically induced contribution to SHG was studied in the antiferromagnet Cr2O3 at exciton transitions in an external magnetic field.