Nonlinear Susceptibility Research Articles

Medium Amplitude Field Susceptometry (MAFS) for magnetic nanoparticles

The linear dynamic susceptibility is arguably the most important property to specify the magnetization dynamics of a given system. Therefore, this quantity has been studied in great detail and the corresponding measurements known as susceptometry are well-established. Notwithstanding its relevance, the linear susceptibility is inherently limited to describe the magnetization response to weak external fields only. Here, we suggest the framework of Medium Amplitude Field Susceptometry (MAFS) to study the non-linear response which complements the linear susceptibility and provides additional information on the magnetic properties of the system and is applicable to magnetic fields of medium amplitudes. In particular, we introduce the general third-order nonlinear susceptibility χˆ3 as a central quantity that completely specifies the lowest-order non-linear response to arbitrary time-dependent magnetic fields. We show that response functions in medium amplitude oscillatory magnetic fields and parallel superposition susceptometry are contained in χˆ3 as special cases. Also included in χˆ3 are interesting intermodulation effects when the system is probed by a superposition of oscillating magnetic fields with different frequencies. We work out the explicit form of χˆ3 for several model systems for the dynamics of magnetic nanoparticles (MNPs). We expect this unifying framework to be not only of theoretical interest, but also useful for a deeper characterization of MNP systems, giving additional information on their suitability for various applications.

Unusual spin dynamics in the van der Waals antiferromagnet FeGa2S4

Spin dynamics in the van der Waals antiferromagnet FeGa2S4with triangular lattices are investigated using magnetometry, neutron scattering, and muon spin relaxation measurements. The characteristic spin relaxation time is thoroughly clarified over thirteen orders of magnitude. Although the temperature dependence of DC and AC susceptibilities recalls a conventional spin-glass transition, nonlinear susceptibilities showing no divergences at the anomalous temperature,T∗=16.87(7) K, deny that and instead hint at other mechanisms. Elastic neutron scattering together with previously measured muon results depict a slowly fluctuated (∼10-5 s) spin state aboveT∗. In juxtaposing the underlying simplest structure among frustrated magnets with an intricate hierarchy of time scales, FeGa2S4can be a playground for studying temporal spin correlations in the two-dimensional limit.

Designing a 2D van der waals oxide with lone-pair electrons as chemical scissor

Abstract 2D van der Waals (vdW) materials are known for their intriguing physical properties, but their rational design and synthesis remain a great challenge for chemists. In this work, we successfully synthesized a new non-centrosymmetric oxide, i.e. InSbMoO6, with Sb3+ lone-pair electrons serving as chemical scissor to generate its 2D vdW crystal structure. Monolayer and few-layer InSbMoO6 flakes are readily obtained via facile mechanical exfoliation. They exhibit strong second-harmonic generation (SHG) response with an effective second-order nonlinear optical susceptibility $\chi _{{\rm{eff}}}^{{\rm{(2)}}}\ $of 32.4 pm·V−1. Meanwhile, the SHG response is in-plane anisotropic and directly proportional to the layer thickness, independent of layer parity. In addition, the InSbMoO6 flakes exhibit excellent thermal and atmospheric stability, along with pronounced anisotropy in Raman spectroscopy. This work implies that using lone-pair electrons as chemical scissor is an effective strategy for designing and synthesizing new 2D vdW materials for integrated photonic applications.

Impact of gamma irradiation on optical and nonlinear properties of Indium chloride phthalocyanine thin films

This study investigates the impact of gamma radiation on indium chloride phthalocyanine (lnPcCl) thin films, which were prepared via vacuum thermal evaporation. x-ray diffraction revealed the amorphous structure of the films, with increasing gamma doses causing more noticeable structural disorders. Optical analysis showed a slight decrease in the optical band gap energy and a significant reduction in the fundamental band gap energy. Additionally, higher gamma doses led to decreased transmittance and increased reflectance. The study also observed substantial enhancements in nonlinear optical parameters, such as third-order nonlinear susceptibility (χ(3)) and nonlinear refractive index (n 2). These findings suggest the potential of gamma-irradiated lnPcCl films for advanced optoelectronic and nonlinear optical applications.

Study on UV-VIS characteristics of Aluminum Zinc Oxide nanoparticles through manganese substitution using Wemple-Di domenico method and diffuse reflectance spectroscopy

In this research Manganese-substitution impact on linear and nonlinear (NL) optical properties of Aluminum-doped ZnO (AlZnO) Nanoparticles (NPs) are investigated. Utilizing measured data of reflectance acquired from the DRS, the higher-order NL optical characteristics of the provided NPs are examined. The maximum quantity of NL susceptibility χ3 is measured to be around 3.945 × 10−10 esu at wavelength λ = 520 nm and 7.467 × 10−11 esu at wavelength λ = 530 nm for AlZnO and Manganese-substituted Aluminum-doped Zinc-Oxide (Mn-also) NPs, for particle sizes 14−67 nm and 11−54 nm, consecutively. Consequently, the synthesis method (sol–gel) which is used in this work concluded a decrease in particle size and different optical behavior especially in UV spectral regions during the substitution with Manganese in comparison with the AlZnO. This decrement assures that a decrease in the size of crystallite induces a decline in the χ3. The obtained optical parameters are red shifted with the Manganese substitution. Also, the NL absorption coefficient (β c(m/W)) is enhanced in the UV range. The maximum of the NL absorption coefficient (β c(m/W)), for AlZnO and Mn-AlZnO NPs, are determined (at λ = 250 nm) 2.24 × 10−18 (m/W) and 5.76 × 10−15 (m/W) respectively.

Recursive algorithm for generating high-temperature expansions for spin systems and the chiral nonlinear susceptibility

Recursive algorithm for generating high-temperature expansions for spin systems and the chiral nonlinear susceptibility

Core-shell nanomaterials based on La2FeCrO6 coated with metal oxides for optical applications

In this research work, the preparation of core/shell nanoparticles comprising La2FeCrO6 (LFCO) as the core was accompanied by the choice of ZnO and CuO as different shells. Structural and optical characteristics were investigated for the LFCO (core) relative to La2FeCrO6/ZnO and La2FeCrO6/CuO core/shell NPs. x-ray diffraction analyses reveal the conformation of core/shell structures within average crystallite sizes of 22.46 nm and 25.03 nm. Raman spectroscopy and Fourier-transform infrared spectroscopy (FTIR) were performed to provide fundamental information about the vibrational modes and the functional groups of core/shell NPs, respectively. x-ray photoelectron spectroscopy (XPS) detects the electronic states of the constituent elements of the core/shell nanostructures, including lanthanum, iron, chromium, oxygen, zinc, and copper. Optical characteristics have been extensively analyzed using UV spectroscopy. The energy gap (Eg) was determined by utilizing both Tauc and Derivation of Absorbance Spectrum Fitting (DASF) methods. LFCO/ZnO and LFCO/CuO core/shell NPs exhibit a direct optical transition, similar to that of the core LFCO NPs, with a decrease in band gap value from 3.4 eV for the core to 3.3 eV and 3.18 eV for LFCO/ZnO and LFCO/CuO core/shell NPs respectively. The enhanced transparency of core/shell NPs, particularly at longer wavelengths, is evident from the decrease in refractive index (n) compared to that of the core (LFCO) NPs. This decrease is attributed to the encapsulation of LFCO with either ZnO or CuO NPs. The samples exhibit a decline in both linear and non-linear optical susceptibilities with respect to the square of photon energy. The LFCO/CuO sample shows excellent results in the photocatalytic degradation of aqueous organic dyes, considering it a promising candidate for wastewater treatment and the removal of organic pollutants.

Nonlinear geometric phase coded ferroelectric nematic fluids for nonlinear soft-matter photonics

Simultaneous manipulation of multiple degrees of freedom of light lies at the heart of photonics. Nonlinear wavefront shaping offers an exceptional way to achieve this goal by converting incident light into beams of new frequencies with spatially varied phase, amplitude, and angular momenta. Nevertheless, the reconfigurable control over structured light fields for advanced multimode nonlinear photonics remains a grand challenge. Here, we propose the concept of nonlinear geometric phase in an emerging ferroelectric nematic fluid, of which the second-order nonlinear susceptibility carries spin-dependent nonlinearity phase. A case study with photopatterned q-plates demonstrates the generation of second-harmonic optical vortices with spin-locked topological charges by using cascaded linear and nonlinear optical spin-orbit interactions. Furthermore, we present the dynamic tunability of second-harmonic structured light through temperature, electric field, and twisted elastic force. The proposed strategy opens new avenues for reconfigurable nonlinear photonics, with potential applications in optical communications, quantum computing, high-resolution imaging, etc.

On‐Demand Generation and Control of Giant Terahertz Nonlinearity with Metasurfaces

AbstractSimultaneous control of the optical linearity and nonlinearity of the materials plays key roles in next‐generation electronics and optics as it offers the potential of manipulating the fundamental properties while generating new frequencies of light. Such control is exceedingly challenging at the technologically important terahertz (THz) frequencies due to the severe scarcity of high‐performance nonlinear materials. Here, a unique method is introduced for achieving THz second‐order nonlinearity through Lorentz force‐driven anharmonic oscillations of free electrons in metasurfaces. It does not depend on natural nonlinear materials and provides ultrahigh design freedom. Using this approach, efficient THz second harmonic generation (SHG) is experimentally demonstrated with remarkably large values of the effective nonlinear susceptibility at room temperature. By engineering the geometry of the metasurfaces, the generation and suppression of the second harmonics can be controlled and customize their polarization states at will. This efficient, configurable, room‐temperature, and ultra‐compact platform for THz SHG provides new perspectives for developing high‐performance THz sources, frequency multipliers, and other nonlinear devices.

Magnetic field-engineered optical nonlinearity in germanene nanotubes

Abstract The linear and nonlinear optical properties of germanene nanotubes (GeNTs) under the influence of magnetic fields are investigated through theoretical analysis. By employing a tight-binding model beyond the Dirac cone approximation, the electronic band structure, density of states, dipole matrix elements, and third-order nonlinear optical susceptibilities are calculated. The application of a magnetic field induces a Zeeman splitting of the energy levels, breaking the band degeneracy. Consequently, the dipole matrix elements exhibit a magnetic field dependence, altering the intensity and number of allowed transitions. In the infrared and ultraviolet energy regions, the linear optical absorption spectrum displays the splitting of peaks into dual neighboring peaks, with the splitting distance linearly dependent on the magnetic field strength. The third-order nonlinear optical susceptibilities, χTHG(3)3ω and χIDIR(3)ω, reveal the emergence of multiple resonance peaks in different energy regions due to two-photon and three-photon absorption processes. The magnetic field significantly influences the number, position, and height of these optical peaks, enabling effective control over the nonlinear optical response. By investigating the scaled energy (E/E_g) dependence, a universal behavior is observed for the three- and two photon resonance peaks, where their positions remain constant, but their peak intensities are significantly enhanced under the influence of the magnetic field. These findings demonstrate the potential of GeNTs as tunable nonlinear optical materials, with the magnetic field serving as an effective parameter for engineering their optical properties for various applications in optoelectronics, photonics, and related fields.

Flexible and innovative PVA/ZrO2/g-C3N4/CNT nanocomposites film for optoelectronic applications

This study successfully prepared polyvinyl alcohol (PVA) polymer films doped with ZrO2/(g-C3N4/CNT) nanofillers using the solution casting technique. The crystal structure of the nanocomposite films was characterized by X-ray diffraction (XRD), revealing the semi-crystalline nature of PVA and an average ZrO2 crystallite size of 13.17 nm. Fourier-transform infrared (FTIR) spectroscopy confirmed the chemical composition and functional groups present in the nanocomposites. Scanning electron microscopy (SEM) and energy-dispersive X-ray (EDX) analysis showed uniform dispersion of the nanofillers without noticeable phase separation, with EDX confirming the successful incorporation of ZrO2, g-C3N4, and CNT into the PVA matrix. X-ray photoelectron spectroscopy (XPS) further validated the elemental composition and chemical states, indicating the presence of carbon, oxygen, nitrogen, and zirconium. Optical analysis demonstrated that increasing ZrO2/(g-C3N4/CNT) content reduced the direct and indirect band gaps from 5.41 eV to 5.25 eV and from 5.18 eV to 4.92 eV, respectively. In addition, the single-oscillator energy (E0) and dispersion energy (Ed) increased, while the static refractive index (n0) decreased. Improvements were also observed in linear optical susceptibility (χ(1)) and third-order nonlinear optical susceptibility (χ(3)), enhancing the polarizability of the polymer molecules. These results indicate that PVA films doped with ZrO2/(g-C3N4/CNT) hold promise for optoelectronic applications due to their enhanced optical properties.

Robust adaptive dynamic control of electromagnetically actuated soft-tethered robots for medical intervention

Electromagnetically actuated soft-tethered robots (EASTRs) exhibit significant potential for medical intervention applications due to their compact size and minimal invasiveness. However, their inherent nonlinear behavior and susceptibility to unexpected disturbances present challenges for achieving robust control performance. To address this issue, in this paper, a dynamic model for EASTRs is first established, which encompasses the actuation model of the magnetic tip and the dynamic model of the soft tether. Subsequently, a robust adaptive dynamic controller is designed to compensate for the inaccuracy of the established dynamic model, thus ensuring robust control performance. The proposed approach integrates adaptive laws based on the Lyapunov method to effectively handle time-varying parameters and disturbances. Experimental results present an excellent control accuracy of the proposed scheme in trajectory tracking tasks, showcasing its superior performance compared to passive schemes and classical proportional–derivative control. This research contributes valuable insights into advancing the control capabilities of EASTRs for diverse applications in medical practices.

Substrate Interference and Strain in the Second-Harmonic Generation from MoSe2 Monolayers.

Nonlinear optical materials of atomic thickness, such as non-centrosymmetric 2H transition metal dichalcogenide monolayers, have a second-order nonlinear susceptibility (χ(2)) whose intensity can be tuned by strain. However, whether χ(2) is enhanced or reduced by tensile strain is a subject of conflicting reports. Here, we grow high-quality MoSe2 monolayers under controlled biaxial strain created by two different substrates and study their linear and nonlinear optical responses with a combination of experimental and theoretical approaches. Up to a 15-fold overall enhancement in second-harmonic generation (SHG) intensity is observed from MoSe2 monolayers grown on SiO2 when compared to its value on a Si3N4 substrate. By considering an interference contribution from different dielectrics and their thicknesses, a factor of 2 enhancement of χ(2) was attributed to the biaxial strain: substrate interference and strain are independent handles to engineer the SHG strength of non-centrosymmetric 2D materials.

Exact Solutions and Qualitative Analysis of the Stochastic Model for Embedded Solitons with $$\chi ^{(2)}$$ and $$\chi ^{(3)}$$ Nonlinear Susceptibilities

Exact Solutions and Qualitative Analysis of the Stochastic Model for Embedded Solitons with $$\chi ^{(2)}$$ and $$\chi ^{(3)}$$ Nonlinear Susceptibilities

Exploring nonlinear optical properties of RbPbI3 nanorods using SSPM technique: Implications for all-optical switching applications

Nowadays, nanomaterials' nonlinear optical (NLO) properties are a fascinating topic for developing a novel all-optical switching application. Spatial self-phase modulation (SSPM) is an important technique to determine the laser-induced coherent light-matter interaction to determine the NLO properties of nanomaterials. This study successfully synthesized RbPbI3 nanorods (NRs) via a low-cost, less complicated chemical route with all the basic characterizations to confirm its structural and compositional analysis. For the first time, we conducted a comprehensive analysis of the nonlinear refractive index (n2) and third-order susceptibility (χ(3)) for RbPbI3 NRs dissolved in two different solvents, namely N-Methyl-2-pyrrolidone (NMP) and 2-propanol, utilizing the SSPM technique. Our investigation revealed significant nonlinear optical (NLO) responses with n2 = 6.19 × 10−5 cm2 W−1 and χmonolaer(3) = 2.38 × 10−8 esu for RbPbI3. We elucidated the factors contributing to this pronounced NLO behaviour, including variations in parameters such as solvent type, viscosity, wavelength, and cuvette length. Additionally, we successfully demonstrated optical information transfer through an all-optical switching application. This research sheds light on the NLO properties of Perovskite materials and holds promise for the development of advanced all-optical device applications.

Nonlinear optical parameters and electronic properties of plasma polymerized methyl acrylate thin films

Plasma polymerized methyl acrylate (PPMA) thin films were fabricated on a borosilicate glass substrate at a plasma power of 28 W to study nonlinear optical parameters and electronic properties. X-ray Diffraction analysis confirmed the amorphous nature of the PPMA films, while Attenuated total reflectance Fourier transform infrared spectroscopy indicated monomer fragmentation due to plasma polymerization. Field emission scanning electron microscope images of the films display a water wave-like structure. PPMA films demonstrated thermal stability up to approximately 574 K in both N2 and air environments. The values of direct band gap energies increase from 3.30 to 3.41 eV with increasing film thicknesses, whereas the Urbach energy values show in an opposite manner. The Wemple-DiDomenico model was employed to analyze both the oscillator energies ranging from 5.54 to 6.44 eV and the dispersion energies ranging from 10.56 to 12.89 eV. The static linear refractive index showed typical dispersion behavior, with film thickness conforming to Moss's rule. The nonlinear refractive index and 2nd and 3rd order nonlinear susceptibilities decrease with increasing the studied films. The lattice dielectric constant values exceeded the high-frequency dielectric constant, indicating the presence of lattice vibrations and free carriers. Electronic parameters are fluctuating with increasing film thickness. The observed changes in nonlinear optical parameters and electronic properties highlight the potential of PPMA films for applications in photovoltaic and optoelectronics.

Moiré photonic superlattice-induced transparency at commensurate angle in a terahertz metasurface composed of triple layer square lattices

The control of the speed of terahertz waves is always a challenge since the bandgap of most optical materials is much larger beyond meV with subtle nonlinear susceptibility. Moiré metasurfaces are shown to exhibit wide tunable optical properties and extraordinary physical phenomena at specific commensurate angles. These can be achieved by a careful design of the metasurface to manipulate terahertz slow light. Herein, we demonstrate a triple layer Moiré metasurface with a distinct electromagnetically induced transparency (EIT) phenomenon at commensurate angles. The proposed metasurface is composed of an intrinsic square lattice embedded into another Moiré photonic superlattice made of twisted square lattice at commensurate angles of 10.39° and 7.63°. The coupling between adjacent meta-atoms on the combined metasurface leads to destructive interference of dual trapped lattice modes, which results in a transparency window at the terahertz band. A maximum group delay of 9.76 ps is found at the transparent window of 0.84 THz when the commensurate angle is 10.39°. When the commensurate angle reduces to 7.63°, the transparency window shifts to 0.57 THz with a 5.96 ps group delay. The coupled Lorentz oscillator model indicates that the nonlinear optical susceptibility at transparency windows is above zero. Our results create an approach to tune the EIT as well as slow light in the terahertz band. Our device can have potential applications in terahertz signal processing and storage.

Optical properties of transition metals complex films derived from hydrazone oxime for optoelectronic devices

Hydrazone incorporating oxime nucleus and its Ni2+, Mn2+, Zn2+ and UO22+ metallic chelates have been prepared and completely characterized by different spectral, theoretical, and analytical techniques including NMR, FT-IR, mass, and EAS spectroscopy. The finding denoted that the Hydrazone ligand bonded as a dibasic tridentate chelator via deprotonated oximato nitrogen, enol carbonyl oxygen and hydrazono azomethine nitrogen atoms resultant in octahedral geometry for Ni2+, Mn2+, Zn2+ and UO22+. Theoretical studies by DFT/B3LYP/LANLDZ together with dipole moment, geometrical optimization, energetic parameters, and energy gap (HOMO–LUMO) were employed to support the geometrical structure of the synthetics. Additionally, these complexes were prepared in the form of thin film onto cleaned glass substrate by spin-coating technique. The values of the optical band gap (Eg) and film index of refraction (n) have been determined by many different methods. It was found that the hydrazone-oxime (OBBH2) film has the highest value of Eg (eV) where the UOBB complex film has the smallest value of Eg (2.56 eV). The latter is very close to the Eg value of ZnSe (2.58 eV). The refractive index changes with wavelengths show normal dispersion which is well discussed in terms of Sellmeier's dispersion model. Also, the nonlinear optical parameters viz. the first (χ(1)) and third (χ(3)) orders of nonlinear optical susceptibilities and the non-linear index of refraction (n2) have been studied. The complex dielectric constant (ε⌣=εr+iεi)), conductivity (σ⌣=σr+iσi), sheet resistance (Rs), and thermal have been investigated over the whole spectral range. According to the results of χ(1), χ(3) and n2 the complex films under study are candidates to be used in optical switching gadgets, optical modulators, and optical signal processing.

Adaptive Variational Quantum Computing Approaches for Green's Functions and Nonlinear Susceptibilities.

We present and benchmark quantum computing approaches for calculating real-time single-particle Green's functions and nonlinear susceptibilities of Hamiltonian systems. The approaches leverage adaptive variational quantum algorithms for state preparation and propagation. Using automatically generated compact circuits, the dynamical evolution is performed over sufficiently long times to achieve adequate frequency resolution of the response functions. We showcase accurate Green's function calculations using a statevector simulator on classical hardware for Fermi-Hubbard chains of 4 and 6 sites, with maximal ansatz circuit depths of 65 and 424 layers, respectively, and for the molecule LiH with a maximal ansatz circuit depth of 81 layers. Additionally, we consider an antiferromagnetic quantum spin-1 model that incorporates the Dzyaloshinskii-Moriya interaction to illustrate calculations of the third-order nonlinear susceptibilities, which can be measured in two-dimensional coherent spectroscopy experiments. These results demonstrate that real-time approaches using adaptive parametrized circuits to evaluate linear and nonlinear response functions can be feasible with near-term quantum processors.

Synthesis, growth and nonlinear optical properties of imidazolium hydrogen adipate monohydrate single crystal

A single crystal of Imidazolium Hydrogen Adipate Monohydrate (IHAM) has been obtained by the slow evaporation technique. The grown crystal belongs to the Triclinic crystal system. The spectral studies were further used to confirm the structure. The Hirshfeld analysis suggests that the major bonding in the crystal occurs through the Hydrogen atom constituting 69 % of the total bonding. The Void analysis shows a lower percentage of voids suggesting that the crystal is strongly packed. The optical constants such as optical and electrical conductivity, optical susceptibility and extinction coefficient were elucidated from the UV–Vis-NIR analysis. The refractive index of IHAM was determined to be 1.391 by the Prism Coupler. The work-hardening coefficient of the title compound was found to be 1.14 which classifies the material as hard. The hardness number shows the normal Indentation Size Effect (ISE). The electrical characteristics were studied by using the dielectric analyser. The solid-state parameters such as the Fermi gap, Penn gap and optical electronegativity were calculated based on the dielectric parameters. The electronic polarizability calculated by different methods is in mutual agreement. The TG/DTA analysis suggests that the material is suitable for applications up to 79 °C. The Z-Scan analysis confirms the Reverse Saturable Absorption behaviour. The third-order nonlinear susceptibility was calculated as 9.77×10−9 esu.