Search Results (62)

Conducting polymer–metal nanocomposites are widely investigated as tunable photonic and optoelectronic media; however, reported property trends often remain empirical because electronic disorder at the absorption edge, refractive-index dispersion, free carrier dielectric response, and third-order nonlinearity are rarely quantified within a single, composition-controlled film series. This limitation is particularly relevant for electrochemically grown PANI coatings on transparent conductive substrates, where nanoparticle incorporation can simultaneously enhance polarization while introducing aggregation-driven heterogeneity. Here, Ag/PANI nanocomposite thin films were fabricated directly on indium tin oxide (ITO) by potentiostatic electrodeposition from an aniline/camphorsulfonic acid electrolyte containing controlled Ag nanoparticle loadings (5–15 wt.%). This study addresses the research gap by integrating complementary optical-disorder and dispersion formalisms with dielectric and nonlinear analyses to establish a composition structure optics map for device-relevant films. Ag incorporation narrows the indirect optical gap from 1.98 eV (PANI) to 1.81 eV (5 wt.%), 1.38 eV (10 wt.%), and 1.19 eV (15 wt.%), while markedly broadening the Urbach tail (0.377 eV → 1.28–1.64 eV at 5–10 wt.%). Wemple–DiDomenico modeling and Drude-type dielectric dispersion reveal strongly non-monotonic evolution of oscillator energetics and the carrier response, culminating in large bound-electron dielectric constants (ε_∞ up to 469.8) and plasma frequencies (ω_p up to 248 × 10¹² Hz) at 15 wt.% Ag. Third-order nonlinearity is substantially enhanced but composition-sensitive: χ³ increases from 6.73 × 10⁻⁹ esu (PANI) to ~7.6 × 10⁻⁸ esu at 5 and 15 wt.%, whereas the Kerr coefficient peaks at 25.91 × 10⁻⁷ esu for 5 wt.% and is suppressed at intermediate/high loading. These results demonstrate that the optimal nonlinear performance is governed by a disorder–dispersion balance and microstructure-dependent local-field effects rather than the Ag fraction alone. Full article

The cavity-less electro-optic combs (EOCs), recognized for exceptional tunability, stability and high power, are a crucial enabler for the fields such as optical communications, precision measurement and metrology, and microwave photonics. This work systematically investigates the fundamental physical factors that govern the spectral flatness via ultrafast measurements and modeling simulations. The ultrafast analysis results demonstrate that, the finite effective modulation extinction ratio of the electro-optic intensity modulators will result in generation of coherent spectral components with identical frequencies but varying phases and amplitudes in ultrashort temporal scale, finally lead to remarkable spectral interference and further intensity fluctuations across the combs spectrum. Furthermore, the established mathematical relationship between the spectral flatness and the modulation extinction ratio of the intensity modulators exhibits a nonlinear dependence up to the third order. Cascading intensity modulators has been exploited to mitigate the spectral interference and improve the modulation extinction ratio, which has been verified by using home-made high sensitive autocorrelator and frequency-resolved optical gating (FROG), and finely spectral flatness of 0.54 dB among 11 lines has been achieved, which recognized for the first time that modulation extinction ratio related spectral interference phenomenon play a subtle role in EOCs generation. Furthermore, photonic analog-to-digital converters (PADCs) have been investigated and an obvious enhancement in signal-to-noise-and-distortion (SINAD) is achieved, These findings will provide crucial theoretical and experimental support for optimizing EOCs performance, and advance the development and application. Full article

Underwater localization using airborne visible light beams offers a promising alternative to acoustic and radio-frequency methods, yet accurate modeling of light propagation through a dynamic air–water interface remains a major challenge. This paper introduces a physics-informed machine learning framework that combines geometric optics with neural network inference to localize submerged optical nodes under both flat and wavy surface conditions. The approach integrates ray-based light transmission modeling with a third-order Stokes wave formulation, enabling a realistic representation of nonlinear surface slopes and their effect on refraction. A multilayer perceptron (MLP) is trained on synthetic intensity–position datasets generated from this model, learning the complex mapping between received optical power (light intensity) and coordinates of the submerged receiver. The proposed method demonstrates high precision, stability, and adaptability across varying geometries and surface dynamics, offering a computationally efficient solution for optical localization in dynamic underwater environments. Full article

A method for the second-harmonic generation (SHG) in optical fibers by exploiting the third-order nonlinearity under an external electric field is proposed. The analysis begins with the electric polarization vector of the SHG, and the analytical solution for the SHG is presented. When fiber birefringence is neglected, a mode-field matching condition is introduced. The nonlinearity-induced shift in propagation constant is provided based on Gaussian approximation. For a specific case, the power of SHG is calculated. The results show that the SHG power scales quadratically with the nonlinear coefficient. Reducing the effective area of the fiber and increasing the nonlinear coefficient can enhance the SHG power by 1–2 orders of magnitude. Since phase matching strongly affects the SHG process, optimizing the fiber design is crucial. Additionally, the polarization state of SHG is shown to have the same as the equivalent optical field of the injected fundamental wave. This work demonstrates potential for distributed sensing of electric fields and lightning events in high-voltage power grids using optical fibers. Full article

Miller’s rule originated as an empirical relation between the nonlinear and linear optical coefficients of materials. It is now accepted as a useful tool for guiding experiments and computational materials discovery, but its theoretical foundation had long been limited to a derivation for the classical Lorentz model with a weak anharmonic perturbation. Recently, we developed a mathematical framework which enabled us to prove that Miller’s rule is equally valid for quantum anharmonic oscillators, despite different dynamics due to zero-point fluctuations and further quantum-mechanical effects. However, our previous derivation applied only to one-dimensional oscillators and to the special case of second- and third-harmonic generation in a monochromatic electric field. Here we extend the proof to three-dimensional quantum anharmonic oscillators and also treat all orders of the nonlinear response to an arbitrary multi-frequency field. This makes the results applicable to a much larger range of physical systems and nonlinear optical processes. The obtained generalized Miller formulae rigorously express all tensor elements of the frequency-dependent nonlinear susceptibilities in terms of the linear susceptibility and thus allow a computationally inexpensive quantitative prediction of arbitrary parametric frequency-mixing processes from a small initial dataset. Full article

There has been considerable scientific interest in third-order nonlinear optical materials for photonic applications. In particular, materials exhibiting a strong electronic optical Kerr effect serve as essential components in the ultrafast nonlinear photonic devices and are instrumental in the development of all-optical signal processing technologies. Therefore, the accurate prediction of material-relevant properties, such as second hyperpolarizabilities, remains a key topic in the search for efficient photonic materials. However, the field standards in quantum chemical computation are still inconsistent, as studies often lack a firm statistical foundation. This work presents a comprehensive in silico investigation based on multiple full-factorial experiments, aiming to clarify the strengths and limitations of various computational approaches. Our results indicate that the coupled-cluster approach at the CCSD level in its current response-equation implementations is not yet able to outperform the range-separated hybrid density functionals, such as LC-BLYP(0.33). The exceptional performance of the specifically tailored basis set Sadlej-pVTZ is also described. Not only was the presence of diffuse functions found to be mandatory, but also adding ample polarization functions is shown to be inefficient resource-wise. HF/Sadlej-pVTZ is proven to be reliable enough to use in molecular screening. Meta functionals are confirmed to produce poorly consistent results, and specific guidelines for constructing range-separated functionals for polarizability calculations are drawn out. Additionally, it was shown that many of the contemporary solvation models exhibit significant limitations in accurately capturing nonlinear optical properties. Therefore, further refinement in the current methods is pending. This extends to the statistical description as well: the mean absolute deviation descriptor is found to be deficient in rating various computational methods and should rather be replaced with the parameters of the linear correlation (the slope, the intercept, and the R²). Full article

This study investigates the influence of vacancy engineering and nitrogen doping on the structural, electronic, and optical properties of T-graphene fragments (TFs) using density functional theory (DFT) and time-dependent DFT (TD-DFT). A central vacancy and five pyridinic nitrogen doping configurations are explored to modulate the optoelectronic behavior. All systems are thermodynamically stable, exhibiting tunable HOMO–LUMO gaps, orbital distributions, and charge transfer characteristics. Optical absorption spectra show redshifts and enhanced oscillator strengths in doped variants, notably v-NTF2 and v-NTF4. Nonlinear optical (NLO) analysis reveals significant enhancement in both static and frequency-dependent responses. v-NTF2 displays an exceptionally high first-order hyperpolarizability (⟨β⟩ = 1228.05 au), along with a strong electro-optic Pockels effect (β (−ω; ω, 0)) and second harmonic generation (β (−2ω; ω, ω)). Its third-order response, γ (−2ω; ω, ω, 0), also exceeds 1.2 × 10⁵ au under visible excitation. Conceptual DFT descriptors and energy decomposition analysis further supports the observed trends in reactivity, charge delocalization, and stability. These findings demonstrate that strategic nitrogen doping in vacancy-engineered TFs is a powerful route to tailor electronic excitation, optical absorption, and nonlinear susceptibility. The results offer valuable insight into the rational design of next-generation carbon-based materials for optoelectronic, photonic, and NLO device applications. Full article

This study synthesizes and comparatively investigates two squaric acid-based phthalocyanine-like dyes, SNF and its long-chain alkylated derivative LNF, to systematically elucidate the influence of peripheral hydrophobic groups on their third-order nonlinear optical (NLO) properties. The NLO characteristics were comprehensively characterized using femtosecond Z-scan and I-scan techniques at both 800 nm and 900 nm. Both dyes exhibited strong saturable absorption (SA), confirming their potential as saturable absorbers. Critically, the comparative analysis revealed that SNF exhibits a significantly greater nonlinear absorption coefficient (β) compared to LNF under identical conditions. For instance, at 800 nm, the β of SNF was approximately 3–5 times larger than that of LNF. This result conclusively demonstrates that the introduction of long hydrophobic alkyl chains attenuates the NLO response. Furthermore, I-scan measurements revealed excellent SA performance, with high modulation depths (e.g., LNF: 43.0% at 900 nm) and low saturation intensities. This work not only clarifies the structure–property relationship in these D-A-D dyes but also presents a clear strategy for modulating the NLO properties of organic chromophores for applications in near-infrared pulsed lasers. Full article

This study explores the (1+1)-dimensional Klein–Fock–Gordon equation, a distinct third-order nonlinear differential equation of significant theoretical interest. The Klein–Fock–Gordon equation (KFGE) plays a pivotal role in theoretical physics, modeling high-energy particles and providing a fundamental framework for simulating relativistic wave phenomena. To find the exact solution of the proposed model, for this purpose, we utilized two effective techniques, including the sine-Gordon equation method and a new extended direct algebraic method. The novelty of these approaches lies in the form of different solutions such as hyperbolic, trigonometric, and rational functions, and their graphical representations demonstrate the different form of solitons like kink solitons, bright solitons, dark solitons, and periodic waves. To illustrate the characteristics of these solutions, we provide two-dimensional, three-dimensional, and contour plots that visualize the magnitude of the (1+1)-dimensional Klein–Fock–Gordon equation. By selecting suitable values for physical parameters, we demonstrate the diversity of soliton structures and their behaviors. The results highlighted the effectiveness and versatility of the sine-Gordon equation method and a new extended direct algebraic method, providing analytical solutions that deepen our insight into the dynamics of nonlinear models. These results contribute to the advancement of soliton theory in nonlinear optics and mathematical physics. Full article

The optical and radiation shielding of PVA have been enhanced through embedding with ZnO/CuO/SWCNT (ZCS) nanocomposites. ZCS polymeric nanocomposites (PNCs) were prepared with the solution casting method. Scanning electron, optical microscopy and FT-IR procedures were performed to examine the surfaces’ morphology and structures’ modifications. UV–visible measurements were carried out to investigate the linear/nonlinear optical properties. The optical investigations show significant alterations in the optical parameters of PVA due to ZCS embedding. The UV–visible analysis shows that the optical parameters, including the transmittance, energy bandgap, refractive index, dielectric constants and optical conductivity of PVA, are tuned through ZCS embedding. The direct and indirect bandgap of PVA shrank from 5.42 eV and 4.99 eV (neat PVA) to 3.20 eV and 2.26 eV (10 wt.% ZCS PNCs). The nonlinear optical (NLO) constants (first order susceptibility (χ⁽¹⁾), third susceptibility (χ⁽³⁾) and refractive index (n₂)) of PVA were improved. Phy-X/PSD software was used to investigate the radiation shielding parameters of all samples. The linear attenuation coefficient (LAC), mean free path (MFP), half value layer (HVL), tenth value layer (TVL) and effective atomic number (Z_eff) of PVA were enhanced through ZCS embedding. It is found that the mass attenuation coefficient (MAC) of the neat PVA increased from 1.14 cm²/g to 7.96 cm²/g at 0.015 MeV. The HVL of PVA decreased from 30.2 cm to 20.6 cm, the TVL decreased from 100.3 cm to 68.5 cm and the MFP decreased from 43.6 cm to 29.8 cm upon embedding 10 wt.% of ZCS NCs at 15 MeV. The samples’ exposure buildup factor (EBF) and energy absorption buildup factor (EABF) in the photon energy range from 0.015 MeV to 15 MeV at 0.5 to 40 MFP values. This study proves that ZCS PNCs are advantageous for applications in optical and radiation shielding fields. Full article

Bismuth telluride (Bi₂Te₃) has attracted significant attention due to its broadband ultrafast optical response and strong nonlinearity at high laser fluence in the field of optoelectronic materials. The objective of this work is to study the effect of Al doping on the structure, linear optical properties, and nonlinear optical absorption behavior of Bi₂Te₃ thin films. The amorphous Al-doped Bi₂Te₃ thin films with varying Al doping concentrations were prepared using magnetron co-sputtering. The structure and linear optical properties were characterized using X-ray diffraction, scanning electron microscopy, energy-dispersive X-ray spectroscopy, X-ray photoelectron spectroscopy, spectroscopic ellipsometry, and UV/Vis/NIR spectrophotometry. The third-order nonlinear optical absorption properties of Al: Bi₂Te₃ thin films were investigated using the open-aperture Z-scan system with a 100 fs laser pulse width at a wavelength of 800 nm and a repetition rate of 1 kHz. The results indicate that Al dopant reduces both the refractive index and extinction coefficient and induces a redshift in the optical bandgap. The optical properties of the films can be effectively modulated by varying the Al doping concentration. Compared with undoped Bi₂Te₃ thin films, Al-doped Bi₂Te₃ thin films exhibit larger nonlinear optical absorption coefficients and higher damage thresholds and maintaining high transmittance. These findings provide experimental evidence and a reliable approach for the further optimization and design of ultrafast nonlinear optical devices. Full article

In recent years, the fabrication of materials with large nonlinear optical coefficients and the investigation of methods to enhance nonlinear optical performance have been in the spotlight. Herein, the bismuth telluride (Bi₂Te₃) thin films were prepared by radio-frequency magnetron sputtering and annealed in vacuum at various temperatures. The structural and optical properties were characterized and analyzed using X-ray diffraction, scanning electron microscopy, X-ray photoelectron spectroscopy, spectroscopic ellipsometry, and UV/VIS/NIR spectrophotometry. The third-order optical nonlinearities of Bi₂Te₃ thin films were investigated using the Z-scan technique, employing a 100 fs pulse width at an 800 nm wavelength. It is found that the crystallinity and the average grain size of the films increase with the annealing temperature. Meanwhile, the extinction coefficient of the annealed films increased, accompanied by a redshift in the optical bandgap. All samples exhibit pronounced saturable absorption and self-focusing behaviors. The nonlinear absorption coefficient and nonlinear refractive index of Bi₂Te₃ films annealed at 300 °C were found to be 2.44 times and 1.85 times higher than those of the as-deposited films, respectively. These findings demonstrate that annealing treatment is an effective approach to tuning the crystalline structure and linear optical properties of Bi₂Te₃ films while simultaneously enhancing their nonlinear optical performance. Full article

In this report, the nonlinear optical (NLO) properties of titanium dioxide nanoparticles (TiO₂ NPs) have been explored experimentally using femtosecond laser light along with the Z-scan approach. The synthesis of TiO₂ NPs was carried out in distilled water through nanosecond second harmonic Nd:YAG laser ablation. Characterization of the TiO₂ NPs colloids was conducted using UV-visible absorption spectroscopy, transmission electron microscopy (TEM), inductively coupled plasma (ICP), and energy-dispersive X-ray spectroscopy (EDX). The TEM analysis indicated that the size distribution and average particle size of the TiO₂ NPs varied from 8.3 nm to 19.1 nm, depending on the laser ablation duration. The third-order NLO properties of the synthesized TiO₂ NPs were examined at different excitation laser wavelengths and incident powers through both open- and closed-aperture Z-scan techniques, utilizing a laser pulse duration of 100 fs and a high repetition rate of 80 MHz. The nonlinear absorption (NLA) coefficient and nonlinear refractive (NLR) index of the TiO₂ NPs colloidal solutions were found to be influenced by the incident power, excitation wavelength, average size, and concentration of TiO₂ NPs. Maximum values of 4.93 × 10⁻⁹ cm/W for the NLA coefficient and 15.39 × 10⁻¹⁵ cm²/W for the NLR index were observed at an excitation wavelength of 800 nm, an incident power of 0.6 W, and an ablation time of 15 min. The optical limiting (OL) effects of the TiO₂ NPs solution at different ablation times were investigated and revealed to be concentration and average size dependent. An increase in concentration results in a more limiting effect. Full article

Spherical quantum wells (SQWs) have proven to be excellent materials for suppressing Auger recombination due to their expanded confinement volume. However, research on the factors and mechanisms of their high-intensity optical properties, such as multiexciton properties and third-order optical nonlinearities, remains incomplete, limiting further optimization of these properties. Here, a series of CdS/CdSe (xML)/CdS SQWs with varying CdSe layer thicknesses were prepared. The modulation effects of CdSe shell variations on the PL properties, defect distribution, biexciton binding energy, and third-order optical nonlinearities of the SQWs were investigated, and their impact on the material’s multiexciton properties was further analyzed. Results showed that the typical CdS/CdSe(3ML)/CdS sample exhibited a large volume-normalized two-photon absorption cross-section (18.17 × 10² GM/nm³) and favorable biexciton characteristics. Optical amplification was observed at 12.4 μJ/cm² and 1.02 mJ/cm² under one-photon (400 nm) and two-photon (800 nm) excitation, respectively. Furthermore, different amplified spontaneous emission spectra were observed for the first time under one/two-photon excitation. This phenomenon was attributed to thermal effects overcoming the biexciton binding energy. This study provides valuable insights for further optimizing multiexciton gain characteristics in SQWs and developing optical gain applications. Full article

Simultaneous interrogation of pump and probe beams interacting in ZnO nanostructures of a two-wave mixing is proposed for dual-path data processing of optical signals by nonlinear optical effects. An enhancement in third-order nonlinear optical properties was exhibited by Al-doped ZnO thin films. Multiphoton absorption and nonlinear refraction were explored by the z-scan technique at 532 nm with nanosecond pulses. The evolution of the optical Kerr effect in the ZnO thin films was analyzed as a function of the incorporation of Al in the sample by a vectorial two-wave mixing method. Electrical and photoconductive effects were evaluated to further characterize the influence of Al in the ZnO solid samples. Potential applications of nonlinear optical parameters for encoding and encrypting information in light can be envisioned. Full article