Nonlinear Optical Absorption Coefficients Research Articles

Kerr coefficient and third-order nonlinear optical absorption coefficient of isotropic diacrylate mesogens at 632.8 nm wavelength

ABSTRACT Third-order optical nonlinearities of diacrylate mesogens RM82 and RM257 in the isotropic phase for a low-power continuous wave laser irradiation at 632.8 nm wavelength have been studied. In their isotropic state, the diacrylate mesogens exhibit quite large nonlinear absorption. We observe a large two-photon absorption coefficients, on an order of 10−6 m/W, for the mesogens. The Kerr coefficients of the mesogens are characterised using single beam Z-scan technique, and found to reach an order of 10−7 m/W. Both diacrylate mesogens exhibit a good material figure of merit.

Octupolar Cyclotriphosphazene-Cored Self-Standing Covalent Organic Framework Membranes as Nonlinear Optical Materials: Impact of Linkage Types and Material Forms.

Conjugated and processable self-standing vinylene-linked covalent organic framework membranes (COFMs) are highly demanding for photonics and optoelectronics. In this work, we have fabricated the first cyclotriphosphazene (CTP) cored vinylene-linked self-standing COFM (CTP-PDAN). For comparison purposes, we have successfully fabricated the imine-linked congener (CTP-PDA). Leveraging the inherent nonlinear optical (NLO) response of the CTP core, both membranes were directly mounted to evaluate NLO parameters using the open-aperture (OA) Z-scan technique. Direct measurement of NLO responses on membranes is advantageous and free from solvent and scattering effects, making it a more practical approach compared to the conventional dispersion mode. The OA Z-scan transmission yields a reverse saturable absorption signature exhibiting a higher NLO absorption coefficient (β) of 58.37 cm/GW for CTP-PDAN, compared to that of the imine-linked CTP-PDA COFM (β = 8.5 cm/GW). These results can be correlated to the efficient conjugation through the vinylene linkage in CTP-PDAN compared to the imine linked congener.

Optical properties of spherical quantum dot using screened Kratzer potential

Here we investigate the optical properties of a spherical quantum dot using the screened Kratzer potential. The density matrix formalism is employed to study refractive index changes, along with linear and nonlinear optical absorption coefficients. To this effect, the radial Schrödinger equation is solved using the Nikiforov-Uvarov functional analysis method, resulting in analytical expressions for the energy eigenvalues and the associated eigen functions. Effects of dot size, potential parameters, and screening length on these properties are analyzed in detail for a GaAs quantum dot. The obtained results reveal that the optical response of the system is highly sensitive to the dot size and potential parameters, and thus it can be tuned accordingly. The impact of external magnetic and Aharonov-Bohm flux fields on the optical properties of the GaAs quantum dot is also discussed. The findings of this study may provide useful insights in design and optimization of quantum dot-based optoelectronic devices.

Multiphotonic Ablation and Electro-Capacitive Effects Exhibited by Candida albicans Biofilms.

This work reports the modification in the homogeneity of ablation effects with the assistance of nonlinear optical phenomena exhibited by C. albicans ATCC 10231, forming a biofilm. Equivalent optical energies with different levels of intensity were irradiated in comparative samples, and significant changes were observed. Nanosecond pulses provided by an Nd:YAG laser system at a 532 nm wavelength in a single-beam experiment were employed to explore the photodamage and the nonlinear optical transmittance. A nonlinear optical absorption coefficient -2 × 10-6 cm/W was measured in the samples studied. It is reported that multiphotonic interactions can promote more symmetric optical damage derived by faster changes in the evolution of fractional photoenergy transference. The electrochemical response of the sample was studied to further investigate the electronic dynamics dependent on electrical frequency, and an electro-capacitive behavior in the sample was identified. Fractional differential calculations were proposed to describe the thermal transport induced by nanosecond pulses in the fungi media. These results highlight the nonlinear optical effects to be considered as a base for developing photothermally activated phototechnology and high-precision photodamage in biological systems.

Nonlinear Optical Refraction and Absorption Features of Methyl Orange Dye in Polar Solvents.

Herein, we report the nonlinear optical (NLO) refraction and absorption features of azo dye namely, methyl orange (MO) dissolved in ethanol, methanol, acetone, 1-propanol, DMF and DMSO. The UV-Visible absorption study reveals that the maximum absorption spectrum of MO dye appeared towards longer wavelength by increasing the solvent polarizability is the result of red shift or bathochromic shift. The Z-scan method is utilized to measure the third-order NLO features of MO dye in different polar solvents. A continuous wave laser with 5-mW power and an excitation wavelength of 405nm is employed in the Z-scan technique. The NLO features including nonlinear index of refraction (n2), nonlinear coefficient of absorption (β) and third-order NLO susceptibility (χ3) are calculated to be the order of 10-7 cm2/W, 10-2cm/W and 10-7 esu, respectively. The NLO index of refraction shows peak-valley transmittance is the result of self-defocusing and NLO absorption coefficient exhibits both positive and negative nonlinearity owing to saturable absorption (SA) and reverse saturable absorption (RSA). The effect of solvent polarizability and dipole moment on third-order NLO susceptibility of MO dye is discussed. Based on the experimental results, an azo dye MO appears to be a promising option for NLO applications in the future.

Exploration of doping-dependent structural, optical, and electrical properties of thermally evaporated CdSe thin films for improved photodetection performance

This paper is devoted to studying the influence of indium doping on the structure, morphology, and electrical properties of thermally deposited CdSe thin films as a powerful approach toward optimized photodetection performance. The variation of incorporated In-level modulated crystallographic and surface morphology as obtained from the X-ray diffraction (XRD) and field emission scanning electron microscopy (FE-SEM), respectively. Besides, the optical properties of the prepared In:CdSe thin films were investigated spectrophotometrically in the UV-Vis-NIR regions. We have deeply evaluated not only the dispersion and absorption features but also the opto-(electronic) parameters of the prepared films. The spectral nonlinear optical refractive index, absorption coefficient, and susceptibility were estimated and analyzed. The tunability of the structural and optical properties is introduced in a systematic explainable manner in terms of the recorded elemental analysis using EDX. The dark conductivity measurements of the prepared films declared that doped CdSe film of 37.5 wt% indium achieved the highest electrical conductivity which coincident with all the structural and optical characterization findings. Furthermore, the fabricated In:CdSe films were integrated with p-type silicon for Au/In:CdSe/p-Si/Al heterojunction formation. The electrical and microelectronic parameters of the designed junctions have been assessed using the measured current-voltage relations. The charge carriers' conduction mechanism within the constructed junctions has been explained in detail. Eventually, the photodetection performance of the fabricated heterojunctions has been tested using the recorded (I-V) and (I-t) response curves. Evidently, 37.5 wt% In doping concentration in the CdSe structure achieved superior optical and electrical properties which have been reflected in its promising photodetection performance compared to not only the other pure and doped films in the present study but also other prior reports. Such a device achieved Jphoto, Rλ, EQE, D*, and tr/tf of about 34.4 mA/cm2, 3.43 A/W, 800%, 4.6 × 1010 Jones, and 3.06 ms/6.10 ms, respectively.

Polaronic Nonlinear Optical Response and All-Optical Switching Based on an Ionic Metal Oxide.

It has been well-established that light-matter interactions, as manifested by diverse linear and nonlinear optical (NLO) processes, are mediated by real and virtual particles, such as electrons, phonons, and excitons. Polarons, often regarded as electrons dressed by phonons, are known to contribute to exotic behaviors of solids, from superconductivity to photocatalysis, while their role in materials' NLO response remains largely unexplored. Here, the NLO response mediated by polarons supported by a model ionic metal oxide, TiO2 , is examined. It is observed that the formation of polaronic states within the bandgap results in a dramatic enhancement of NLO absorption coefficient by over 130 times for photon energies in the sub-bandgap regions, characterized by a 100fs scale ultrafast response that is typical for thermalized electrons in metals. The ultrafast polaronic NLO response is then exploited for the development of all-optical switches for ultrafast pulse generation in near-infrared (NIR) fiber lasers and modulation of optical signal in the telecommunication band based on evanescent interaction on a planar waveguide chip. These results suggest that the polarons supported by dielectric ionic oxides can fill the gaps left by dielectric and metallic materials and serve as a novel platform for nonlinear photonic applications.

Linear and nonlinear optical absorption coefficients in InGaN/GaN quantum wells: Interplay between intense laser field and higher-order anharmonic potentials

This computational investigation delves into the electronic and optical attributes of InGaN/GaN nanostructures subjected to both harmonic and anharmonic confinement potentials, coupled with the influence of a nonresonant intense laser field (ILF). The theoretical framework incorporates higher-order anharmonic terms, specifically quartic and sextic terms. The solutions to the Schrödinger equation have been computed employing the finite element method and the effective mass theory. Moreover, linear and third-order nonlinear optical absorption coefficients are derived via a density matrix expansion. Our analysis reveals the feasibility of manipulating electronic and optical properties by adjusting confinement potential parameters, system attributes, and laser field intensity. In addition, the ILF induces remarkable modifications, characterized by reduced resonance peak amplitudes and a blue shift in absorption coefficients. Intriguingly, regardless of potential harmonicity, the impact of incident electromagnetic intensity is notably more pronounced in the absence of the ILF. These findings hold significant promise for advancing theoretical predictions, providing valuable insights into the intricate interplay between confinement potentials, laser fields, and their effects on electronic and optical behaviors within nanostructures.

Donor-π-Acceptor Porphyrin-Assisted Bifunctional Defect Passivation for Enhanced Temporal Domain-/Wavelength-Dependent Nonlinear Absorption Properties in Perovskite Films.

Perovskite layer defects are a primary inhibiting factor for their optical nonlinearity, which restricts their use in nonlinear photonics devices. Nevertheless, due to the variety of defect types, the passivation and repair of these defects remain challenging. Herein, a novel bifunctional passivation strategy was proposed, and the porphyrin with a donor-π-acceptor structure was designed to bifunctionally repair perovskite defects by linking different types of functional groups via acetylenic π-conjugated linkage bridges on both sides, thus improving the nonlinear optical (NLO) absorption properties of porphyrin-perovskite hybrid materials. Research results indicate that the amino and carboxyl groups of porphyrins endow the ability to bifunctionally passivate charged defects via effective coordination interactions. The nonlinear absorption properties of all porphyrin-passivated MAPbI3 films were remarkably enhanced compared to that of the MAPbI3 film across multiple wavelengths and temporal domains. Particularly, the Por3-passivated perovskite film (MAPbI3/Por3) exhibited optimized strongest NLO performance, including reverse saturable absorption (RSA) under 800 nm femtosecond (fs) and 1064 nm nanosecond (ns) laser irradiations, as well as saturable absorption (SA) with 515 and 532 nm ns laser excitations. The value of the NLO absorption coefficient (β = 266.23 cm GW-1) is 1 order of magnitude higher than that of the pristine perovskite film (β = 12.93 cm GW-1), also outperforming other porphyrin-passivated perovskite films and some reported materials. The bifunctional passivation mechanism of porphyrin not only intensifies the perovskite's photoinduced ground-state dipole moment in the two-photon absorption (TPA) process and the free carrier absorption ability to deepen the RSA properties under 800 nm fs and 1064 nm ns lasers, respectively, but also enables the improvement of SA responses under 515 nm fs and 532 nm ns lasers by expediting the Pauli blocking effect of perovskite. Our study offers a viable paradigm, which aims at exploiting high-performance NLO perovskite materials across wide spectral regions and time scales.

Optical absorption coefficients of a single electron in a multilayer spherical quantum dot with a Kratzer-like confinement potential

The current study looks at how the Kratzer confinement potential affects the linear, third-order nonlinear, and total optical absorption coefficients (ACs) of a single electron in a multilayered spherical quantum dot (MSQD) by using the finite element method within the effective mass approximation. The variation of the transition energy has been investigated for two allowed transitions, 1p-2s and 2s-2p. Furthermore, we investigated the variation of the linear, third-order nonlinear, and total optical absorption coefficients as a function of the incident photon energy for several transitions while accounting for the effect of the Kratzer confinement potential. The findings show that the optical ACs and transition energy are strongly influenced by the Kratzer confinement potential.

Crystal structure, DFT study, Hirshfeld analysis and optical third order nonlinear properties of new 1-naphthylaminium hydrogen fumarate salt

This study reports the crystal structure and its supramolecular framework, quantum chemical calculations and nonlinear optical properties of 1-naphthylaminium hydrogen fumarate salt. The supramolecular self-assembly of fumarate anions and 1-naphthylaminium cation of the salt is primarily stabilized by N-H…O, O-H…O and C-H…O interactions. The construction of strong hydrogen bonds such as N-H…O and O-H…O produces two-dimensional corrugated sheet parallel to (010) plane, which resembles a supramolecular grid type architecture in the crystal structure. Two weak C-H…O interactions interlink the parallel (010) supramolecular sheet generating a three-dimensional molecular network. The molecular stability of the experimentally determined structure is theoretically optimized by DFT quantum chemical calculations using 6-31G(++) basis set. The relative molecular interaction-based charge distribution and the chemical reactivity of the titled salt were identified using electrostatic potential contouring and HOMO-LUMO maps. The crystal structure is subjected to Hirshfeld surface analysis to gain better understanding on the intermolecular interactions exhibited by the molecules. The optical nonlinearities of the titled salt are examined using Z-scan experimentation, the optical nonlinear refractive index and optical nonlinear absorption coefficient is estimated by closed and open aperture Z-scan methods. The observed nonlinear values are quite comparable to the conventional optical nonlinear values.

Structural, electrical and nonlinear optical characterization of Sn-doped CdO thin film synthesized via spray pyrolysis for optoelectronic applications

Transparent conducting metal oxides (TCOs) are well known for their application in optoelectronic devices. However, the nonlinear optical (NLO) study of TCOs helps to understand the characteristic features which give insight into their practical utilization as well as device application in each optical spectrum. In this work, we studied the structural, electrical, optical, and nonlinear optical properties of Sn-doped CdO. The structural, electrical, optical, and nonlinear optical properties of Sn-doped CdO were studied by using an X-ray diffractometer (XRD), Hall measurement system, UV–vis spectrometer, and Z-scan measurement. The XRD analysis shows that Sn-doped CdO is a polycrystalline material with a preferential peak of a plane (111) shifting slightly toward the (200) plane as Sn doping suddenly increases. Sn-doped CdO proved good electrical properties with conductivity increase from 0.192 × 102 Ω−1 cm−1 to 2.03 × 102 Ω−1 cm−1 and decrease in resistivity from 52.1 × 10−3 Ωcm to 4.92 × 10−3 Ωcm as the molar dopant concentration increase from 0.0001 M to 0.0005 M. The obtained bandgap for undoped and 0.0005 M, 0.0004 M, 0.0003 M, 0.0002 M, 0.0001 M Sn-doped CdO are 2.37, 1.63, 1.70, 1.81, 1.86, and 2.09 respectively. The NLO absorption coefficient (β) for 0.0003 M, 0.0004 M and 0.0005 M are 6.31 × 10−3 m/W, 11.47 × 10−3 m/W and 10.6 × 10−3 m/W respectively.

Synthesis, structural, spectral, thermal, and optical characterization of a new curcumin derivative: A promising material for NLO applications

A novel Curcumin derivative 1-(4-chlorobenzoyl)-3,5-bis((E)-3,4-dimethoxybenzylidene)piperidin-4-one (CDMBP) has been synthesized by Claisen-Schmidt condensation and Schotten-Baumann reaction methods. CDMBP single crystal was grown from acetone by slow evaporation method at ambient temperature. The crystal structure of the compound was derived by Single Crystal X-ray Diffraction studies (SCXRD). The title compound CDMBP was crystallized in a triclinic crystal system with a P ͞1 space group. NMR spectral analysis reveals the different types of carbon and proton in the molecular structure of the title compound. The modes of vibrations of different chemical groups were identified using FT-Raman and Fourier Transform Infrared spectral analysis (FTIR). Utilizing the UV–Vis spectrum, the cutoff wavelength and linear optical constants such as the band gap, extinction coefficient, and refractive index were calculated. The Photoluminescence spectrum (PL) has been studied and it shows a high-intensity peak at 504 nm and belongs to the green emission radiation region. Fluorescence profiling of the compound was done to get an outline of the emission features of the excited states with the emission decay mechanisms using Lifetime measurements. The third-order nonlinear optical property (NLO) of CDMBP was investigated in detail using a Z-scan technique with a He–Ne laser at 632.8 nm as a laser source. The nonlinear optical susceptibility (χ3), absorption coefficient (β), and refractive index (n) were calculated using transmittance data. The thermal stability of the grown crystal was investigated from the Thermogravimetric Analysis (TGA) and Differential Thermal Analysis (DTA).

Optical absorption in core–shell quantum antidot with donor impurity under applied co-directed electric and magnetic fields

In this article, we have investigated an electron energy spectrum, optical absorption coefficients (OACs) and polarizability under the effect of the co-directed electric and magnetic fields in the multilayer spherical quantum antidot (MSQAD) Al0.3 Ga0.7 As/GaAs/Al0.3Ga0.7 As with off-center impurity. The calculations were done for different dot sizes within the effective mass approximation using the matrix method. The dependence of the total, linear, and nonlinear OACs on the incident photon energy is calculated considering the intraband electron quantum transitions. The donor polarizability and impurity binding energy as function of electric field intensity are obtained at different values of the magnetic field induction.

Investigation of band parameters and electrochemical analysis of multi core-shell CdSe/CdS/ZnS quantum dots

Highly emissive core−multi-shell (CdSe/CdS/ZnS) quantum dots (QDs) within size range of ∼ 2 nm–5 nm were prepared via hot injection method. Capping agent (polymers) were used to increase the lifetime of QDs, without a protective atmosphere. Red shift was observed in an absorption spectrum of QDs peaks at 362 nm, 365 nm, 558 nm, and 556 nm for CdSe/CdS and CdSe/CdS/ZnS with respect to CdSe core. Voltammetry measurements (Eg ∼ 2. 09 eV) for band gaps were in good agreement with the UV–visible spectroscopic data (Eg ∼ 2.65 eV). QDs exhibited three distinguished peaks comparing to (111), (220), and (311) planes of cubic structures of CdSe, CdSe/CdS and CdSe/CdS/ZnS within crystallite size of 20–27 nm as observed by XRD spectra. A larger active surface area 0.06 cm−2, computed by CV increased the catalytic activity of sensors by exposing the electroactive sites. Linear, nonlinear optical susceptibility and absorption coefficients were computed by an effective mass model. Quantum confinement was confirmed by taking electron probability density as function of radial distance of quantum dots.

Toward strong nonlinear optical absorption properties of perovskite films via porphyrin axial passivation

Defects within perovskite layers are considered to be a primary factor that inhibits nonlinear optical (NLO) performance, and mitigating or eliminating them is indispensable for the implementation of high-performance perovskite-based photonic and energy devices. Herein, we propose a novel defect modulation strategy through binding the functional groups at the axial positions of porphyrins with the defects of perovskites. Two axially-coordinated porphyrin molecules (TiOPr and SnOHPr) were utilized as effective functional additives to passivate the defects and control perovskite crystallization, while the role of axial functional groups of porphyrins has been systematically studied. Z-scan measurement results demonstrate that porphyrin-treated perovskite films exhibit prominently enhanced optical absorption nonlinearities under ultrafast femtosecond (fs) laser excitation at 800 nm in comparison to the MAPbI3 perovskite film, the NLO absorption coefficient (β) values for the modified films are approximately one or two orders of magnitudes superior to that of the pristine film. This significant improvement in NLO performance likely stems from the increased photoinduced ground-state dipole moment of the perovskite film treated by porphyrin during the process of two-photon absorption (TPA), and their photoinduced charge/energy transfer between perovskite and porphyrin. Particularly, the MAPbI3/SnOHPr film displays the largest β values (636.92–6621.42 cm GW−1) among all measured samples at different irradiation energies and a low optical limiting threshold of 5 mJ cm−2, which may profit from the dual-functional passivation effect of SnOHPr onto perovskite, suggesting its great potential as optical limiters. These observations strongly indicate that porphyrin-axial passivated perovskite films are outstanding material candidates for optical limiting applications towards ultrafast fs laser pulses in the near-infrared region. Our work affords a feasible paradigm for constructing high-performance NLO perovskite materials through porphyrin-axial passivation of defects.

Nonlinear optical properties in organic fish gelatin, potassium dichromate, and organic–inorganic mix

The nonlinear optical properties of fish gelatin, potassium dichromate, and a mix of both are presented. The z-scan experimental technique and the photo-induced thermal lens formation model are used to determine nonlinear optical parameters such as the non-linear refractive index and the nonlinear optical absorption coefficient. The spatial self-phase modulation in the mixture is analyzed with an Ar continuous wave (cw) laser at 477 nm at different light powers. Furthermore, we theoretically studied the electrostatic interaction between potassium dichromate and fish collagen based on the Density Functional Theory. The experimental and theoretical results show that the nonlinear optical properties of the mixture are improved due to better thermal conductivity and stability, indicating a high potential for optical applications such as nonlinear gratings and holography.

Nonlinear Optical Response of Dispersed Medium Based on Conjugates Single-Walled Carbon Nanotubes with Phthalocyanines

Nanosecond lasers have recently been widely involved in human activity. However, high-intensity laser radiation can cause severe damage to organs of vision and expensive photonic devices. Radiation in the near UV range is especially dangerous for human eyes, since it is strongly absorbed by biological media and is also invisible, i.e., the reaction time of the eye to such radiation is much lower than that of visible light. Passive limiters have high transmission (>70%) at a low light intensity and begin to “darken” only when the threshold value of the laser radiation intensity is reached. In this work, we studied liquid nanodispersed nonlinear optical limiters based on hybrids of single-walled carbon nanotubes (SWCNTs) with metal-free tetra(hydroxy)phthalocyanine (OH)4PcHH). The value of the hydrodynamic radius of separate particles after (OH)4PcHH binding increased from 288 ± 55 nm to 350 ± 60 nm, which confirms the attachment of phthalocyanine complexes to nanotubes. The third harmonic of a Nd:YAG nanosecond laser (355 nm, 20 ns) was used to study the nonlinear optical response. Based on a Z-scan with open-aperture and input-output dependence curves, third-order nonlinear optical absorption coefficients of 149, 236, and 229 cm/GW were obtained for dispersions of composites of SWCNTs and (OH)4PcHH in water, dimethylformamide (DMF), and dimethylsulfoxide (DMSO), respectively. Threshold values did not exceed 100 mJ/cm2. The Z-scan showed a gradual decrease in the duration of the laser pulse by 53%; however, near the focus, there was a sharp increase in the duration of the transmitted pulse, reaching a value of 29 ns in z = 0. This phenomenon confirms the occurrence of reverse saturable absorption in the investigated media and can be used in photonic devices to control the temporal characteristics of the signal. Thus, the possibility of protection of sensitive photonic devices and human eyes from nanosecond laser pulses in the near UV range by nanodispersed liquid media based on composites of SWCNTs with (OH)4PcHH has been discussed in this paper.

A Cut-to-Link Strategy for Cubane-Based Heterometallic Sulfide Clusters with Giant Third-Order Nonlinear Optical Response

Although the synthesis of low-dimensional metal sulfides by assembling cluster-based units is expected to promote the development of optical materials and models of enzyme active centers such as dinitrogenase, it is faced with limited assembly methodology. Herein we present a cut-to-link strategy to generate high-nuclearity assemblies, inspired by the formation of a Z-type dimer of the W-S-Cu analogues of PN cluster through in situ release of active linkers. Four new compounds with structures based on the same {Tp*WS3Cu3} incomplete cubane-like units were obtained using varied combinations of mild reagents. Open-aperture Z-scan measurements demonstrated the highest-nuclearity complex has the largest nonlinear optical absorption coefficient among discrete cluster-based materials reported to date. This approach enables building high-nuclearity metal sulfide clusters through cluster-based building blocks and opens a way to the design and exploration of materials based on well-identified building blocks.

Linear and nonlinear optical absorption coefficients and refractive index changes of GaAs/GaAsSb/GaAs V-shaped quantum wells affected by intense laser fields

Linear and nonlinear optical absorption coefficients and refractive index changes of GaAs/GaAsSb/GaAs V-shaped quantum wells affected by intense laser fields