Broadband third-order optical nonlinearities of layered franckeite towards mid-infrared regime

The study of nonlinear optical responses in the mid-infrared(mid-IR)regime is essential for advancing ultrafast mid-IR laser applications.However,nonlinear optical effects under mid-IR excitation are rarely reported due to the lack of suitable nonlinear optical materials.The natural van derWaals heterostructure franckeite,known for its narrow bandgap and stability in air,shows great potential for developing mid-IR nonlinear optical devices.We have experimentally demonstrated that layered franckeite exhibits a broadband wavelength-dependent nonlinear optical response in the mid-IR spectral region.Franckeite nanosheets were prepared using a liquid-phase exfoliation method,and their nonlinear optical response was characterized in the spectral range of 3000 nm to 5000 nm.The franckeite nanosheets exhibit broadband wavelengthdependent third-order nonlinearities,with nonlinear absorption and refraction coefficients estimated to be about 10^(-7)cm/W and 10^(-11)cm^(2)/W,respectively.Additionally,a passively Q-switched fluoride fiber laser operating around a wavelength of 2800 nm was achieved,delivering nanosecond pulses with a signal-to-noise ratio of 43.6 dB,based on the nonlinear response of franckeite.These findings indicate that layered franckeite possesses broadband nonlinear optical characteristics in the mid-IR region,potentially enabling new possibilities for mid-IR photonic devices.

Ultrafast third-order optical nonlinearity of several sandwich-type phthalocyaninato and porphyrinato europium complexes

The third-order optical nonlinearity of two sandwich-type phthalocyaninato and porphyrinato europium com- plexes, including double- and triple-deckers （Eu[Pc（OC5H11）8]2, Eu2（Pc）（TPP）2, Pc=phthalocyanine, TPP=5, 10, 15, 20- tetraphenylporphyrinate）, was investigated by using the femtosecond time-resolved optical Kerr gate method at 830 nm wavelength. Their second-order hyperpolarizability is estimated to be 0.74× 10^-30esu and 3.0× 10^-3esu respectively. This exhibits an evident enhancement in comparison with 0.47×10^-30esu for one-decker Eu（Pc）（acac） （acac=acetylacetonate）, which is also measured under the same conditions. The enhancement is attributed to the introduction of lanthanide metal to the large π-conjugated system, intermacrocycle interaction and two-photon resonance etc.

The Synthesis of Third-order Optical Nonlinear Organic Polyheterocyclic Materials

Synthesis of the third-order nonlinear materials: bis (1,4-dihydroxynaphthalene) tetrathiafulvalene and bis (1,4-dialkoxylnaphthalene) tetrathiafulvalene has been achieved in four steps, starting from 2,3-dichloro-1,4-naphthaquinone. The materials exhibit larger third-order nonlinear optical susceptibilities c(3) .

Giant and light modifiable third-order optical nonlinearity in a free-standing h-BN film

Recently,hexagonal boron nitride(h-BN)has become a promising nanophotonic platform for on-chip information devices due to the practicability in generating optically stable,ultra-bright quantum emitters.For an integrated information-processing chip,high optical nonlinearity is indispensable for various fundamental functionalities,such as all-optical modulation,high order harmonic generation,optical switching and so on.Here we study the third-order optical nonlinearity of free-standing h-BN thin films,which is an ideal platform for on-chip integration and device formation without the need of transfer.The films were synthesized by a solution-based method with abundant functional groups enabling high third-order optical nonlinearity.Unlike the highly inert pristine h-BN films synthesized by conventional methods,the free-standing h-BN films could be locally oxidized upon tailored femtosecond laser irradiation,which further enhances the third-order nonlinearity,especially the nonlinear refraction index,by more than 20 times.The combination of the free-standing h-BN films with laser activation and patterning capability establishes a new promising platform for high performance on-chip photonic devices with modifiable optical performance.

Research progress of third-order optical nonlinearity of chalcogenide glasses

Chalcogenide glasses （ChGs） are a promising candidate for applications in nonlinear photonic devices. In this paper, we review the research progress of the third-order optical nonlinearity （TONL） of ChGs from the following three aspects： chemical composition, excitation condition, and post processing. The deficiencies in previous studies and further research of the TONL property of ChGs are also discussed.

Investigation on Third-Order Optical Nonlinearities of Two Organometallic Dmit2- Complexes Using Z-Scan Technique

The third-order nonlinear optical properties of two dmit organometallic complexes, [(CH3)4N] [Au(C3S5)2] (MeAu) and [(CH3)4N][Ni(C3S5)2] (Me Ni) in acetone solutions, were characterized us- ing a short pulse Z-scan technique at 1064 nm wavelength. Self-defocusing effects were found in both samples and stronger saturable absorp-tion was observed in MeNi solution comparing with that of MeAu. The origins were analyzed for the differences between the results. Two figures of merit W and T were also calculated to evalu-ate the suitability of two materials for all-optical integrated devices. The results of W=22.84 and T≈0 of MeAu make it an excellent candidate for the all-optical applications.

Modulation of epsilon-near-zero wavelength and enhancement of third-order optical nonlinearity in ITO/Au multilayer films

We report the modulation of epsilon-near-zero(ENZ)wavelength and enhanced third-order nonlinearity in indium tin oxide(ITO)/Au multilayer films.The samples consisting of five-layer 40 nm ITO films spaced by four-layer ultrathin Au films of different thickness,i.e.,ITO(40 nm)/[Au(x)/ITO(40 nm)]4,were prepared by magnetron sputtering at room temperature.The ENZ wavelength in the multilayer films is theoretically calculated and experimentally confirmed.The nonlinear refractive index and nonlinear absorption coefficient of the samples of x=0,2,3,4 nm were determined using the Z-scan method at a wavelength of 1.064μm.The large nonlinear refractive index n2=1.12×10^(−13) m^(2)=W and nonlinear absorption coefficient β=−1.78×10^(−7) m=W in the sample of x=4 nm are both four times larger than those in the single-layer ITO film.The large optical nonlinearity due to the ENZ enhancement and carrier concentration is discussed.The results indicate that the ITO/Au multilayer films are promising for advanced all-optical devices.

Using harmonic beam combining to generate pulse-burst in nonlinear optical laser

The ultrashort lasers working in pulse-burst mode reveal great machining performance in recent years. The number of pulses in bursts effects greatly on the removal rate and roughness. To generate a more equal amplitude of pulses in burst with linear polarization output and time gap adjustable, we propose a new method by the harmonic beam combining(HBC).The beam combining is commonly used in adding pulses into the output beam while maintaining the pulse waveform and beam quality. In the HBC, dichroic mirrors are used to combine laser pulses of fundamental wave(FW) into harmonic wave(HW), and nonlinear crystals are used to convert the FW into HW. Therefore, HBC can add arbitrarily more HW pulses to generate pulse-burst in linear polarization with simple structure. The amplitude of each pulse in bursts can be adjusted the same to increase the stability of the burst, the time gap of each pulse can be adjusted precisely by proper time delay. Because HBC adds pulses sequentially, the peak power density of the burst is the same as each pulse, pulses can be combined without concern of back-conversion which often occurs in high peak power density. In the demonstration, the extendibility of HBC was verified by combining two beams with a third beam. The combined efficiency rates were larger than 99%, and the beam quality of each beam was maintained at M^(2)≈1.4.

Symmetry transformation of nonlinear optical current of tilted Weyl nodes and application to ferromagnetic MnBi_(2)Te_(4)

A Weyl node is characterized by its chirality and tilt.We develop a theory of how nth-order nonlinear optical conductivity behaves under transformations of anisotropic tensor and tilt, which clarifies how chirality-dependent and-independent parts of optical conductivity transform under the reversal of tilt and chirality.Built on this theory, we propose ferromagnetic Mn Bi2Te4as a magnetoelectrically regulated, terahertz optical device, by magnetoelectrically switching the chiralitydependent and-independent DC photocurrents.These results are useful for creating nonlinear optical devices based on the topological Weyl semimetals.

Quasi-anti-parity–time-symmetric single-resonator micro-optical gyroscope with Kerr nonlinearity

Parity–time(PT) and quasi-anti-parity–time(quasi-APT) symmetric optical gyroscopes have been proposed recently which enhance Sagnac frequency splitting. However, the operation of gyroscopes at the exceptional point(EP) is challenging due to strict fabrication requirements and experimental uncertainties. We propose a new quasi-APT-symmetric micro-optical gyroscope which can be operated at the EP by easily shifting the Kerr nonlinearity. A single resonator is used as the core sensitive component of the quasi-APT-symmetric optical gyroscope to reduce the size, overcome the strict structural requirements and detect small rotation rates. Moreover, the proposed scheme also has an easy readout method for the frequency splitting. As a result, the device achieves a frequency splitting 10~5 times higher than that of a classical resonant optical gyroscope with the Earth's rotation. This proposal paves the way for a new and valuable method for the engineering of micro-optical gyroscopes.

Electrical and nonlinear optical properties of TGZO transparent conducting films deposited by magnetron sputtering

Thin transparent oxide conducting films(TCOFs)of titanium and gallium substituted zinc oxide(TGZO)were fabricated via radio frequency(RF)magnetron sputtering technique.The effects of RF power on electrical,linear and nonlinear optical characteristics were investigated by Hall tester,Ultraviolet(UV)-visible spectrophotometer and optical characterization method.The results indicate that RF power significantly influences the electrical and optical properties of the deposited films.As RF power raises,the resistivity and Urbach energy fall initially and then rise,while the figure of merit,mean visible transmittance and optical bandgap show the reverse variation trend.At RF power of 190 W,the TGZO sample exhibits the highest electro-optical properties,with the maximum figure of merit(1.14×10^(4)Ω^(-1)∙cm^(-1)),mean visible transmittance(86.9%)and optical bandgap(3.50 eV),the minimum resistivity(6.26×10^(-4)Ω∙cm)and Urbach energy(174.23 meV).In addition,the optical constants of the deposited films were determined by the optical spectrum fitting method,and the RF power dependence of nonlinear optical properties was studied.It is observed that all the thin films exhibit normal dispersion characteristics in the visible region,and the nonlinear optical parameters are greatly affected by the RF power in the ultraviolet region.

Structure,electronic,and nonlinear optical properties of superalkaline M_(3)O(M=Li,Na)doped cyclo[18]carbon

Cyclo[18]carbon has received considerable attention thanks to its novel geometric configuration and special electronic structure.Superalkalis have low ionization energy.Doping a superalkali in cyclo[18]carbon is an effective method to improve the optical properties of the system because considerable electron transfer occurs.In this paper,the geometry,bonding properties,electronic structure,absorption spectrum,and nonlinear optical(NLO)properties of superalkaline M_(3)O(M=Li,Na)-doped cyclo[18]carbon were studied by using density functional theory.M_(3)O and the C_(18) rings are not coplanar.The C_(18) ring still exhibits alternating long and short bonds.The charge transfer between M_(3)O and C_(18) forms stable[M_(3)O]+[C_(18)]-ionic complexes.C_(18)M_(3)O(M=Li,Na)shows striking optical nonlinearity,i.e.,their first-and second-order hyperpolarizability(βvec andγ||)increase considerably atλ=1907 nm and 1460 nm.

Galerkin-Bernstein Approximations for the System of Third-Order Nonlinear Boundary Value Problems

This paper is devoted to find the numerical solutions of one dimensional general nonlinear system of third-order boundary value problems (BVPs) for the pair of functions using Galerkin weighted residual method. We derive mathematical formulations in matrix form, in detail, by exploiting Bernstein polynomials as basis functions. A reasonable accuracy is found when the proposed method is used on few examples. At the end of the study, a comparison is made between the approximate and exact solutions, and also with the solutions of the existing methods. Our results converge monotonically to the exact solutions. In addition, we show that the derived formulations may be applicable by reducing higher order complicated BVP into a lower order system of BVPs, and the performance of the numerical solutions is satisfactory. .

The third-order optical nonlinearity of the stainless steel doped SrTiO_3 thin film grown by L-MBE

Stainless steel-doped SrTiO3 thin films were fabricated by laser molecular beam epitaxy (L-MBE). Nonlinear optical property of the thin film was measured by the single beam Z-scan technique at the wavelength of 532 nm. Two two-phonon absorption coefficient and nonlinear refractive index were determined to be 9.37 x 10-7 m/W and 1.55 x 10-6 esu, respectively. The merit figure T was calculated to be 1.8, satisfying condition T < 1 for an optical switch. The thin film has a very promising prospect for the applications in optical device.

Synthesis of Poly (3-acetylpyrrolyl methine) with Azobenzene Side Groups and Study on Its Third-order Nonlinear Optical Property

A novel soluble π-conjugated polymer, poly [（3-acetylpyrrole-2, 5-diyl） p-（N, N-dimethylamino） azobenzylidene] （PAPDMAABE）, was synthesized by condensation of 3-acetylpyrrole with 4-aldehyde-4＇-dimethylaminoazobenzene （ADMAA）. The chemical structure of PAPDMAABE was characterized by Fourier transform infrared spectroscopy （FTIR）, ^1H-NMR, and UV-Vis-NIR spectra. Transmission electron microscope （TEM） analysis for PAPDMAABE indicates that part of PAPDMAABE is in crystal state, due to the short-range order of the polymer. Thermogravimetric analysis （TGA） curve shows that the polymer has good thermal stability and its decomposition temperature is 248℃. The optical band gap of PAPDMAABE obtained from the optical absorption spectrum is about 1.73 eV. The resonant third-order nonlinear optical property of PAPDMAABE at 532 nm was studied using degenerate four-wave mixing （DFWM） technique. The resonant third-order nonlinear optical susceptibility of the polymer is about 7.48×10^-8 esu.

The Third-Order Nonlinear Optical Properties in Cobalt-Doped ZnO Films

We quantitatively investigate the third-order optical nonlinear response of Co-doped ZnO thin films prepared by magnetron sputtering using the Z-scan method. The two-photon absorption and optical Kerr effect are revealed to contribute to the third-order nonlinear response of the Co-doped ZnO films. The nonlinear absorption coefficient β is determined to be approximately 8.8 × 10-5 cm/W and the third-order nonlinear susceptibility X（3） is 2.93 × 10-6 esu. The defect-associated energy levels within the band gap are suggested to be responsible for the enhanced nonlinear response observed in Co-doped ZnO films.

UV-Vis Spectrum and the Third-order Nonlinear Optical Properties of the Chiral Camphorderived β-diketonate Platinum Complexes

UV-Vis spectrum and the third-order nonlinear optical properties of the chiral camphor-derived β-diketonate have been studied at the B3LYP/6-31G＊ level. The results showed that the introduction of electron-drawing group -CF3 and -C3F7 on β-diketonate made the strongest absorption peak red-shift and the lowest energy absorption blue-shied. Introduction of -OC2H5 on the benzene or pyridine ring made the lowest energy absorption blue-shift. When the -C2H3 was introduced on the benzene or pyridine ring, the lowest energy absorption was red-shifted. Introduction of electron-donating group on β-diketonate can enlarge their nonlinear optical properties. On the contrary, the introduction of electron-drawing group dropped it down.

Third-order optical nonlinearities for lanthanum (Ⅲ) complexes with 1,10-phenanthroline components

The nonlinear refractive indexes n 2 for the ethanol solutions of 1,10-phenanthroline (2.0×10 -3 mol·L -1), [bis(1,10-phenanthroline) lanthanum (Ⅲ)] nitrate (1.0×10 -3 mol·L -1), and [nitrato-fluoracil-bis (1,10-phenanthroline) lanthanum (Ⅲ)] nitrate (1.0×10 -3 mol·L -1) are first measured, the third-order nonlinear optical susceptibilities χ (3) and <γ> are calculated, and the mechanisms of the third-order optical nonlinearities enhanced by lanthanum (Ⅲ) are discussed preliminarily.

Third-order nonlinear optical properties of graphene composites:A review

Graphene has excellent thirdorder nonlinear optical(NLO)properties due to its unique electronic band structure and wideband gap tunability.This paper focuses on the research progress of graphene and its composite materials in nonlinear optics in recent years.In this review,recent results on graphene(or graphene oxide)-metal nanoparticles(G-MNPs),graphene-metal-oxide nanoparticles(G-MONPs),graphene-metal sulfide nanoparticles(G-MSNPs),and graphene-organic molecular composites(G-OM)have been discussed.In addition,the enhancement mechanism of nonlinear absorption(NLA)and optical limiting(OL)have also been covered.

Electronic Absorption Spectra and Third-Order Nonlinear Optical Property of Dinaphtho[2,3-b:2’,3’-d]Thiophene-5,7,12,13- Tetraone (DNTTRA) and Its Phenyldiazenyl Derivatives: DFT Calculations

Third-order nonlinear optical (NLO) materials have broad application prospects in high-density data storage, optical computer, modern laser technology, and other high-tech industries. The structures and frequencies of Dinaphtho[2,3-b:2’,3’-d]thiophene-5,7,12,13-tetraone (DNTTRA) and its 36 derivatives containing azobenzene were calculated by using density functional theory B3LYP and M06-2X methods at 6-311++g(d, p) level, respectively. Besides, the atomic charges of natural bond orbitals (NBO) were analyzed. The frontier orbitals and electron absorption spectra of A-G5 molecule were calculated by TD-DFT (TD-B3LYP/6-311++g(d, p) and TD-M06-2X/6-311++g(d, p)). The NLO properties were calculated by effective finite field FF method and self-compiled program. The results show that 36 molecules of these six series are D-π-A-π-D structures. The third-order NLO coefficients γ (second-order hyperpolarizability) of the D series molecules are the largest among the six series, reaching 107 atomic units (10-33 esu) of order of magnitude, showing good third-order NLO properties. Last, the third-order NLO properties of the azobenzene ring can be improved by introducing strong electron donor groups (e.g. -N(CH3)2 or -NHCH3) in the azobenzene ring, so that the third-order NLO materials with good performance can be obtained.