Theoretical study on stability of Z-scan technique by use of quasi-one-dimensional slit beam

The modified Z-scan technique using the quasi-one-dimensional slit (QODS) beam for characterizing the third-order optical nonlinearity has been reported recently. In the present work, we investigate the effect of the finite length of the slit in the QODS beam Z-scan for the practical experimental conditions, and then give an empirical expression that allows the direct estimation of nonlinear refraction coefficient from the measured normalized peak-valley transmittance difference. In particular, we explore relatively in detail the influences of the sample imperfection on the Z-scan traces, such as the hollow hole of the sample and the nonuniform nonlinearity. Compared with the other Z-scan techniques, such as the top-hat and Gaussian-beam Z-scans, we find that the QODS beam Z-scan has the great improvement for the sample imperfections. The results suggest that the QODS beam Z-scan is a more promising and useful technique for characterizing the optical nonlinearity of an imperfect sample.     

Direct measurement of free carrier nonlinearity in semiconductor-doped glass with picosecond pump-probe Z-scan experiment

We report the direct measurement of free carrier nonlinearity in a semiconductor-doped glass with picosecond pump-probe Z-scan experiment. A strong Z-scan signal from a weak and time delayed probe beam is observed. The probe beam Z-scan signal is comparable in magnitude to the Z-scan signal of the intense pump beam, clearly showing the dominance of the effective fifth order nonlinearity due to the pump beam generated free carriers in the overall nonlinear response of semiconductor-doped glass. The estimated magnitude of the fifth order nonlinearity is consistent with that obtained from earlier reported experiments.     

Measurement of nonlinear properties and optical limiting ability of Rhodamine6G doped silica and polymeric samples

The third order nonlinear optical properties of Rhodamine6G (Rh6G) doped silica and polymeric samples have been investigated using single beam z-scan technique under excitation by the second harmonic of Nd:YAG laser beam (532 nm). The nonlinear refractive index, nonlinear absorption coefficient, real and imaginary parts of third order nonlinear susceptibility in the samples of silica and poly-methylmethacrylate (PMMA) matrices are measured. Thermal contribution to the nonlinear refractive index in case of undoped silica samples has been calculated in order to have better accuracy of the material response contribution to third order nonlinearity. The comparative study of the optical limiting performance of Rh6G doped silica and polymeric samples show that Rh6G doped silica is relatively superior for optical limiting applications.     

Data analysis of z-scan experiment using Fresnel–Kirchoff integral method in colloidal TiO2 nanoparticles

In this study, a precise method to evaluate nonlinear optical absorption and refraction of materials using z-scan method based on Fresnel–Kirchhoff integral method (FK method) has been offered. The real electric field of a Gaussian beam passing through a nonlinear sample having both nonlinear absorption and refraction has been investigated using FK method. Subsequently, the z-scan curves have been studied. This is the first time that FK method has been used for calculating the nonlinear absorption coefficient. Additionally, an appropriate numerical curve-fitting method for calculating the nonlinear optical coefficients based on z-scan method has been suggested. Z-scan curves and nonlinear optical coefficients have been obtained for TiO₂ nanoparticles in CW irradiation regime with the particle size ranges from 70 to 90 nm. This is the first experimental study which uses this analytical numerical method. Finally, all calculated results extracted from this new method have been compared with those of the previous methods.     

Investigation of nonlinear optical properties of organic dye by Z-scan technique using He-Ne laser

The third-order nonlinear optical properties of Basic Green 1 dye were measured by the Z-scan technique and measurements were carried out at different concentrations and several incident intensities. The results showed that the Basic Green 1 dye exhibited large nonlinear refractive coefficient () and nonlinear absorption coefficient () at the wavelength 632.8 nm of He-Ne. The negative sign of the nonlinear refractive index n₂ indicates that this material exhibits self-defocusing optical nonlinearity. These results show that Basic Green 1 dye has potential applications in nonlinear optics.     

Measurement of two-photon absorption using the photo-thermal lens effect

We report on new schemes for pump-probe photo-thermal lens methods aimed for measuring the two-photon absorption coefficient of a given material. We show that by focusing a probe beam in the presence of a nearly collimated pump beam, we create a thermal lens which yields measurement of the two-photon absorption coefficient of nitrobenzene of (3.9 ± 0.3) 10⁻¹⁰ cm/W at 532 nm. We also show that when the pump field is focused in the presence of a nearly collimated probe beam the width of the z-scan signature of a two-photon absorption process is nearly one order of magnitude smaller than that of a one-photon process. We show experimental evidence of the effect obtained for nitrobenzene.     

Nonlinear optical and optical power limiting studies on a new thiophene-based conjugated polymer in solution and solid PMMA matrix

An experimental investigation of the third-order nonlinear optical properties of new poly{2-{5-[3,4-ditetradecyloxy-5-(1,3,4-oxadiazol-2-yl)thiophen-2-yl]-1,3,4-oxadiazol-2-yl}pyridine} (P) in tetrahydrofuran (THF) solution and in solid poly(methylmethacrylate) (PMMA) matrix, by Z-scan technique is reported. The Z-scan traces reveal that the composite films exhibit large negative nonlinear refractive index of the order 10⁻¹⁰ esu. The excited-state absorption cross-section was found to be larger than the ground-state absorption indicating that the operating nonlinear process is reverse saturable absorption (RSA). The new polymer P exhibits good optical power limiting properties in the nanosecond regime in solution and as well in solid PMMA matrix.     

Time analogue of the z-scan technique suitable to waveguides

We propose a new technique to perform measurements of nonlinearities in optical waveguides based on the variation of an optical pulse chirp. This technique is analogous to the z-scan technique in the time domain. We analyze the new experimental method analytically and numerically, obtaining an useful expression relating the nonlinearity with a peak-valley structure. Practical ways to implement the technique are discussed. Received 13 March 2001     

Multilayer Au/TiO2Composite Films with Ultrafast Third-Order Nonlinear Optical Properties

We report on the ultrafast third-order optical nonlinearity in multilayer Au/TiO2 composite films fabricated on quartz substrates by pulsed laser deposition technique. The linear optical properties of the films are determined and optical absorption peaks due to surface plasmon resonance of Au particles are observed at about 590hm. The third-order optical nonlinearities of the films are investigated by z-scan method using a femtosecond laser （50 fs） at the wavelength of 800 nm. The sample showed fast nonlinear optical responses with nonlinear absorption coefficient and nonlinear refractive index being -3.66 × 10^-10 m/W and -2.95 × 10^-17 m^2/W, respectively. The results also show that the nonlinear optical effects increase with the increasing Au concentration in the composite films.     

Wavefront study in a Gaussian beam passed through a nonlinear optical medium

We present a numerical model to study the wavefront of a Gaussian laser beam propagated through a nonlinear Kerr media. The model is based on the Gaussian decomposition method. The interaction between a laser beam and a self-focusing or self-defocusing media is discussed from the viewpoint of wavefront distortion. The method is useful for simulation of the wavefront of the beam next to the sample. We also compare our results with those obtained from z-scan method. There is a quite good agreement between data from z-scan method and our results.     

Simultaneous estimation of optical nonlinear refractive and absorptive parameters by solvent induced changes in optical density

With picosecond pulses at the wavelength of 532 nm, we have determined the optical nonlinear refractive and absorptive parameters of the dye N,N′-bis(2,5-di-tert-butylphenyl)-3,4,9,10-perylenedicarboximide (DBPI) by a single closed-aperture (CA) Z-scan technique. This technique uses a theoretical model that elucidates the refractive and absorptive optical nonlinearity present simultaneously in the CA Z-scan profile. The observed remarkable red shift in the absorption spectrum of the dye in the acidic medium as compared to that in the polar medium has been used to vary the optical density at a single frequency. We find that the effect of saturable absorption (SA) is complete at higher concentrations. The effect of reverse saturable absorption (RSA) is dominating in dilute concentrations. The observed variations in the excited state refractive cross-section (σ_r) with the concentration and the energy have been attributed to the contributions of higher order nonlinearity along with the existing third-order nonlinearity.     

Method for measurements of second-order nonlinear optical coefficient based on Z-scan

The method for measuring second-order nonlinear optical coefficients based on well-known Z-scan is presented. The influence of linear absorption coefficients on normalized transmittance is discussed. Using this method, we obtained the second-order nonlinear coefficient d₃₁(5%MgO:LiNbO₃) = 4.5 × 10⁻¹² m/v at 1064 nm, which agrees well with theoretical calculations and previous well-known values.     

Third order nonlinear optical studies of bromocresol purple in liquid and solid media

The quest for materials exhibiting high nonlinear refraction and absorption are required for photonic device application. In this paper we report a simplified Z-scan technique, to study the optical nonlinearity of the dye bromocresol purple in methanol and ethanol for different concentration and dye doped polymer film at the wavelength 532 nm of Nd:YAG laser. The experimental results show that the investigated organic dye molecule exhibits saturation absorption and negative nonlinearity. The nonlinear absorption co-efficient and the nonlinear refractive index were measured for the dye doped film, and for dye in methanol and ethanol at the concentration of 0.03 mM and 0.05 mM. The measured third order susceptibility was found to be of the order of 10⁻⁶ e.s.u. in both solid and liquid medium. The result shows that the dye has potential applications in nonlinear optics.     

Third-order optical nonlinearity of (Ba0.7Sr0.3)TiO3 ferroelectric thin films fabricated by soft solution processing

(Ba_0.7Sr_0.3)TiO₃ (BST) ferroelectric thin films with perovskite crystal structure were fabricated by soft solution processing on a quartz substrate. The third-order nonlinear optical properties were investigated by using Z-scan technique. Positive nonlinear refractive index and nonlinear absorption coefficient were determined to be 4×10⁻⁷ esu and 1.2×10⁻⁶ m/w, respectively. The real part and imaginary part of third-order optical nonlinear susceptibility were calculated and the values were 6.43×10⁻⁸ and 5.14×10⁻⁸ esu, respectively. All of these results show ferroelectric BST thin film is promising for applications in nonlinear optical devices.     

Optical and nonlinear optical characteristics of the Ge and GaAs nanoparticle suspensions prepared by laser ablation

The laser ablation of Ge and GaAs targets placed in water and ethanol was carried out using the fundamental radiation of nanosecond Nd:YLF laser. The results of preparation and the optical and nonlinear optical characterization of the Ge and GaAs nanoparticle suspensions are presented. The considerable shift of the band gap energy of the nanoparticles compared to the bulk semiconductors was observed. The distribution of nanoparticle sizes was estimated in the range of 1.5-10 nm on the basis of the TEM and spectral measurements. The nonlinear refractive indices and nonlinear absorption coefficients of Ge and GaAs nanoparticles were defined by the z-scan technique using second harmonic radiation of picosecond Nd:YAG laser (λ = 532 nm).     

Fastscan z-scan system for determining optical non-linearities in semiconductors

Traditional z-scan techniques have been used to determine the non-linear optical coefficients of semiconductors. This is usually carried out by scanning a sample along the optical z-axis using a manual or computer-controlled linear translation stage. We report upon a novel z-scan method involving a fastscanning sampleholder: This gives real-time z-scan traces and greatly improves experimental efficiency and applicability. The technique is used here to study the two-photon absorption coefficient of ZnSe.     

Nonlinear responses and optical limiting behavior of Basic Violet 16 dye under CW laser illumination

Nonlinear optical properties of Basic Violet 16 dye solution in water are studied employing different optical techniques. Experiments are performed using the second harmonic of a continuous Nd-Yag laser beam at 532 nm wavelength and 100 mW power. The effect of nonlinearity of Basic Violet 16 dye in broadening the laser beam is observed. The optical limiting behavior is investigated by measuring the transmission of the samples. The third-order nonlinearity, χ³ of Basic Violet 16 dye, is measured using Z-scan data. The nonlinear absorption coefficient is calculated using the open aperture Z-scan data, while its nonlinear refractive index is measured using the closed aperture Z-scan data. All experiments are done for different concentrations and thicknesses of Basic Violet 16 dye solution. The effect of intensity of input laser beam on the nonlinear susceptibility is studied experimentally. Results indicate that Basic Violet 16 dye is a potential candidate for low-power optical limiting applications.     

I-scan thermal lens experiment in the pulse regime for measuring two-photon absorption coefficient

We present a new pump-probe mode-mismatched thermal lens method for pulse excitation aimed to the measurement of nonlinear absorption coefficient in optical materials. We develop a theoretical model based on the Fresnel diffraction approximation and their predictions are verified experimentally with samples of Rhodamine 6G and Rhodamine B in ethanol solution. The principal advantage of this technique is that it does not require any mechanical movement during measurement. Below we perform the new type of thermal lens experiment in the pulse regime for the measurement of nonlinear absorption coefficient in transparent samples and we demonstrate the validity of theoretical predictions using an alternative method to the classical thermal lens technique.     

Third-order nonlinear optical response of Au:SiO 2 thin films: Influence of gold nanoparticle concentration and morphologic parameters

We report a study on the third-order nonlinear optical properties of nanocomposite thin films composed of gold particles embedded in a silica host matrix. Samples of various metal volume fractions, ranging from 8 to 35%, are synthesized by the sputtering technique. Some of them are annealed. Nonlinear optical measurements, which are performed by using the z-scan technique, reveal both a very large nonlinear absorption and a weak nonlinear refraction close to the surface plasmon resonance frequency of the particles. We especially study the effect of the metal concentration and the influence of thermal treatment on the real and imaginary components of the third-order nonlinear susceptibility. Our results reveal that, as the metal concentration reaches a few percent, the mutual electromagnetic interactions between particles greatly enlarge the nonlinear optical response of the material and can not be neglected in the theoretical analysis. Moreover, the thermal treatment leads, for a given concentration, to a significant increase of the nonlinear response, which is ascribed to a modification of the material morphology. We finally point out that the material nonlinear properties are very sensitive to the incident wavelength through the local field enhancement phenomenon. Received 12 December 2001     

Nonlinear properties of polyurethane-urea/multi-wall carbon nanotube composite films

The third-order nonlinear optical properties of polyurethane-urea/multiwalled carbon nanotube composites (PU/MWNT) films with different MWNT concentrations are investigated by the use of the Z-scan technique at a wavelength of 532 nm with a pulse duration of 8 ns. The results reveal that the nonlinear refraction and absorption coefficients are linearly dependent on the MWNT concentration. The negative nonlinear refraction effect is validated from the closed-aperture Z-scan measurements. We find that PU/MWNT films are promising nonlinear optical materials, and the nonlinear coefficients can be controlled.