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.     

Effect of incorporating nonlanthanoidal indium on optical properties of ferroelectric Bi4Ti3O12 thin films

Bi₄Ti₃O₁₂ (BTO) and Bi_3.25In_0.75Ti₃O₁₂ (BTO:In) thin films were prepared on fused quartz and LaNiO₃/Si (LNO) substrates by chemical solution deposition (CSD). Their microstructures, ferroelectric and optical properties were investigated by X-ray diffraction, scanning electron microscope, ferroelectric tester and UV-visible-NIR spectrophotometer, respectively. The optical band-gaps of the films were found to be 3.64 and 3.45 eV for the BTO and BTO:In films, respectively. Optical constants (refractive indexes and extinction coefficients) were determined from the optical transmittance spectra using the envelope method. Following the single electronic oscillator model, the single oscillator energy E₀, the dispersion energy E_d, the average interband oscillator wavelength λ₀, the average oscillator strength S₀, the refractive index dispersion parameter (E₀/S₀), the chemical bonding quantity β, and the long wavelength refractive index n_∞ were obtained and analyzed. Both the refractive index and extinction coefficient of the BTO:In films are smaller than those of the BTO films. Furthermore, the refractive index dispersion parameter (E₀/S₀) increases and the chemical bonding quantity β decreases in the BTO and BTO:In films compared with those of bulk.     

Determination of optical properties in nanostructured thin films using the Swanepoel method

We present the methodological framework of the Swanepoel method for the spectrophotometric determination of optical properties in thin films using transmittance data. As an illustrative case study, we determined the refractive index, thickness, absorption index, and extinction coefficient of a nanostructured 3 mol% Y₂O₃-doped ZrO₂ (yttria stabilized zirconia, 3YSZ) thin film prepared by the sol-gel method and deposited by dipping onto a soda-lime glass substrate. In addition, using the absorption index obtained with the Swanepoel method, we calculated the optical band gap of the film. The refractive index was found to increase, then decrease, and finally stabilize with increasing wavelength of the radiation, while the absorption index and extinction coefficient decreased monotonically to zero. These trends are explained in terms of the location of the absorption bands. We also deduced that this 3YSZ thin film has a direct optical band gap of 4.6 eV. All these results compared well with those given in the literature for similar thin films. This suggests that the Swanepoel method has an important role to play in the optical characterization of ceramic thin films.     

Effect of indium incorporation on the optical properties of spray pyrolyzed Cd0.22Zn0.78S thin films

In this study, effect of indium incorporation on the optical properties is investigated for the spray pyrolyzed onto glass substrates at 275°C substrate temperature undoped and indium doped Cd_0.22Zn_0.78S thin films. The average optical transmittance of all the films was over 77% in the wavelength range between 450 and 800 nm. The optical band gap energies of the thin films have been investigated by the measurement of the optical absorbance as a function of wavelength. The optical absorption studies reveal that the transitions are direct band gaps of 3.02 and 3.05 eV for undoped and doped indium Cd_0.22Zn_0.78S thin films, respectively. The Urbach tail parameter and optical constants such as refractive index, extinction coefficient, and dielectric constants were calculated for these films. The dispersion parameters such as single-oscillator energy and dispersive energy were discussed in terms oft he single-oscillator Wemple—DiDomenico model.     

Effects of Pb addition and heat treatment on optical properties of thermally evaporated Ge1−xSe2Pbx thin films

Thin chalcogenide films of Ge_1−xSe₂Pb_x (x=0, 0.2, 0.4, 0.6 and 0.8) have been prepared by the thermal evaporation technique, from previously synthesized bulk samples. The X-ray diffraction showed the amorphous nature for the as-deposited films and the partially crystalline for the annealed films. The optical constants (the refractive index, n, and absorption index k) were determined for as-deposited and annealed Ge_1−xSe₂Pb_x films of different thicknesses by using spectrophotometeric measurements of the transmittance and reflectance at normal incidence in the spectral range 200-2500 nm. The obtained values of both n and k were found to be independent of the film thickness. The optical absorption edges are described using both the Urbach rule and the indirect transition. In transparent region, the spectral dependences of refractive index were interpreted in the frame of a single oscillator model.     

Z-scan determination of third-order nonlinear optical nonlinearity of three azobenzenes doped polymer films

The third-order nonlinear response of methyl red (MR), methyl orange (MO) and p-dimethylamino benzene arsenic acid (PDBAA) doped polyvinyl alcohol (PVA) films are studied by using the Z-scan technique under 532 nm and 1064 nm excitations. The larger third-order nonlinear refractive index of PDBAA doped PVA film is discussed in terms of fall of the energy level in excited state for the effect of heavy-atom arsenic. At the end, the second hyperpolarizabilities of the films are estimated and the figures of merit are evaluated for their value of applications in ultra-fast all-optical devices.     

Effect of Ag Nanoparticles on Optical Properties of R6G Doped PMMA Films

The composite PMMA films containing Ag nanoparticles and rhodamine 6G are prepared. We investigate the fluorescence properties and nonlinear optical properties of R6G/PMMA films influenced by Ag nanoparticles. The fluorescence enhancement factor is about 3.3. The corresponding nonlinear refractive index is measured to be -2.423 ×10^-8 esu using the Z-scan technique, which is much enhanced compared with the R6G/PMMA film. The results indicate that these enhancements are attributed to surface plasmon resonance of Ag nanoparticles.     

Spectroscopic studies of Nd and Er in KGd(WO4)2 single crystals

Single crystals of KGd(WO₄)₂ doped with Nd³⁺ and Er³⁺ ions were grown by the top seeded solution growth method. Detailed analysis of the room-temperature absorption spectra was performed using the conventional Judd-Ofelt theory and actual dependence of the refractive index on the wavelength. In addition to the intensity parameters Ω_2,Ω_4,Ω₆, the branching ratios and radiative lifetimes were estimated for all possible transitions in the studied spectral region. Those transitions which can be potentially used for laser applications have been identified for both ions.     

Optical properties of SrTiO<Subscript>3</Subscript> thin films by pulsed laser deposition

SrTiO₃ thin films were prepared on a fused-quartz substrate by pulsed laser deposition (PLD). Dense and homogeneous films with a thickness of 260 nm were prepared. Optical constants (refractive index n and extinction coefficient k) were determined from the transmittance spectra using the envelope method. The optical band gap energy of the films was found to be 3.58 eV, higher than the 3.22 eV for bulk SrTiO₃, attributable to the film stress exerted by the substrate. The dispersion relation of the refractive index vs. wavelength follows the single electronic oscillator model. The refractive index and the packing density for the PLD-prepared SrTiO₃ thin films are higher than those for the SrTiO₃ films prepared by physical vapor deposition, sol–gel and RF sputtering. Received: 18 March 2002 / Accepted: 7 October 2002 / Published online: 8 January 2003 RID="*" ID="*"Corresponding author. Fax: +86-25/359-5535, E-mail: mszhang@nju.edu.cn     

FTIR and optical properties for irradiated PVA–GdCl3 and its possible use in dosimetry

There are various chemical and physical changes caused when polymers are exposed to a source of radiation. In the present work, four films of polyvinyl alcohol (PVA) doped with 2, 4, 6 and 8 wt% of gadolinium chloride (GdCl₃) have been irradiated by low-dose fast neutrons using Am-241/Be-9. The structural properties of the synthesized films have been investigated pre- and post-irradiation on the basis of Fourier transform infrared technique. The optical properties of the PVA–GdCl₃ films have been investigated for doses up to 1.2 KGy. The energy gap of the synthesized films showed a neutron dose dependence and was decreased by 0.81 eV after exposing to 1.2 kGy. At a wavelength of 1000 nm, the refractive index of the PVA doped with 8 wt% GdCl₃ has been increased by nearly 16%. The results suggested the possible use of PVA--GdCl₃ as a dosimeter for the neutron beams.     

Thickness dependence of optical parameters for ZnTe thin films deposited by electron beam gun evaporation technique

Zinc telluride thin films with different thicknesses have been deposited by electron beam gun evaporation system onto glass substrates at room temperature. X-ray and electron diffraction techniques have been employed to determine the crystal structure and the particle size of the deposited films. The stoichiometry of the deposited films was confirmed by means of energy-dispersive X-ray spectrometry. The optical transmission and reflection spectrum of the deposited films have been recorded in the wavelength optical range 450-2500 nm. The variation of the optical parameters, i.e. refractive index, n, extinction coefficient, k, with thickness of the deposited films has been investigated. The refractive index dispersion in the transmission and low absorption region is adequately described by the single-oscillator model, whereby the values of the oscillator strength, oscillator position, dispersion parameter as well as the high-frequency dielectric constant were calculated for different film thickness. Graphical representations of the surface and volume energy loss function were also presented.     

Infrared optical properties of Ba(Zr0.20Ti0.80)O3 and Ba(Zr0.30Ti0.70)O3 thin films prepared by sol-gel method

Ba(Zr_xTi_1−x)O₃ (BZT) (x = 0.20 and 0.30) thin films are deposited on Pt(1 1 1)/Ti/SiO₂/Si(1 0 0) substrate by sol-gel method. X-ray diffraction patterns show that the thin films have a good crystallinity. Optical properties of the films in the wavelength range of 2.5-12 μm are studied by infrared spectroscopic ellipsometry (IRSE). The optical constants of the BZT thin films are determined by fitting the IRSE data using a classical dispersion formula. As the wavelength increases, the refractive index decreases, while the extinction coefficients increase. The effective static ionic charges are derived, which are smaller than that in a purely ionic material for the BZT thin films.     

Nonlinear optical response of Au and Ag nanoparticles doped polyvinylpyrrolidone thin films

Colloidal Au and colloidal Ag were prepared by chemical reaction method and the nonlinear optical properties of Au and Ag nanoparticles doped polyvinylpyrrolidone (PVP) composite films were investigated using Z-scan technique with 38 ps pulses at 532 nm. Open aperture Z-scan measurements indicated that both the Au/PVP and Ag/PVP composite films exhibited reverse saturable absorption. Nonlinear absorption coefficients and third-order nonlinear refractive indices were determined. The mechanisms accounting for the process of nonlinear refractions were analyzed and the figures of merit W and T of the Au/PVP and Ag/PVP composite films were evaluated.     

Ultrasensitive UV-tunable grating in all-solid photonic bandgap fibers

We study the shift of a long period grating’s resonance wavelength with UV induced refractive index changes in an all-solid photonic bandgap fiber. A long period grating is mechanically imprinted in an all-solid photonic bandgap fiber with Germanium doped silica high-index rods in a lower-index silica background. The index of the high-index rods is modified through UV exposure, and we observe that the long period grating’s resonance shifts with the bandgaps. With a sensitivity of 21,000 nanometers per refractive index unit and a 8.8 nm resonance width changes of refractive index of 3 × 10⁻⁶ are in principle detectable     

Derivation of the optical constants of spin coated CeO2-TiO2-ZrO2 thin films prepared by sol-gel route

Ternary thin films of cerium titanium zirconium mixed oxide were prepared by the sol-gel process and deposited by a spin coating technique at different spin speeds (1000-4000 rpm). Ceric ammonium nitrate, Ce(NO₃)₆(NH₄)₂, titanium butoxide, Ti[O(CH₂)₃CH₃]₄, and zirconium propoxide, Zr(OCH₂CH₂CH₃)₄, were used as starting materials. Differential calorimetric analysis (DSC) and thermogravimetric analysis (TGA) were carried out on the CeO₂-TiO₂-ZrO₂ gel to study the decomposition and phase transition of the gel. For molecular, structural, elemental, and morphological characterization of the films, Fourier Transform Infrared (FTIR) spectral analysis, X-ray diffraction (XRD), energy dispersive X-ray spectroscopy (EDS), cross-sectional scanning electron microscopy (SEM), and atomic force microscopy (AFM) were carried out. All the ternary oxide thin films were amorphous. The optical constants (refractive index, extinction coefficient, band gap) and thickness of the films were determined in the 350-1000 nm wavelength range by using an nkd spectrophotometer. The refractive index, extinction coefficient, and thickness of the films were changed by varying the spin speed. The oscillator and dispersion energies were obtained using the Wemple-DiDomenico dispersion relationship. The optical band gap is independent of the spin speed and has a value of about E_g≈2.82±0.04 eV for indirect transition.     

Microstructural, optical and photocatalytic properties of CdS doped TiO2 thin films

CdS doped TiO₂ thin films (with CdS content=0, 3, 6, 9 and 12 at%) were grown on glass substrates. The X-ray diffraction analysis revealed that the films are polycrystalline of monoclinic TiO₂ structure. The microstructure parameters of the films such as crystallite size (D_ν) and microstrain (e) are calculated. Both the crystallites size and the microstrain are decreased with increasing CdS content. The optical constants have been determined in terms of Murmann's exact equations. The refractive index and extinction coefficient are increased with increasing CdS content. The optical band gap is calculated in the strong absorption region. The possible optical transition in these films is found to be an allowed direct transition. The values of E_g^opt are found to decrease as the CdS content increased. The films with 3 at% CdS content have better decomposition efficiency than undoped TiO₂. The films with 6 at% and 9 at% CdS content have decomposition efficiency comparable to that of undoped TiO₂, although they have lower band gap. The CdS doped TiO₂ could have a better impact on the decomposing of organic wastes.     

Factors affecting optical dispersion in borate glass systems

Series of ternary glass systems namely, Na₂O, B₂O₃, and RO (R=Ba or Mg) doped with TiO₂ are synthesized. The present glasses are dictated by requirement for a small refractive index and a small nonlinear coefficient needed for waveguide and laser fabrication requirements. The effect of MgO and BaO as alkaline earth metals on the optical properties of the glass systems is investigated. The dependence of the refractive index and extinction coefficient dispersion curves on composition is carried out over a wavelength range of 0.3-. Applying a genetic algorithm technique, the parameters of Sellmeier dispersion formula that fit index data to accuracy consistent well with the measurements are given. The zero material dispersion-wavelength (ZMDW) and group velocity are also determined using the refractive index data. The Fermi level is calculated exploiting the extinction coefficient dispersion curves. The absorption coefficient, both direct and indirect optical energy gaps, and Urbach energy are evaluated using the absorption edge calculations. The different factors that play a role for controlling the refractive indices such as coordination number, electronic polarizability, field strength of cations, bridging and nonbridging oxygen, and optical basicity are discussed in accordance with the obtained index data. IR spectroscopy is used as a structural probe of the nearest-neighbor environment in the glass network.     

Nonlinear optical absorption in Bi3TiNbO9 thin films using Z-scan?technique

Bi₃TiNbO₉ (BTN) thin films with layered perovskite structure were fabricated on fused silica by pulsed laser deposition. The XRD pattern revealed that the films are single-phase perovskite and highly (00l) textured. Their fundamental optical constants, such as band gap, linear refractive index, and linear absorption coefficient, were obtained by optical transmittance measurements. The dispersion relation of the refractive index vs. wavelength follows the single electronic oscillator model. The nonlinear optical absorption of the films was investigated by single beam Z-scan method at a wavelength of 800 nm with laser duration of 80 fs. We obtained the nonlinear absorption coefficient β=1.44×10⁻⁷ m/W. The results show that the BTN thin films are promising for applications in absorbing-type optical devices.     

Nanocrystalline formation and optical properties of germanium thin films prepared by physical vapor deposition

Amorphous and nanocrystalline germanium thin films were prepared on glass substrates by physical vapor deposition (PVD). The influence of thermal annealing on the characteristics of the Ge thin films has been investigated. X-ray diffraction (XRD) and SEM show amorphous structure of films deposited at room temperature. After thermal annealing, the crystallinity was improved when the annealing temperature increases. The Ge thin films annealed at different temperatures in air were nanocrystalline, having the face-centered cubic structure with preferred orientation along the 〈1 1 1〉 direction. The nanostructural parameters have been evaluated by using a single-order Voigt profile analysis. Moreover, the analysis of the optical transmission and reflection behavior was carried out. The values of direct and indirect band gap energies for amorphous and nanocrystalline phases are 0.86±0.02, 0.65±0.02 and 0.79±0.02, 0.61±0.02 eV, respectively. In addition, the complex optical functions for the wavelength range 600-2200 nm are reported. The refractive index of the nanocrystalline phase drops from 4.80±0.03 to 2.04±0.02, and amorphous phase changes from 5.18±0.03 to 2.42±0.02 for the whole wavelength range. The dielectric functions ε₁ and ε₂ of the deposited films were recorded as a function of wavelength within the range from 600 to 2200 nm.     

Structure and optical analysis of Ta2O5 deposited on infrasil substrate

Electron beam gun technique was used to prepare Ta₂O₅ thin films onto infrasil substrates of thicknesses 333 and 666 nm. The structure characterization was investigated using X-ray diffraction patterns. Transmittance measurements in the wavelength range (240-2000 nm) were used to calculate the refractive index n and the absorption index k depending on Swanepole's method. The dispersion curve of the refractive index shows an anomalous dispersion in the absorption region and a normal one in the transparent region. The analysis of the optical absorption data revealed that the optical band gap E_g was indirect transition. It was found that the refractive index dispersion data obeyed the single oscillator of the Wemple-DiDomenico model, from which the dispersion parameters (E_o and E_d) and the high frequency dielectric constant were determined. The electric free carrier susceptibility and the carrier concentration to the effective mass ratio were estimated according to the model of Spitzer and Fan. Graphical representation of the relaxation time as a function of photon energy was also presented.