Analysis of codeposited Gd2O3/SiO2 composite thin films by phase modulated spectroscopic ellipsometric technique

Tailoring of the refractive index of optical thin films has been a very fascinating as well as challenging topic for developing new generation optical coatings. In the present work a novel Gd₂O₃/SiO₂ composite system has been experimented and probed for its superior optical properties through phase modulated spectroscopic ellipsometry, spectrophotometry and atomic force microscopy. The optical parameters of the composite films have been evaluated using Tauc-Lorentz (TL) formulations. In order to derive the growth dependent refractive index profiles, each sample film has been modeled as an appropriate multilayer structure where each sub-layer was treated with the above TL parameterizations. All codeposited films demonstrated superiority with respect to the band gap and morphological measurements. At lower silica mixing compositions such as in 10-20% level, the composite films depicted superior spectral refractive index profile, band gap as well as the morphology. This aspect highlighted the fact that microstructural densifications in composite films can override the chemical compositions while deciding the refractive index and optical properties in such thin films.     

Morphological, microstructural and optical properties supremacy of binary composite films—A study based on Gd2O3/SiO2 system

Composites are pragmatic choices for tailoring the material to have a desired property. Besides, such thin films have scopes to display superior optical, microstructural and morphological properties which are otherwise not possible to obtain from the pure component films. Vapor-phase-mixed binary composite Gd₂O₃/SiO₂ thin film is one such interesting system where band gap as well as refractive index superiority is observed simultaneously under certain compositional mixings. Such and similar observations in composites cannot be explained by Moss empirical rule. Our systematic study on the microstructure of this composite system based on ellipsometry and scanning probe microscopy has satisfactorily provided the information that can explain such optical properties supremacy. Morphological measurements and its derived parameters like autocorrelation and height-height correlation functions have provided several clues that represent the superior grain structures of the composites. Besides, refractive index modeling through effective single oscillator model has strongly supported such analysis results favoring the superior microstructure in composite films.     

Structure-related infrared optical properties of BaTiO3 thin films grown on Pt/Ti/SiO2/Si substrates

BaTiO₃ thin films with different thickness have been grown on Pt/Ti/SiO₂/Si substrates by a modified sol-gel method. X-ray diffraction analyses show that the BaTiO₃ thin films are polycrystalline. The crystalline quality of the films is improved with increasing thickness. The infrared optical properties of the BaTiO₃ thin films have been investigated using an infrared spectroscopic ellipsometry in the wave number range of 800-4000 cm⁻¹ (2.5-12.5 μm). By fitting the measured pseudodielectric functions with a three-phase model (Air/BaTiO₃/Pt), and a derived classical dispersion relation for the thin films, the optical constants and thicknesses of the thin films have been simultaneously obtained. The refractive index of the BaTiO₃ thin films increases and on the other hand, the extinction coefficient does not change with increasing thickness in the entirely measured wave number range. The dependence of the refractive index on the film thickness has been discussed in detail and was mainly due to both the crystalline quality of the films and packing density. Finally, the absorption coefficient was calculated in the infrared region for applications in the pyroelectric IR detectors.     

Correlation of optical and microstructural properties of Gd2O3 thin films through phase-modulated ellipsometry and multi-mode atomic force microscopy

Gadolinium oxide thin films have been prepared by electron beam evaporation with different reactive oxygen pressures at low ambient substrate temperature. These thin films have been analyzed with phase-modulated spectroscopic ellipsometry and multi-mode atomic force microscopy (AFM). The distinct influences of oxygen pressure on surface topographies, microstructures and refractive indices of the thin films have been observed from the results of these advanced measurements. Both these techniques have displayed very strong co-relationships in the characterisation results acquired through respective modes of measurements and data analysis. Unequivocally, these two techniques indicated an optimum value of the oxygen pressure leading to best optical and structural properties of such a novel optical coating material.     

Influence of ZrO2 in HfO2 on reflectance of HfO2/SiO2 multilayer at 248 nm prepared by electron-beam evaporation

Influence of ZrO₂ in HfO₂ on the reflectance of HfO₂/SiO₂ multilayer at 248 nm was investigated. Two kinds of HfO₂ with different ZrO₂ content were chosen as high refractive index material and the same kind of SiO₂ as low refractive index material to prepare the mirrors by electron-beam evaporation. The impurities in two kinds of HfO₂ starting coating materials and in their corresponding single layer thin films were determined through glow discharge mass spectrum (GDMS) technology and secondary ion mass spectrometry (SIMS) equipment, respectively. It showed that between the two kinds of HfO₂, either the bulk materials or their corresponding films, the difference of ZrO₂ was much larger than that of the other impurities such as Ti and Fe. It is the Zr element that affects the property of thin films. Both in theoretical and in experimental, the mirror prepared with the HfO₂ starting material containing more Zr content has a lower reflectance. Because the extinction coefficient of zirconia is relatively high in UV region, it can be treated as one kind of absorbing defects to influence the optical property of the mirrors.     

Effects of Annealing on Microstructure and Optical Properties of TiO2 Sculptured Thin Films

The evolution of microstructure and optical properties of TiO2 sculptured thin films under thermal annealing is reported. XRD, field emission SEM, UV-Vis-NIR spectra are employed to characterize the microstructural and optical properties. It is found that the optimum annealing temperature for linear birefringence is 500℃. The maximum of transmission difference for linear birefringence is up to 18%, which is more than twice of that in as-deposited thin films. In addition, the sample annealed at 500℃ has a minimum of column angle about 12℃. The competitive process between the microstructural and optical properties is discussed in detail. Post-annealing is a useful method to improve the linear birefringence in sculptured thin films for practical applications.     

AlF3 film deposited by IAD with end-Hall ion source using SF6 as working gas

A novel and effective process to fabricate high quality fluoride thin films was presented. Aluminum fluoride films deposited by a conventional thermal evaporation with an ion-assisted deposition (IAD) using SF₆ as a working gas at around room temperature were investigated. In this study, the optimal voltage and current, 50 V and 0.25 A, were found according to the optical properties of the films: high refractive index (1.489 at 193 nm), low optical absorption and extinction coefficient (<10⁻⁴ at 193 nm) in the UV range. The physical properties of the film are high packing density and amorphous without columnar structure. It was proved that using SF₆ working gas in IAD process is a good choice and significantly improves the quality of AlF₃ films.     

Determination and analysis of non-linear index profiles in electron-beam-deposited MgOAl2O3ZrO2 ternary composite thin-film optical coatings

Thickness-dependent index non-linearity in thin films has been a thought provoking as well as intriguing topic in the field of optical coatings. The characterization and analysis of such inhomogeneous index profiles pose several degrees of challenges to thin-film researchers depending upon the availability of relevant experimental and process-monitoring-related information. In the present work, a variety of novel experimental non-linear index profiles have been observed in thin films of MgOAl₂O₃ZrO₂ ternary composites in solid solution under various electron-beam deposition parameters. Analysis and derivation of these non-linear spectral index profiles have been carried out by an inverse-synthesis approach using a real-time optical monitoring signal and post-deposition transmittance and reflection spectra. Most of the non-linear index functions are observed to fit polynomial equations of order seven or eight very well. In this paper, the application of such a non-linear index function has also been demonstrated in designing electric-field-optimized high-damage-threshold multilayer coatings such as normal- and oblique-incidence edge filters and a broadband beam splitter for p-polarized light. Such designs can also advantageously maintain the microstructural stability of the multilayer structure due to the low stress factor of the non-linear ternary composite layers. PACS 78.20.Bh; 78.20.Ci; 77.55.+f; 81.15.Ef     

Third-order optical nonlinearities of lead-free (Na1−xKx)0.5Bi0.5TiO3 thin films

(Na_1−xK_x)_0.5Bi_0.5TiO₃ (NKBT) (x = 0.1, 0.2, and 0.3) thin films with good surface morphology and rhombohedral perovskite structure were fabricated on quartz substrates by a sol-gel process. The fundamental optical constants (the band gaps, linear refractive indices and absorption coefficients) of the films were obtained through optical transmittance measurements. The nonlinear optical properties were investigated by Z-scan technique performed at 532 nm with a picosecond laser. A two-photon absorption effect closely related with potassium-doping content was found in thin films, and the nonlinear refractive index n₂ increases evidently with potassium-doping. The real part of the third-order nonlinear susceptibility χ⁽³⁾ is much larger than its imaginary part, indicating that the third-order optical nonlinear response of the NKBT films is dominated by the optical nonlinear refractive behavior. These results show that NKBT thin films have potential applications in nonlinear optics.     

Influence of temperature annealing on optical properties of SrTiO3/BaTiO3 multilayered films on indium tin oxide

We have prepared SrTiO₃/BaTiO₃ thin films with multilayered structures deposited on indium tin oxide (ITO) coated glass by a sol-gel deposition and heating at 300-650 °C. The optical properties were obtained by UV-vis spectroscopy. The films show a high transmittance (approximately 85%) in the visible region. The optical band gap of the films is tunable in the 3.64-4.19 eV range by varying the annealing temperature. An abrupt decrease towards the bulk band gap value is observed at annealing temperatures above 600 °C. The multilayered film annealed at 650 ° C exhibited the maximum refractive index of 2.09-1.91 in the 450-750 nm wavelength range. The XRD and AFM results indicate that the films annealed above 600 ° C are substantially more crystalline than the films prepared at lower temperatures which were used to change their optical band gap and complex refractive index to an extent that depended on the annealing temperature.     

Ge20Sb15Se65薄膜的热致光学特性变化研究

采用磁控溅射法制备了Ge₂₀Sb₁₅Se₆₅薄膜, 研究热处理温度(150—400 ℃)对薄膜光学特性的影响. 通过分光光度计、X射线衍射仪、显微拉曼光谱仪对热处理前后薄膜样品 的光学特性和微观结构进行了表征, 并根据Swanepoel方法以及Tauc公式分别计算了薄膜折射率色散曲线和光学带隙等参数. 结果表明当退火温度(T_a)小于薄膜的玻璃转化温度(T_g)时,薄膜的光学带隙(E_g^opt)随着退火温度的增加由1.845 eV上升至1.932 eV, 而折射率由2.61降至2.54; 当退火温度大于薄膜的玻璃转化温度时,薄膜的光学带隙随退火温度的增加由1.932 eV降至1.822 eV, 折射率则由2.54增至2.71. 最后利用Mott和Davis提出的非晶材料由非晶到晶态的结构转变模型对结果进行了解释, 并通过薄膜XRD和Raman光谱进一步验证了结构变化是薄膜热致变化的重要原因. 关键词： 20Sb₁₅Se₆₅薄膜')" href="#">Ge₂₀Sb₁₅Se₆₅薄膜 热处理 光学带隙 折射率     

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.     

Waveguide properties and optical switching of prism-coupled Au:SiO2 nanocomposite films

In this study, we present theoretical and experimental analyses on the waveguide mode properties of prism-coupled Au:SiO₂ nanocomposite films with the near infrared laser of 1550 nm wavelength where the optical absorption diminished enough for the generation of guided mode. The evolution of guided mode in the nanocomposite waveguide and its propagation properties were also evaluated. As an effective way of utilizing the surface plasmon resonance properties for the application to optical switching devices, we employed an attenuated total internal reflection type optical switch geometry and tested its effectiveness for the absorptive opto-functional materials system using a cross-modulation technique with 532-nm pump and 1550-nm probe beams. The index change probe beam experiences was found to be purely refractive in nature and negative in sign, presumably due to the photo-thermal effect induced in the nanocomposite film by the irradiation of pump beam.     

Ellipsometric studies on TiO2 thin films synthesized by spray pyrolysis technique

TiO₂ thin films were synthesized on quartz substrates at substrate temperatures of 350 °C and 450 °C by thermal spray pyrolysis technique using titanium oxy-acetyl acetonate as a precursor. The optical properties of the thin films were characterized by a Spectroscopic Ellipsometer (SE). The surface morphology of the thin films was studied using Atomic Force Microscopy (AFM). The surface roughness values obtained using AFM and SE was compared. The refractive indices of the films were computed using a point by point ellipsometric data extraction procedure. The porosity of the films were modeled from the optical data by effective medium approximation and corroborated from empirical relations. Using Forouhi-Bloomer optical dispersion model, further treatment of SE data was carried out. The experimental investigations and modeling of the data were directed towards optical benchmarking of spray pyrolyzed titania thin films.     

Optical and structural studies on Ba(Mg1/3Ta2/3)O3 thin films obtained by radiofrequency assisted pulsed plasma deposition

Single-phase Ba(Mg_1/3Ta_2/3)O₃ thin films were prepared by radiofrequency plasma beam assisted pulsed laser deposition (RF-PLD) starting from a bulk ceramic target synthesized by solid state reaction. Atomic force microscopy, X-ray diffraction and spectroscopic ellipsometry were used for morphological, structural and optical characterization of the BMT thin films. The X-ray diffraction spectra show that the films exhibit a polycrystalline cubic structure. From spectroscopic ellipsometry analysis, the refractive index varies with the thin films deposition parameters. By using the transmission spectra and assuming a direct band to band transition a band gap value of ≈4.72 eV has been obtained.     

紫外光辐照对TiO2薄膜光学性能的影响

 采用电子束热蒸发技术在不同工艺下制备了TiO2薄膜,利用椭偏仪和分光光度计研究了紫外光辐照后薄膜光学特性的变化。实验结果表明：不同工艺下制备的TiO2薄膜经相同条件的紫外光辐照后,其折射率均有所下降,折射率的变化量随着沉积速率上升、基底温度上升、工作真空度下降分别有增大的趋势。薄膜的透射率在紫外光辐照后有一定下降。相同工艺条件下制备的TiO2薄膜,其折射率随着辐照时间的增加,先迅速降低,随后又有所增加,但均低于辐照前薄膜的折射率。     

Optical and acoustic properties of TeO2/WO3 glasses with small amount of additive ZrO2

The optical and acoustic properties of tellurite glasses in the system TeO₂/ZrO₂/WO₃ have been investigated. The refractive index at different wavelengths and the optical spectra of the glasses have been measured. From the refractive index and absorption edge studies for prepared glasses, the optical parameter viz; optical band gap (E_opt), Urbach energy, (ΔE), dispersion energy, E_d, and the average oscillator energy, E₀, have been calculated. Sound velocities were measured by pulse echo technique. From these velocities and densities values, various elastic moduli were calculated. The variations in the refractive index, optical energy gap and elastic moduli with WO₃ content have been discussed in terms of the glass structure. Quantitatively, we used the bond compression model for analyzing the room temperature elastic moduli data. By calculating the number of bonds per unit volume, the average stretching force constant, and the average ring size we can extract valuable information about the structure of the present glasses.     

Photoexpansion and photobleaching effects in oxysulfide thin films of the GeS2+Ga2O3 system

Oxysulfide systems undergo structural transformations upon illumination with laser light of near bandgap energy, as well as chalcogenide materials (glasses and films). In this paper, photoinduced effects such as photoexpansion and photobleaching were observed in GeS₂+Ga₂O₃ (GGSO) films synthesized by electron beam evaporation. A surface expansion of the thin films and a shift to shorter wavelengths of the optical absorption edge were observed as a result of UV laser irradiation (wavelength of 351 nm) and they are dependent on laser power density, exposure time and film composition. These parameters were varied to evaluate and enhance the observed effects. In addition, the irradiated GGSO samples exhibited a decrease in refractive index, measured with a prism-coupling technique, which makes these films suitable candidates for applications as gratings and waveguides in integrated optics.     

Structural and optical properties of pulsed laser deposited SrBi2Nb2O9 thin films

SrBi₂Nb₂O₉ (SBN) thin films were prepared on fused quartz substrates at room temperature by pulsed laser deposition. The influence of deposition parameters such as target-to-substrate distance, oxygen pressure and annealing temperature on film crystallization behavior was investigated by X-ray diffraction. Results indicated that the films grown at the optimum processing conditions have polycrystalline structure with a single layered perovskite phase. The optical transmittance of the films prepared at various oxygen pressures was measured in the wavelength range 200–900 nm using UV–vis spectrophotometer. The results showed that there is a red shift in the optical absorption edge with a rise in the oxygen pressure. Refractive index as a function of wavelength and optical band gap of the films were determined from the optical transmittance spectra. The results indicated that the refractive index increases with increasing oxygen pressure at the same incident light wavelength, while the band gap reduces from 4.13 to 3.88 eV. It may be attributed to an increase in packing density and grain size, and decrease in oxygen defects.     

Size dependence of non-linear optical properties of SiO2 thin films containing InP nanocrystals

SiO₂ composite thin films containing InP nanocrystals were fabricated by radio-frequency magnetron co-sputtering technique. The microstructure of the composite thin films was characterized by X-ray diffraction and Raman spectrum. The optical absorption band edges exhibit marked blueshift with respect to bulk InP due to strong quantum confinement effect. Non-linear optical absorption and non-linear optical refraction were studied by a Z-scan technique using a single Gaussian beam of a He-Ne laser (632.8 nm). We observed the saturation absorption and two-photon absorption in the composite films. An enhanced third-order non-linear optical absorption coefficient and non-linear optical refractive index were achieved in the composite films. The nonlinear optical properties of the films display the dependence on InP nanocrystals size. Received: 27 June 2000 / Accepted: 27 June 2000 / Published online: 13 September 2000