Delayed onset of photochromism in molybdenum oxide films caused by photoinduced defect formation

We report the photochromic properties of amorphous MoO₃ films deposited by dc sputtering with different O₂ flow rates. The kinetics of film coloration under UV light irradiation is determined using optical transmission spectroscopy. Changes in the absorbance and refractive index were derived from the analysis of transmittance spectra. The absorbance spectra exhibited a growing broad peak centered around 830 nm, which was induced by the UV irradiation. In the early stages of irradiation, the absorbance of the films did not change but their refractive indices did change. This induction time was correlated with the O₂ partial pressure during the film deposition, which was controlled by the O₂ flow rate. The origins of this observation are discussed.     

Delayed onset of photochromism in molybdenum oxide films caused by photoinduced defect formation

Abstract

We report the photochromic properties of amorphous MoO₃ films deposited by dc sputtering with different O₂ flow rates. The kinetics of film coloration under UV light irradiation is determined using optical transmission spectroscopy. Changes in the absorbance and refractive index were derived from the analysis of transmittance spectra. The absorbance spectra exhibited a growing broad peak centered around 830 nm, which was induced by the UV irradiation. In the early stages of irradiation, the absorbance of the films did not change but their refractive indices did change. This induction time was correlated with the O₂ partial pressure during the film deposition, which was controlled by the O₂ flow rate. The origins of this observation are discussed.     

Low refraction properties of F-doped SiOC:H thin films prepared by PECVD

Low refractive index materials which F-doped SiOC:H films were deposited on Si wafer and glass substrate by low temperature plasma enhanced chemical vapor deposition (PECVD) method as a function of rf powers, substrate temperatures, gas flow ratios (SiH₄, CF₄ and N₂O). The refractive index of the F-doped SiOC:H film continuously decreased with increasing deposition temperature and rf power. As the N₂O gas flow rate decreases, the refractive index of the deposited films decreased down to 1.378, reaching a minimum value at an rf power of 180 W and 100 °C without flowing N₂O gas. The fluorine content of F-doped SiOC:H film increased from 1.9 at.% to 2.4 at.% as the rf power was increased from 60 W to 180 W, which is consistent with the decreasing trend of refractive index. The rms (root-mean-square) surface roughness significantly decreased to 0.6 nm with the optimized process condition without flowing N₂O gas.     

Linear and non-linear optics of nano-scale 2′,7′dichloro-fluorescein/FTO optical system: Bandgap and dielectric analysis

2′,7′ dichloro-Fluorescein (DCF) is a promising organic semiconductor material in different technological aspects such as solar cell, photodiode, Schottky diode. DCF thin film/conductive glass (FTO glass) was prepared by a low-cost spin coating technique. The spectrophotometric data such as the absorbance, reflectance and transmittance were cogitated in the 350–2500 nm wavelength range, at the normal incidence. The absorption (n) and linear refractive indices (k) were computed using the Fresnel's equations. The optical band gap was evaluated and it was found that there is two band gap described as follows: (1) It is related to the band gap of FTO/glass which is equal 3.4 eV and (2) the second one is related to the absorption edge of DCF equals 2.25 eV. The non-linear parameters such as the refractive index (n₂) and optical susceptibility χ⁽³⁾ were evaluated by the spectroscopic method based on the refractive index. Both (n₂) and χ⁽³⁾ increased rapidly on increasing the wavelength with redshift absorption. Our work represents a new idea about using FTO glass for a new generation of the optical device and technology.     

Temperature-dependent Sellmeier equations of nonlinear optical crystal Na3La9O3(BO3)8

The principal refractive indices of Na₃La₉O₃(BO₃)₈ (NLBO) crystal in the wavelength range of 0.363–2.325 μm were accurately measured by using the minimum deviation method within the temperature range from 23.5 °C to 160 °C. We derived the expressions of thermal refractive index coefficient as a function of wavelength that could be used to calculate the principal refractive indices at different wavelengths. The temperature-dependent Sellmeier equations were also derived and used to calculate the phase-matching (PM) angles for a frequency conversion device based on NLBO crystal at different temperatures. We found that the thermal refractive index coefficients of NLBO crystal changed from positive to negative values with the increase of wavelength. In addition, the phase matching conditions for third harmonic generation (THG) at different temperatures were also investigated.     

Infrared Refractive Index and Extinction Coefficient of Polyimide Films

We have measured the transmittance of several polyimide (C₂₂H₁₀N₂O₄) films at wave numbers from 6000 to 500 cm^–1 (wavelengths from 1.67 to 20 m) using a Fourier-transform infrared (FT-IR) spectrometer. The free-standing polyimide films are made by spin coating and thermal curing processes. The thickness of the films ranges from 0.1 to 4 m. In the nonabsorbing region from 6000 to 4000 cm^–1, the minimum transmittance caused by interference is used to obtain the refractive index for film thicknesses greater than 1 m. The film thicknesses are determined by fitting the spectral transmittance using the refractive index. Molecular absorption strongly reduces the transmittance at wave numbers from 2000 to 500 cm^–1. The optical constants, i.e., the refractive index and the extinction coefficient, are determined from the measured transmittance for several films of different thickness using a least-squares method. A Lorentzian oscillator model is also developed, which in general agrees well with the measured transmittance at wave numbers from 6000 to 500 cm^–1. This study will facilitate the application of polyimide films in the fabrication of infrared filters and other optoelectronic applications. The methods presented in this paper can be used to determine the optical constants of other types of thin-film materials.     

Characterization of high quality tantalum pentoxide film synthesized by oxygen plasma enhanced pulsed laser deposition

Tantalum pentoxide films were deposited on BK7 glass substrates using oxygen plasma enhanced pulsed laser deposition (OPE-PLD). X-ray diffraction, atomic force microscopy, ultraviolet–visible–near infrared scanning spectrophotometry, and spectroscopic ellipsometry were used to characterize the crystallinity, microscopic morphology and optical properties of films. Results show that the film roughness increased with the increase of oxygen pressure, and decreased with the application of OPE. Meanwhile the use of oxygen plasma in a 2 Pa O₂ pressure resulted in the transmittance of the thin film of 91.8% at its peak position (the transmittance of bare substrate). Moreover, the root-mean-square roughness as low as 0.736 nm, and refractive index of 2.18 at 633 nm wavelength, close to the refractive index of bulk Ta₂O₅ (~ 2.20 at 633 nm wavelength), were obtained.     

Microstructure, optical and dielectric properties of compositional graded (Ba,Sr)TiO3 thin films derived by RF magnetron sputtering

Thin films of compositional graded Ba_1−x Sr _x TiO₃ (BST) (x decreasing from 0.3 to 0) were prepared on fused quartz and Pt/Ti/SiO₂/Si substrates by RF magnetron sputtering. The microstructure of the graded BST thin films was characterized by X-ray diffraction (XRD). It indicates that the films were crystallized with peroveskite structure and (100) + (111) preferred orientation. The refractive index and the band gap were determined at room temperature in the wavelength 200–1100 nm from spectrophotometric measurements of the transmittance. The average value of the refractive index is found to be 2.17 for the graded BST films in the wavelength 400–1000 nm. The optical band gap of the graded BST film was 3.77 eV. The dielectric measurement showed that the dielectric constant and loss factor of the graded BST film was 318.04 and 0.028 at 100 KHz and room temperature.     

Evaluation of thin film passivation using inorganic Mg-Zn-F heterointerface for polymer light emitting diode

In this study, we manufactured Mg-Zn-F targets using magnesium fluoride (MgF₂) and zinc (Zn). The passivation films were deposited on a poly-ethylenenaphthalate (PEN) substrate using a radio-frequency magnetron sputter. The thickness of the manufactured passivation film was 120 nm. Among the three targets tested, the 4:6 weight target of MgF₂ to Zn resulted in films with the highest Zn content that would increase the packing density of the thin film. The water vapor transmission rate of a 120 nm Mg-Zn-F film prepared from this target and inserted between two 40 nm MgF₂ interlayers on PEN was 2.9 × 10^− 2 g/(m² day) at a relative humidity of 90% and a temperature 38 °C. Its optical transmittance was approximately 80%.     

Optical dispersion of homogeneously mixed ZnSMgF2 films

Mixed films of ZnSMgF₂ were prepared by co-evaporation from a single source. The dispersion of the optical constants was obtained from the reflectance and transmittance data of the films for various compositions in the spectral range 2000–7000 Å. The values of the optical constants of the mixed films at any wavelength lie between the values of the optical constants of pure ZnS and MgF₂ films. The refractive index of the mixed films closely obeys the Lorentz-Lorenz relation at wavelengths at which the absorption is small. The fundamental absorption edge of the mixed films shifts from that of MgF₂ to that of ZnS continuously but non-linearly on increasing the concentration of ZnS in MgF₂. Thus it is possible to use these films as variable frequency cut-off filters. The fundamental absorption edge of the mixed films follows the (hv-E_g)² relation, indicating an indirect optical transition, in sharp contrast to the direct optical transition observed in bulk ZnS.     

聚合物乳液粒子制备纳米多孔增透膜

采用提拉法在载玻片上沉积了PMMA/PS混合乳液粒子,用环己烷选择性地溶解掉表层PS粒子,制备了孔隙率从表向里梯度变化的纳米粒子增透膜,在578 nm处透过率可达99.5%;研究了两种聚合物纳米粒子的比例及环己烷浸泡时间对增透性能的影响。本方法可用于大面积和不规则基材上制备增透膜,并解决了提拉法成膜的粒子堆积紧密、孔隙率低且不易调节的缺点,使粒子膜的透过率大幅度提高。     

Microstructure and optical properties of Al2O3/ZrO2 nano multilayer thin films prepared by pulsed laser deposition

The aluminium oxide/zirconium oxide (Al₂O₃/ZrO₂) nanolaminate thin films (5/20 nm with 4 bilayers, 5/15 nm with 5 bilayers and 5/10 nm with 7 bilayers) were deposited on Si (100) and quartz substrates at an optimized oxygen partial pressure of 3 × 10⁻² mbar at room temperature using pulsed laser deposition. The multilayer films were characterized using X-ray diffraction, X-ray reflectivity, Atomic force microscopy and UV–Visible spectroscopy. The X-ray diffraction studies showed amorphous nature for 5/20 nm film, whereas 5/15 nm and 5/10 nm multilayers showed only tetragonal zirconia at room temperature. X-ray reflectivity studies showed the Kiessig fringes and Bragg peaks, indicating the well defined formation of individual layers and bilayer periodicity in the multilayer films. The AFM studies showed the RMS roughness values of 0.7 nm, 0.9 nm and 1.1 nm for 5/10 nm, 5/15 nm and 5/20 nm multilayers respectively. The optical performance of the combined Al₂O₃/ZrO₂ nanolaminates showed that the refractive indices of the films increased from 1.75 to 1.99 with the decrease of ZrO₂ layer thickness from 20 to 10 nm.     

Reflectance spectra and refractive index of a Nd:YAG laser-oxidized Si surface

The reflectance spectra and refractive index of Nd:YAG laser-oxidized SiO₂ layers with thicknesses from 15 to 75 nm have been investigated with respect to the laser beam energy density and substrate temperature. Thickness and refractive index of films have been determined from reflectance measurements at normal light incidence in the spectral range 300–800 nm. It was found that the oxide-growth conditions at higher substrate temperatures and laser powers greater than 3.36 J cm⁻² provides a better film quality in terms of both optical thickness and refractive index. However, the refractive indices of the films are smaller in the whole spectral range studied as compared to that of conventional thermally grown SiO₂. This might be due to the porous structure formed during the laser-assisted oxidation. The results suggest the need of post-oxidation annealing to improve the refractive indices of the films, suitable for Si-device applications.     

The optical properties of Bi3.25La0.75Ti3O12 thin films with different thickness prepared by chemical solution deposition

Bi_3.25La_0.75Ti₃O₁₂(BiLT) thin films with different thickness were successfully deposited onto fused quartz by chemical solution deposition. X-ray diffraction analysis shows that BiLT thin films are polycrystalline with (0 0 2)-preferred orientation. The dispersion of refractive indices of the BiLT thin films was investigated by the optical transmittance spectrum. The optical band gap energy was estimated from the graph of (hνα)² versus hν. The results show that the refractive index and band-gap energy of the BiLT thin films decrease with the films thickness.     

Optical properties of TiO2 thin films deposited on polycarbonate by ion beam assisted evaporation

TiO₂ thin films were deposited on polycarbonate (PC) substrate by ion beam assisted evaporation. The grain size increased with the ion anode voltage and film thickness. The TiO₂ thin films had an amorphous structure. Moiré deflectometry was used to measure the nonlinear refractive indices of TiO₂ thin films on PC substrates. The nonlinear refractive index was measured to be of the order of 10^− 8 cm² W^− 1 and a change in refractive index was of the order of 10^− 5. Dense TiO₂ films exhibited high linear refractive indices, red-shift of the optical absorbance, and absorbance in the near-IR region.     

High refractive index and good mechanical property UV-cured hybrid films containing zirconia nanoparticles

UV-curable zirconia (ZrO₂) nanoparticle coatings, prepared by dispersing highly-crystalline zirconia nanoparticles (4 nm) in tetrahydrofuran with the aid of 3-glycidoxypropyltrimethoxysilane (GPTMS) and following addition of a cationic photoinitiator, were cast on silicon wafers (or glass substrates) by dip-coating or spin-coating and photopolymerized to get transparent ZrO₂ nanoparticle films. Ellipsometrical characterization indicates that the refractive index of the film changes from 1.63 to 1.77 at wavelength of 632 nm when the molar ratio of GPTMS-to-ZrO₂ decreases from 0.30 to 0.15. Nano-indentation tests show that the films exhibit robust mechanical performance though they are not heat-treated.     

χ measurements and optical limiting studies of 2-chloro-5-nitro-N′-[(1E)-phenylmethylidene] benzohydrazide with substituents

The nonlinear optical properties of hydrazones substituted with different donor groups were studied using single beam Z-scan technique with nanosecond laser pulses at 532 nm. The nonlinear response in these molecules was found to increase with increase in the donor strength of the substituted group. The χ⁽³⁾ value of these molecules is found to be of the order of 10⁻¹³ esu. The nonlinear refractive index (n₂) of the samples is found to be negative and the largest value of n₂ obtained for the strong donor-substituted molecule is −8.83 × 10⁻¹¹ esu. All samples show good optical limiting behavior at 532 nm. The best optical limiting behavior was observed with the molecule substituted by a strong electron donor.     

Influence of gamma irradiation on the refractive index of Fe-doped barium titanate thin films

Polycrystalline Fe-doped barium titanate (Fe-doped BaTiO₃) thin films were grown by thermal decomposition of the precursors deposited from a sol-gel system onto quartz substrates. The changes in the transmittance spectra induced by gamma irradiation on the Fe-doped BaTiO₃ thin films were quantified. The values for the optical energy band gap were in the range of 3.42-3.95 eV depending on the annealing time. The refractive index of the film, as measured in the 350-750 nm wavelength range was in the 2.17-1.88 range for the as prepared film, and this increased to 2.34-1.95 after gamma irradiation at 15 kGy. The extinction coefficient of the film was in the order of 10⁻² and increased after gamma irradiation. We obtained tuneable complex refractive index of the films by exposure to various gamma rays doses.     

Morphological characterization of TiO2 thin films

Films prepared by reactive magnetron sputtering always present some structural and morphological heterogeneities.In this work, optical parameters, n(λ), k(λ) and E₀, of TiO₂ thin films were obtained, using only optical transmittance measurements. Films were described according to Abèles's model. Using a mono-oscillator type dispersion curve for the refractive index and a Lorentzian type curve for the absorption coefficient, we were able to demonstrate that the films were optically equivalent to a porous layer, with some dispersion in film thickness.The detailed analysis of the experimental transmittance data, fitted between 330 nm to 2200 nm, also enabled us to correlate the effective refractive index of each film with its deposition conditions.     

Tuning Excitonic Properties of Monolayer MoS2 with Microsphere Cavity by High‐Throughput Chemical Vapor Deposition Method

Tuning the optical properties of 2D direct bandgap semiconductors is crucial for applications in photonic light source, optical communication, and sensing. In this work, the excitonic properties of molybdenum disulphide (MoS₂) are successfully tuned by directly depositing it onto silica microsphere resonators using chemical vapor deposition method. Multiple whispering gallery mode (WGM) peaks in the emission wavelength range of ≈650–750 nm are observed under continuous wave excitation at room temperature. Time‐resolved photoluminescence (TRPL) and femtosecond transient absorption (TA) spectroscopy are conducted to study light‐matter interaction dynamics of the MoS₂ microcavities. TRPL study suggests radiative recombination rate of carrier‐phonon scattering and interband transition processes in MoS₂ is enhanced by a factor of ≈1.65 due to Purcell effect in microcavities. TA spectroscopy study shows modulation of the interband transition process mainly occurs at PB‐A band with an estimated F ≈ 1.60. Furthermore, refractive index sensing utilizing WGM peaks of MoS₂ is established with sensitivity up to ≈150 nm per refractive index unit. The present work provides a large‐scale and straightforward method for coupling atomically thin 2D gain media with cavities for high‐performance optoelectronic devices and sensors.