Preparation of sol-gel ZrO2-SiO2 highly reflective multilayer films and laser-induced damage threshold characteristic

Sol-gel (ZrO₂/SiO₂)¹² ZrO₂ films were prepared by spin coating method. The reflectivity spectrum of the films was measured with a Lambda 900 spectrometer. In order to investigate laser-induced damage threshold (LIDT) characteristic of highly reflective films, one-layer ZrO₂ and SiO₂ films, two-layer ZrO₂/SiO₂ and SiO₂/ZrO₂ films were also prepared by spin coating method. LIDT of each film was measured. Damage morphology after laser irradiation was characterized by optical microscopy (Nikon E600K). The experimental results showed that the reflectivity of (ZrO₂/SiO₂)¹² ZrO₂ film at 1064 nm and 355 nm wavelength is 99.7%. The LIDT results decreases as the number of layer of films increases. All the films have similar damage morphology. The experimental results are explained by the different temperature profiles of the films.     

Investigation of annealing effects on the laser-induced damage threshold of amorphous Ta2O5 films

Ta₂O₅ films were deposited using the conventional electron beam evaporation method and then annealed at temperatures in the range 373-673 K. Chemical composition, scattering and absorption were examined by X-ray photoelectron spectroscopy (XPS), total integrated scattering (TIS) measurement and the surface thermal lensing (STL) technique, respectively. The laser-induced damage threshold (LIDT) was assessed using the output from an Nd:YAG laser with a pulse length of 12 ns. The results showed that the improvement of the LIDT after annealing was due to the reduced substoichiometric and structural defects present in the film. The LIDT increased slightly below 573 K and then increased significantly with increase in annealing temperature, which could be attributed to different dominant defects. Moreover, the root mean square (RMS) roughness and scattering had little effect on the LIDT, while the absorption and the LIDT were in accord with a general relation.     

Calculation of temperature fields with a film-substrate interfacial layer model to discuss the layer-pair number effects on the damage thresholds of LaF3/MgF2 high reflectors at 355 nm

Laser induced damage thresholds (LIDT) of LaF₃/MgF₂ high reflectors at 355 nm were measured and investigated as a function of layer-pair number. Generally, LaF₃/MgF₂ coatings with more layer pairs possessed higher LIDT, but coatings with too high layer-pair number crazed because of high tensile stress, so the LIDT of them decreased badly. The temperature rise in the coatings was calculated based on a film-substrate interfacial absorption model, and the depth of the damage in the coatings were measured by a Veeco optical profilograph. The two characterization methods together were used to interpret the effects of layer-pair number on LIDT, and the damage mechanism of coatings at laser wavelength of 355 nm was also discussed.     

Influence of negative ion element impurities on laser induced damage threshold of HfO2 thin film

Negative ion element impurities breakdown model in HfO₂ thin film was reported in this paper. The content of negative ion elements were detected by glow discharge mass spectrum analysis (GDMS); HfO₂ thin films were deposited by the electron-beam evaporation method. The weak absorption and laser induced damage threshold (LIDT) of HfO₂ thin films were measured to testify the negative ion element impurity breakdown model. It was found that the LIDT would decrease and the absorption would increase with increasing the content of negative ion element. These results indicated that negative ion elements were harmful impurities and would speed up the damage of thin film.     

Y2O3 stabilized ZrO2 thin films deposited by electron beam evaporation: Structural, morphological characterization and laser induced damage threshold

Four kinds of Y₂O₃ stabilized ZrO₂ (YSZ) thin films with different Y₂O₃ content have been prepared on BK7 substrates by electron-beam evaporation method. Structural properties and surface morphology of thin films were investigated by X-ray diffraction (XRD) spectra and scanning probe microscope. Laser induced damage threshold (LIDT) was determined. It was found that crystalline phase and microstructure of YSZ thin films was dependent on Y₂O₃ molar content. YSZ thin films changed from monoclinic phase to high temperature phase (tetragonal and cubic) with the increase of Y₂O₃ content. The LIDT of stabilized thin film is more than that of unstabilized thin films. The reason is that ZrO₂ material undergoes phase transition during the course of e-beam evaporation resulting in more numbers of defects compared to that of YSZ thin films. These defects act as absorptive center and the original breakdown points.     

Influence of SiO2 additional layers on the laser induced damage threshold of Ta2O5 films

A series of Ta₂O₅ films with different SiO₂ additional layers including overcoat, undercoat and interlayer was prepared by electron beam evaporation under the same deposition process. Absorption of samples was measured using the surface thermal lensing (STL) technique. The electric field distributions of the samples were theoretical predicted using thin film design software (TFCalc). The laser induced damage threshold (LIDT) was assessed using an Nd:YAG laser operating at 1064 nm with a pulse length of 12 ns. It was found that SiO₂ additional layers resulted in a slight increase of the absorption, whereas they exerted little influence on the microdefects. The electric field distribution among the samples was unchanged by adding an SiO₂ overcoat and undercoat, yet was changed by adding an interlayer. SiO₂ undercoat. The interlayer improved the LIDT greatly, whereas the SiO₂ overcoat had little effect on the LIDT.     

Effects of deposition parameters on laser-induced damage threshold of Ta2O5 films

Ta₂O₅ films were deposited on BK7 substrates by e-beam evaporation with different deposition parameters such as substrate temperature (323-623 K), oxygen pressure (0.5-3.0×10⁻² Pa) and deposition rate (0.2-0.5 nm/s). Absorption, scattering and chemical composition were investigated by surface thermal lensing (STL) technique, total integrated scattering (TIS) measurement and X-ray photoelectron spectroscopy (XPS), respectively. The laser-induced damage threshold (LIDT) was assessed using pulsed Nd:YAG 1064 nm laser at a pulse length of 12 ns. The results showed that optical properties, absorption and LIDT were influenced by the deposition parameters and annealing. However, scattering was little correlated with the deposition parameters. On the whole, the LIDT increased with increasing substrate temperature and oxygen pressure, whereas it increased firstly and then decreased upon increasing deposition rate. After annealing at 673 K for 12 h, the LIDT of films improved significantly. The dependence of possible damage mechanism on deposition parameters was discussed.     

Influence of substoichiometer on the laser-induced damage characters of HfO2 thin films

HfO₂ is one of the most important high refractive index materials for depositing high power optical mirrors. In this research, HfO₂ thin films were prepared by dual-ion beam reactive sputtering method, and the laser-induced damage thresholds (LIDT) of the sample were measured in 1-on-1 mode for laser with 1064 nm wavelength. The results indicate that the LIDT of the as-grown sample is only 3.96 J/cm², but it is increased to 8.98 J/cm² after annealing under temperature of 200 °C in atmosphere. By measuring the laser weak absorption and SIMS of the samples, we deduced that substoichiometer is the main reason for the low LIDT of the as-grown sample, and the experiment results were well explained with the theory of electronic-avalanche ionization.     

Influences of oxygen partial pressure on structure and related properties of ZrO2 thin films prepared by electron beam evaporation deposition

ZrO₂ thin films were prepared by electron beam evaporation at different oxygen partial pressures. The influences of oxygen partial pressure on structure and related properties of ZrO₂ thin films were studied. Transmittance, thermal absorption, structure and residual stress of ZrO₂ thin films were measured by spectrophotometer, surface thermal lensing technique (STL), X-ray diffraction and optical interferometer, respectively. The results showed that the structure and related properties varied progressively with the increase of oxygen partial pressure. The refractive indices and the packing densities of the thin films decreased when the oxygen partial pressure increased. The tetragonal phase fraction in the thin films decreased gradually as oxygen partial pressure increased. The residual stress of film deposited at base pressure was high compressive stress, the value decreased with the increase of oxygen partial pressure, and the residual stress became tensile with the further increase of oxygen pressure, which was corresponding to the evolution of packing densities and variation of interplanar distances.     

Modification of laser induced damage threshold of ZrO2 thin films by using time-temperature gradient annealing

As a result of using time-temperature gradient annealing, the structural and optical properties and hence, thermal properties of ZrO₂ thin films deposited by electron gun, enhanced considerably compared with rapid thermal annealing. Also, it can be seen time- temperature gradient annealing caused to decrease the total stress and number of thermal barrier along the film. Therefore, according to our experimental results, which is agree with theoretical analysis, the laser induced damage threshold of ZrO₂ films can be enhanced significantly compared with rapid annealing procedure.     

溶胶-凝胶ZrO2-TiO2高折射率光学膜层的抗激光损伤性能研究

采用溶胶-凝胶方法制备了ZrO₂-TiO₂(Ti含量为0—100mol%)高折射率光学薄膜. 借助激光动态光散射技术研究溶胶微结构. 采用傅里叶变换红外光谱、原子力显微镜、薄膜光学常数分析仪、漫反射吸收光谱及强激光辐照实验，对膜层的结构、光学性能及抗激光损伤性能进行了系统表征. 结果显示，溶胶-凝胶工艺可以在部分牺牲折射率的情况下，使膜层的抗激光损伤性能得到大幅度提升. 随Ti含量从0mol%增加至100mol%，膜层的平均损伤阈值呈下降趋势，当Ti含量从0mol%增加至60mol%时，平均损伤阈值从57.1J/cm²下降到21.1J/cm²(辐照激光波长为1053nm，脉冲宽度为10ns，“R/1”测试模式)，当Ti含量从60mol%增加至100mol%时，平均损伤阈值变化很小. 综合溶胶微结构、膜层光学性能和损伤实验结果可以推断，强激光诱导多光子吸收是引起膜层损伤的主要原因. 不同配比的复合膜之间光学带隙的显著差异导致相同辐照激光情况下多光子吸收的概率发生变化，从而导致损伤阈值的规律性变化. 关键词： 2-TiO₂薄膜')" href="#">ZrO₂-TiO₂薄膜 溶胶-凝胶 激光诱导损伤 光学带隙     

Influence of Annealing Temperature on Structure, Optical Loss and Laser-Induced Damage Threshold of TiO2 Thin Films

TiO2 thin films are prepared on fused silica with conventional electron beam evaporation deposition. After annealed at different temperatures for 4h, the spectra and XRD patterns of the TiO2 thin film are obtained. Weak absorption of coatings is measured by the surface thermal lensing technique, and laser-induced damage threshold （LIDT） is determined. It is found that with the increasing annealing temperature, the transmittance of TiO2 films decreases. Especially when coatings are annealed at high temperature over 1173K, the optical loss is very serious. Weak absorption detection indicates that the absorption of coatings decreases firstly and then increases, and the absorption and defects play major roles in the LIDT of TiO2 thin films.     

Effects of annealing on laser-induced damage threshold of TiO2/SiO2 high reflectors

The mechanism of improving 1064 nm, 12 ns laser-induced damage threshold (LIDT) of TiO₂/SiO₂ high reflectors (HR) prepared by electronic beam evaporation from 5.1 to 13.1 J/cm² by thermal annealing is discussed. Through optical properties, structure and chemical composition analysis, it is found that the reduced atomic non-stoichiometric defects are the main reason of absorption decrease and LIDT rise after annealing. A remarkable increase of LIDT is found at 300 °C annealing. The refractive index and film inhomogeneity rise, physical thickness decrease, and film stress changes from compress stress to tensile stress due to the structure change during annealing.     

Influence of substrate temperature on properties of MgF2 coatings

Thermal boat evaporation was employed to prepare MgF₂ single-layer coatings upon both JGS1 and UBK7 substrates at different substrate temperatures. Microstructure, transmittance and residual stress of these coatings were measured by X-ray diffraction, spectrophotometer, and optical interferometer, respectively. Measurement of laser induced damage threshold (LIDT) of the samples was performed at 355 nm, 8 ns pulses. The results showed that high substrate temperature was beneficial to crystallization of the film. Above 244 °C, the refractive index increased gradually with the substrate temperature rising. Whereas, it was exceptional at 210 °C that the refractive index was higher than those deposited at 244 and 277 °C. The tensile residual stresses were exhibited in all MgF₂ films, but not well correlated with the substrate temperature. In addition, the stresses were comparatively smaller upon JGS1 substrates. A tendency could be seen that the LIDTs reached the highest values at about 244 °C, and the films upon JGS1 had higher LIDTs than those upon UBK7 substrates at the same temperature. Meanwhile, the damage morphologies showed that the laser damage of the coating resulted from an absorbing center at the film-substrate interface. The features of the damages were displayed by an absorbing center dominated model. Furthermore, the reason of the difference in LIDT values was discussed in detail.     

Influence of overcoat on laser-induced damage threshold of 532 and 800 nm TiO2/SiO2 high reflectors

TiO₂/SiO₂ high reflectors with and without a SiO₂ overcoat are deposited by electron-beam evaporation. The film properties are characterized by visible spectrometry measures, structure analysis, roughness and laser-induced damage threshold (LIDT) tests, surface defects and damage morphology observation. The effects of overcoats on LIDT at 532 nm, 8 ns and 800 nm, 220 ps laser pulses are investigated. The relations between film structure, roughness, surface defects, electric field and LIDT are discussed. It is found that overcoats can increase the LIDT at these two laser wavelengths. The reduction of peak temperature, the low defects density and roughness, the low intrinsic absorption of SiO₂ and its amorphous structure are the main reasons for LIDT improvement by overcoats.     

PVP掺杂-ZrO2溶胶-凝胶工艺制备多层激光高反射膜的研究

以丙醇锆(ZrPr)为锆源，二乙醇胺(DEA)为络合剂，原位引入聚乙烯吡咯烷酮(PVP)，在乙醇体系中成功地合成了PVP掺杂-ZrO₂溶胶.采用旋涂法在K9玻璃基片上制备了PVP-ZrO₂单层杂化薄膜.用不同掺杂量的PVP-ZrO₂高折射率膜层与相同的SiO₂低折射率膜层交替沉积四分之一波堆高反射膜.借助小角X射线散射研究胶体微结构，用红外光谱、原子力显微镜、紫外/可见/近红外透射光谱、椭圆偏振仪以及1064nm的强激光辐照实验对薄膜的结构、光学和抗激光损伤性能进行表征.研究发现，体系组成的适当配置可以在溶胶稳定的前提下实现ZrPr的充分水解，赋予薄膜良好的结构、光学和抗激光损伤性能.杂化体系中，DEA与ZPr之间强的配合作用大大降低了ZrO₂颗粒表面羟基的活性，使得PVP大分子只是以微弱的氢键与颗粒的表面羟基作用而均匀分散于ZrO₂颗粒的周围，对颗粒的形成和生长无显著影响.因而在实验研究范围内，随PVP含量的增大，PVP-ZrO₂杂化膜层的折射率和激光损伤阈值均无显著变化.但是，薄膜中均匀分布的PVP柔性链可以有效促进膜层应力松弛，显著削弱不同膜层之间的应力不匹配程度、大大方便多层光学薄膜的制备.当高折射率膜层中PVP的质量分数达到15%—20%时，膜层之间良好的应力匹配使得多层高反射膜的沉积周期数可达到10以上.沉积10个周期的多层反射膜，在中心波长1064nm处透射率约为1.6%—2.1%，接近全反射特征，其激光损伤阈值为16.4—18.2J/cm²(脉冲宽度为1ns). 关键词： 溶胶-凝胶 2')" href="#">PVP-ZrO₂ 高反射膜 激光损伤     

Comparison of laser-induced damage in Ta2O5 and Nb2O5 single-layer films and high reflectors

Ta2O5 and Nb2O5 films are deposited on BK7 glass substrates using an electron beam evaporation method and are annealed at 673 K in the air.In this letter,comparative studies of the optical transmittance,microstructure,chemical composition,optical absorption,and laser-induced damage threshold(LIDT) of the two films are conducted.Findings indicate that the substoichiometric defect is very harmful to the laser damage resistance of Ta2O5 and Nb2O5 films.The decrease of absorption improves the LIDT in films deposited by the same material.However,although the absorption of the Ta2O5 single layer is less than that of the Nb2O5 single layer,the LIDT of the former is lower than that of the latter.High-reflective(HR) coatings have a higher LIDT than single layers due to the thermal dissipation of the SiO2 layers and the decreased electric field intensity(EFI).In addition,the Nb2O5 HR coating achieves the highest LIDT at 25.6 J/cm 2 in both single layers and HR coatings.     

Comparison of TiO2 and ZrO2 Films Deposited by Electron-Beam Evaporation and by Sol-Gel Process

TiO2 and ZrO2 films are deposited by electron-beam （EB） evaporation and by sol-gel process. The film properties are characterized by visible and Fourier-transform infrared spectrometry, x-ray diffraction analysis, surface roughness measure, absorption and laser-induced damage threshold （LIDT） test. It is found that the sol-gel films have lower refractive index, packing density and roughness than EB deposited films due to their amorphous structure and high OH group concentration in the film. The high LIDT of sol-gel films is mainly due to their amorphous and porous structure, and low absorption. LIDT of EB deposited film is considerably affected by defects in the film, and LIDT of sol-gel deposited film is mainly effected by residual organic impurities and solvent trapped in the film.     

多孔TiO2/Al/SiO2纳米复合结构的紫外光吸收特性研究

在SiO₂玻璃衬底上用脉冲激光沉积(PLD)技术，分别沉积Ti和Ti/Al膜，经电化学阳极氧化成功制备了多孔TiO₂/SiO₂和TiO₂/Al/SiO₂纳米复合结构. 其中TiO₂薄膜上的微孔阵列高度有序，分布均匀. 实验研究了Al过渡层对多孔TiO₂薄膜光吸收特性的影响. 结果表明：无Al过渡层的多孔TiO₂薄膜其紫外吸收峰在27     

Effect of Process Parameters on Laser Damage Threshold of TiO2 Coatings

We investigate the laser damage behaviour of an electron-beam-deposited TiO2 monolayer at different process parameters. The optical properties, chemical composition, surface defects, absorption and laser-induced damage threshold （LIDT） of films are measured. It is found that TiO2 films with the minimum absorption and the highest LIDT can be fabricated using a TiO2 starting material after annealing. LIDT is mainly related to absorption and is influenced by the non-stoichiometric defects for TiO2 films. Surface defects show no evident effects on LIDT in this experiment.