激光沉积TiO_2基复合薄膜及其光学特性
摘要
在本论文工作中,我们利用脉冲激光沉积(PLD)技术生长了TiO_2薄膜和掺Au纳米颗粒的TiO_2复合薄膜,并对薄膜的结构和光学性质进行了详细研究,采用飞秒激光和Z扫描方法测量了薄膜的非线性光学性质,所制备的薄膜表现出优良的非线性光学性质。论文的主要内容和结论如下:
(1)系统研究了在PLD制备TiO_2薄膜过程中基片沉积温度、氧气分压、激光能量密度等参数对于TiO_2薄膜结构的影响。利用PLD技术在Si(100)基片和石英玻璃基片上制备了C轴取向的锐钛矿相TiO_2薄膜和(110)择优取向的金红石相薄膜,X射线衍射(XRD)、红外光谱、拉曼光谱结果显示薄膜具有良好的结晶性能。
(2)采用Z扫描技术对制备的锐钛矿相和金红石相TiO_2薄膜的光学非线性进行了研究,测试中采用了放大级飞秒激光和振荡级飞秒激光作为光源。当采用放大级飞秒激光进行测量时,锐钛矿相和金红石相TiO_2薄膜的非线性折射率分别为-6.32×10~(17)m~2/W和-2.7×10~(-17)m~2/W,非线性吸收系数分别为-6.2×10~(-11)m/W和-2.6×10~(-10)m/W;当采用振荡级飞秒激光进行测量时,薄膜表现出负的非线性吸收系数和正的非线性折射率。
(3)采用PLD方法制备了不同掺杂浓度的Au:TiO_2复合薄膜,采用XRD方法分析了薄膜的晶体结构。通过透射光谱分析了复合薄膜的线性光学性质。采用Z扫描方法测量了复合薄膜的非线性光学性质。采用放大级飞秒激光为光源时,薄膜的非线性吸收系数和非线性折射率均为负,随着掺杂浓度的提高,非线性效应增强;采用振荡级飞秒激光为光源时时,薄膜的非线性折射率为正,然而在退火前薄膜随着Au掺杂浓度的增长非线性吸收系数由负变正,退火后薄膜的非线性吸收系数均为负。
(4)采用PLD的方法制备了Au/TiO_2多层薄膜,测量了薄膜的透射光谱,结果表明随着Au掺杂浓度的增加,多层薄膜的吸收峰发生了红移。采用放大级飞秒激光对复合薄膜的非线性光学性质进行了Z扫描测量,结果表明薄膜的非线性吸收系数和非线性折射率均为负。
(5)在石英玻璃基片上制备了掺杂周期阵列排布Au颗粒的TiO_2复合薄膜,研究了Au颗粒大小和TiO_2基质对薄膜的吸收峰的影响,结果表明随着Au颗粒的增长和TiO_2基质的加入,吸收峰发生红移。
In this work,TiO_2 films and nano-composite films containing Au particles embedded in TiO_2 matrices were fabricated using pulsed laser deposition technique(PLD).The structure and nonlinear optical properties of the films were investigated.The nonlinear optical properties were measured by Z-scan method using femtosecond laser.And the films show large optical nonlinear responses.The main results are listed as follows,
(1) The effects of the substrate temperature,oxygen pressure and laser fluences on the crystal structure of TiO_2 films were studied.For the first time,c-axes oriented anatase TiO_2 films and(110) oriented rutile TiO_2 films were fabricated on Si(100),respectively. The results of X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR) and Raman spectra show that the prepared films have good crystal structure.
(2) The nonlinear optical properties of the anatase and rutile TiO_2 films were investigated by z-scan method using amplified femtosecond laser and seed femtosecond laser.When amplified femtosecond laser was used,the nonlinear optical refractive indexes of the anatase films and the rutile film were measured to be 6.32×10~(-17)m~2/W and -2.7×10~(-17)m~2/W,the nonlinear refractive indexis were -6.2×10~(-11)m/W和-2.6×10~(-10)m/W, respectively.When the seed femtosecond laser was used,the nonlinear optical absorption coefficients were negative,but the nonlinear refractive indexes were positive.
(3) Au:TiO_2 composite films were fabricated using PLD method.The crystal structure of the films was determined by XRD.The linear optical properties of the films were analyzed by transmission spectra.The results show that the position of surface plasmon resonance(SPR) peaks of the composite films changes to longer wavelength with the increasing of the annealing temperature and Au concentration.The nonlinear optical properties of the films were investigated by z-scan method using amplified femtosecond laser and seed femtosecond laser.When the amplified femtosecond laser was used,the nonlinear optical absorption coefficients and refractive indexes of the films were negative. The nonlinear optical responses increase with the increasing of the Au concentration. When the seed femtosecond laser was used,the nonlinear refractive indexes were positive, the nonlinear absorption coefficients of the films before annealing treatment change from negative to positive with the increasing of Au concentration.However,after annealing the nonlinear absorption coefficients were negative for all composite films.
(4) Multilayer Au/TiO_2 composite films were fabricated by PLD.The transmission spectra were measured.The results show that the SPR peak position of Au/TiO_2 films change to longer wavelength with the increasing of the Au concentration.The nonlinear optical absorption coefficients and refractive indexes were determined to be negative by z-scan method using amplified femtosecond laser.
(5) Composite films consisting of periodic gold nanoparticle arrays coated with TiO_2 were fabricated using PLD method.The effects of the Au particle size and the TiO_2 matrix on the peak position of the films were investigated.The results show the peak position show red shift with the increasing of the Au particle size.
(1)系统研究了在PLD制备TiO_2薄膜过程中基片沉积温度、氧气分压、激光能量密度等参数对于TiO_2薄膜结构的影响。利用PLD技术在Si(100)基片和石英玻璃基片上制备了C轴取向的锐钛矿相TiO_2薄膜和(110)择优取向的金红石相薄膜,X射线衍射(XRD)、红外光谱、拉曼光谱结果显示薄膜具有良好的结晶性能。
(2)采用Z扫描技术对制备的锐钛矿相和金红石相TiO_2薄膜的光学非线性进行了研究,测试中采用了放大级飞秒激光和振荡级飞秒激光作为光源。当采用放大级飞秒激光进行测量时,锐钛矿相和金红石相TiO_2薄膜的非线性折射率分别为-6.32×10~(17)m~2/W和-2.7×10~(-17)m~2/W,非线性吸收系数分别为-6.2×10~(-11)m/W和-2.6×10~(-10)m/W;当采用振荡级飞秒激光进行测量时,薄膜表现出负的非线性吸收系数和正的非线性折射率。
(3)采用PLD方法制备了不同掺杂浓度的Au:TiO_2复合薄膜,采用XRD方法分析了薄膜的晶体结构。通过透射光谱分析了复合薄膜的线性光学性质。采用Z扫描方法测量了复合薄膜的非线性光学性质。采用放大级飞秒激光为光源时,薄膜的非线性吸收系数和非线性折射率均为负,随着掺杂浓度的提高,非线性效应增强;采用振荡级飞秒激光为光源时时,薄膜的非线性折射率为正,然而在退火前薄膜随着Au掺杂浓度的增长非线性吸收系数由负变正,退火后薄膜的非线性吸收系数均为负。
(4)采用PLD的方法制备了Au/TiO_2多层薄膜,测量了薄膜的透射光谱,结果表明随着Au掺杂浓度的增加,多层薄膜的吸收峰发生了红移。采用放大级飞秒激光对复合薄膜的非线性光学性质进行了Z扫描测量,结果表明薄膜的非线性吸收系数和非线性折射率均为负。
(5)在石英玻璃基片上制备了掺杂周期阵列排布Au颗粒的TiO_2复合薄膜,研究了Au颗粒大小和TiO_2基质对薄膜的吸收峰的影响,结果表明随着Au颗粒的增长和TiO_2基质的加入,吸收峰发生红移。
In this work,TiO_2 films and nano-composite films containing Au particles embedded in TiO_2 matrices were fabricated using pulsed laser deposition technique(PLD).The structure and nonlinear optical properties of the films were investigated.The nonlinear optical properties were measured by Z-scan method using femtosecond laser.And the films show large optical nonlinear responses.The main results are listed as follows,
(1) The effects of the substrate temperature,oxygen pressure and laser fluences on the crystal structure of TiO_2 films were studied.For the first time,c-axes oriented anatase TiO_2 films and(110) oriented rutile TiO_2 films were fabricated on Si(100),respectively. The results of X-ray diffraction(XRD),Fourier transform infrared spectroscopy(FTIR) and Raman spectra show that the prepared films have good crystal structure.
(2) The nonlinear optical properties of the anatase and rutile TiO_2 films were investigated by z-scan method using amplified femtosecond laser and seed femtosecond laser.When amplified femtosecond laser was used,the nonlinear optical refractive indexes of the anatase films and the rutile film were measured to be 6.32×10~(-17)m~2/W and -2.7×10~(-17)m~2/W,the nonlinear refractive indexis were -6.2×10~(-11)m/W和-2.6×10~(-10)m/W, respectively.When the seed femtosecond laser was used,the nonlinear optical absorption coefficients were negative,but the nonlinear refractive indexes were positive.
(3) Au:TiO_2 composite films were fabricated using PLD method.The crystal structure of the films was determined by XRD.The linear optical properties of the films were analyzed by transmission spectra.The results show that the position of surface plasmon resonance(SPR) peaks of the composite films changes to longer wavelength with the increasing of the annealing temperature and Au concentration.The nonlinear optical properties of the films were investigated by z-scan method using amplified femtosecond laser and seed femtosecond laser.When the amplified femtosecond laser was used,the nonlinear optical absorption coefficients and refractive indexes of the films were negative. The nonlinear optical responses increase with the increasing of the Au concentration. When the seed femtosecond laser was used,the nonlinear refractive indexes were positive, the nonlinear absorption coefficients of the films before annealing treatment change from negative to positive with the increasing of Au concentration.However,after annealing the nonlinear absorption coefficients were negative for all composite films.
(4) Multilayer Au/TiO_2 composite films were fabricated by PLD.The transmission spectra were measured.The results show that the SPR peak position of Au/TiO_2 films change to longer wavelength with the increasing of the Au concentration.The nonlinear optical absorption coefficients and refractive indexes were determined to be negative by z-scan method using amplified femtosecond laser.
(5) Composite films consisting of periodic gold nanoparticle arrays coated with TiO_2 were fabricated using PLD method.The effects of the Au particle size and the TiO_2 matrix on the peak position of the films were investigated.The results show the peak position show red shift with the increasing of the Au particle size.
引文
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