几种金属氧化物材料的非线性光学性能研究
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摘要
因为具有良好的光学、电学以及磁学性能，金属氧化物材料得到了广泛的关注。金属氧化物物理性能的多样性使得它们具有广阔的器件应用前景。但金属氧化物具有复杂的结构,比金属或者半导体更难制备。氧化物中的杂质和缺陷严重影响了材料本身的性质。本论文针对几种典型金属的氧化物以生长技术和缺陷调控入手，提高材料的品质，优化其物理性能。
第一章，我们简介了几种典型氧化物材料的基本性质，并且对论文中应用的材料制备方法进行了简要的介绍。
第二章，我们制备了掺锆铌酸锂晶体，该晶体在可见光波段具有良好的抗光损伤性能。我们通过对其紫外波段的抗光损伤性能研究发现，当Zr掺入晶体以后，紫外光折变得到了很好的抑制。掺杂锆2mol%的铌酸锂晶体的衍射效率仅为0.1%，相应光致折射率变化比名义纯晶体低一个量级，抗紫外光损伤的光强阈值可以达到10~5W/cm~2。该晶体是目前仅有的具有抗紫外光损伤性能的铌酸锂晶体。通过对擦除曲线进行拟合分析，我们发现存在两个紫外光折变中心，根据实验结果我们提出了紫外光照射下载流子输运的模型，合理解释了掺杂铌酸锂晶体的紫外光折变性能。
第三章，我们通过缺陷能级设计，生长了LiNbO_3:Zr,Fe,Mn和LiNbO_3:Zr,Cu,Ce晶体，对它们的非挥发性全息存储性能进行了研究。掺入锆元素之后，LiNbO_3:Zr,Fe,Mn晶体的响应时间得到了极大的缩短，降到了1秒以下，光折变灵敏度为1.31cm/J，比双掺LiNbO_3:Fe,Mn晶体提高了十几倍，LiNbO_3:Zr,Cu,Ce晶体的光折变灵敏度也得到了提高，达到0.099cm/J，与近化比的LiNbO_3:Cu,Ce晶体的灵敏度相当。而后分别对两种三掺晶体的光致散射进行了研究。我们的实验结果结果表明三掺晶体是实现非挥发性全息存储实际应用的优良材料。
第四章，我们利用脉冲激光沉积法生长了CuScO_2薄膜，其禁带宽度为4.35eV，激子结合能达到了0.4eV。通过利用泵浦探测技术研究发现，其透射率变化ΔT/T非常小，时间演变曲线包括一个延迟的增长以及指数弛豫部分，激子的热化以及复合时间分别为10ps以及0.75ns。我们利用修正的多体Elliott模型对这些结果进行了合理的解释。
第五章，我们利用脉冲激光沉积法在YAlO_3衬底上生长了EuO的薄膜，对其光学以及磁学性能进行了研究。发现飞秒脉冲激发之后，薄膜内的磁化先增强，接着出现退磁化现象。通过对不同温度下的磁动力学进行研究，我们认为光激发导致的Eu原子内f-d电子交换相互作用的增强，使得薄膜的磁化增加，而光激发造成的温度增加又使得EuO出现退磁化，两种作用相互竞争。而后我们在EuO薄膜中观察到磁进动现象以及反法拉第效应，实现了薄膜磁性的超快调控。
第六章，我们对整篇论文进行了总结，并展望了上述金属氧化物材料的研究和应用前景。
Metal oxide materials have received a lot of attention because of their uniqueoptical, electric, and magnetic properties. It is very promsing for using oxidematerials in device applications in the future. But oxides often have complex crystalstructures, they are more difficult to fabricate than metals and semiconductors. Theimpurities and defects inside the materials obstruct wide-spread applications of metaloxide. In this thesis we optimized the growth conditions and defects of several metaloxides, improved the material quality and modified the physical properties.
In Chapter1, we briefly introduced several metal oxides and the growthprocesses adopted in this thesis.
In Chapter2, LiNbO_3:Zr crystals were grown and investigated. LiNbO_3:Zr wasknown to be one of the best photo damage resistant crystals in the visible region. Bystudying the ultraviolet (UV) photorefractive properties, we found that the ultravioletphotorefraction was restricted effectively. The diffraction efficiency of2mol%Zrdoped lithium niobate was only0.1%. The corresponding refractive index changewas one order of magnetitude smaller that that of normally pure lithium niobate, theintensity threshold of resistance to UV optical damage was10~5W/cm~2. Zr dopedcrystals was the first reported UV photo damage resistant crystal. Through analyzingthe erasing curve, we found that there were two kinds of UV photorefractive centers,one model of light induced charge transport was proposed under ultraviolet lightillumination.
In Chapter3, we designed and grew triply doped LiNbO_3:Zr,Fe,Mn andLiNbO_3:Zr,Cu,Ce crystals, and investigated the nonvolatile holographic storageproperties. By doping Zr elements into doubly doped lithium niobate crystals, theresponse time of LiNbO_3:Zr,Fe,Mn was shortened very much, being less than onesecond; The sensitivity was1.31cm/J，which was tens of times larger than that ofLiNbO_3:Fe,Mn. The sensitivity of LiNbO_3:Zr,Cu,Ce crystal was also improved toabout0.099cm/J, equivalent to that of near stiochrometric LiNbO_3:Cu,Ce crystal.The ligh induced scattering were also studied for these two kinds of triply doped crystals, our experimental results indicated that triply doped lithium niobate crystalswere the promising candidate for nonvolatile holographic data storage.
In Chapter4, we grew CuScO_2thin films using plused laser deposition (PLD)method. CuScO_2is an excellent wide band gap semiconductor, the band gap ofwhich is4.35eV，the binding energy of exciton is about0.4eV. The transmissionchange was investigated under exciaton of4.6eV photons, the time race included adelayed raise-up and exponential decay component, the thermalization andrecombination time were10ps and0.75ns, respectively. These features could bedescribed within the framework of generalized many-body Elliott model.
In chapter5, The EuO thin films were grown on YAlO_3substrate by PLDmethod. The optical and magnetic properties were investigated. We found that afterfemtosecond laser pulse exciation, the magnetization was first enhanced and thenbecame demagnetized. Throug studying the magnetization dyanmcis under differenttemperatures, we thought that the magnetization enhancement was due to f-dexchange interaction via free electrons generated by optical pulses, thedemagnetization was related to the thermal effect of laser exciation, these two effectswere competing with each other. We also found precession dynamics and inverseFaraday effect in EuO, achieving non-thermal control of magnetization.
In Chapter6, we summarized the work of this thesis, and prospected the futurefor the research and device applicaton of metal oxide.
第一章，我们简介了几种典型氧化物材料的基本性质，并且对论文中应用的材料制备方法进行了简要的介绍。
第二章，我们制备了掺锆铌酸锂晶体，该晶体在可见光波段具有良好的抗光损伤性能。我们通过对其紫外波段的抗光损伤性能研究发现，当Zr掺入晶体以后，紫外光折变得到了很好的抑制。掺杂锆2mol%的铌酸锂晶体的衍射效率仅为0.1%，相应光致折射率变化比名义纯晶体低一个量级，抗紫外光损伤的光强阈值可以达到10~5W/cm~2。该晶体是目前仅有的具有抗紫外光损伤性能的铌酸锂晶体。通过对擦除曲线进行拟合分析，我们发现存在两个紫外光折变中心，根据实验结果我们提出了紫外光照射下载流子输运的模型，合理解释了掺杂铌酸锂晶体的紫外光折变性能。
第三章，我们通过缺陷能级设计，生长了LiNbO_3:Zr,Fe,Mn和LiNbO_3:Zr,Cu,Ce晶体，对它们的非挥发性全息存储性能进行了研究。掺入锆元素之后，LiNbO_3:Zr,Fe,Mn晶体的响应时间得到了极大的缩短，降到了1秒以下，光折变灵敏度为1.31cm/J，比双掺LiNbO_3:Fe,Mn晶体提高了十几倍，LiNbO_3:Zr,Cu,Ce晶体的光折变灵敏度也得到了提高，达到0.099cm/J，与近化比的LiNbO_3:Cu,Ce晶体的灵敏度相当。而后分别对两种三掺晶体的光致散射进行了研究。我们的实验结果结果表明三掺晶体是实现非挥发性全息存储实际应用的优良材料。
第四章，我们利用脉冲激光沉积法生长了CuScO_2薄膜，其禁带宽度为4.35eV，激子结合能达到了0.4eV。通过利用泵浦探测技术研究发现，其透射率变化ΔT/T非常小，时间演变曲线包括一个延迟的增长以及指数弛豫部分，激子的热化以及复合时间分别为10ps以及0.75ns。我们利用修正的多体Elliott模型对这些结果进行了合理的解释。
第五章，我们利用脉冲激光沉积法在YAlO_3衬底上生长了EuO的薄膜，对其光学以及磁学性能进行了研究。发现飞秒脉冲激发之后，薄膜内的磁化先增强，接着出现退磁化现象。通过对不同温度下的磁动力学进行研究，我们认为光激发导致的Eu原子内f-d电子交换相互作用的增强，使得薄膜的磁化增加，而光激发造成的温度增加又使得EuO出现退磁化，两种作用相互竞争。而后我们在EuO薄膜中观察到磁进动现象以及反法拉第效应，实现了薄膜磁性的超快调控。
第六章，我们对整篇论文进行了总结，并展望了上述金属氧化物材料的研究和应用前景。
Metal oxide materials have received a lot of attention because of their uniqueoptical, electric, and magnetic properties. It is very promsing for using oxidematerials in device applications in the future. But oxides often have complex crystalstructures, they are more difficult to fabricate than metals and semiconductors. Theimpurities and defects inside the materials obstruct wide-spread applications of metaloxide. In this thesis we optimized the growth conditions and defects of several metaloxides, improved the material quality and modified the physical properties.
In Chapter1, we briefly introduced several metal oxides and the growthprocesses adopted in this thesis.
In Chapter2, LiNbO_3:Zr crystals were grown and investigated. LiNbO_3:Zr wasknown to be one of the best photo damage resistant crystals in the visible region. Bystudying the ultraviolet (UV) photorefractive properties, we found that the ultravioletphotorefraction was restricted effectively. The diffraction efficiency of2mol%Zrdoped lithium niobate was only0.1%. The corresponding refractive index changewas one order of magnetitude smaller that that of normally pure lithium niobate, theintensity threshold of resistance to UV optical damage was10~5W/cm~2. Zr dopedcrystals was the first reported UV photo damage resistant crystal. Through analyzingthe erasing curve, we found that there were two kinds of UV photorefractive centers,one model of light induced charge transport was proposed under ultraviolet lightillumination.
In Chapter3, we designed and grew triply doped LiNbO_3:Zr,Fe,Mn andLiNbO_3:Zr,Cu,Ce crystals, and investigated the nonvolatile holographic storageproperties. By doping Zr elements into doubly doped lithium niobate crystals, theresponse time of LiNbO_3:Zr,Fe,Mn was shortened very much, being less than onesecond; The sensitivity was1.31cm/J，which was tens of times larger than that ofLiNbO_3:Fe,Mn. The sensitivity of LiNbO_3:Zr,Cu,Ce crystal was also improved toabout0.099cm/J, equivalent to that of near stiochrometric LiNbO_3:Cu,Ce crystal.The ligh induced scattering were also studied for these two kinds of triply doped crystals, our experimental results indicated that triply doped lithium niobate crystalswere the promising candidate for nonvolatile holographic data storage.
In Chapter4, we grew CuScO_2thin films using plused laser deposition (PLD)method. CuScO_2is an excellent wide band gap semiconductor, the band gap ofwhich is4.35eV，the binding energy of exciton is about0.4eV. The transmissionchange was investigated under exciaton of4.6eV photons, the time race included adelayed raise-up and exponential decay component, the thermalization andrecombination time were10ps and0.75ns, respectively. These features could bedescribed within the framework of generalized many-body Elliott model.
In chapter5, The EuO thin films were grown on YAlO_3substrate by PLDmethod. The optical and magnetic properties were investigated. We found that afterfemtosecond laser pulse exciation, the magnetization was first enhanced and thenbecame demagnetized. Throug studying the magnetization dyanmcis under differenttemperatures, we thought that the magnetization enhancement was due to f-dexchange interaction via free electrons generated by optical pulses, thedemagnetization was related to the thermal effect of laser exciation, these two effectswere competing with each other. We also found precession dynamics and inverseFaraday effect in EuO, achieving non-thermal control of magnetization.
In Chapter6, we summarized the work of this thesis, and prospected the futurefor the research and device applicaton of metal oxide.
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