贵金属纳米颗粒阵列的三阶非线性光学特性研究
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摘要
21世纪以来,随着信息化社会的发展,光纤通讯技术的广泛应用在一定程度上满足了人们对高传输速率、高信噪比的要求。但是,在光纤通讯系统里面常见的光电转换器件会导致响应时间慢、噪声增大等缺陷,直接制约着光通讯技术的发展。因此,人们试图直接用光来对光进行控制和处理,即“以光控光”。目前,主要是通过较强的控制激光激发传输介质中的三阶非线性光学特性,使介质的吸收系数,折射率或偏振等光学参数发生改变,从而实现对信号光的间接控制。其中,较为主流的干涉型全光开光器件是利用控制激光引起其中一束光的传输介质的折射率发生改变,从而改变其中信号光的相位,来实现全光开关的目的。这就要求人们找到一种同时具有高的非线性折射率和较低的非线性吸收系数的非线性光学材料。此外,在器件微型化、集成化的发展趋势下,对各种微纳光源的研究也引起人们广泛的兴趣,其中基于材料非线性特性的光泵浦式纳米激光器需要材料具有很高的非线性光学吸收特性。所以,各种纳米微结构的制备及其三阶非线性光学特性,是目前光学材料领域中的研究热点之一。
研究材料非线性光学特性的一个重要手段就是对光学材料的三阶光学非线性特性进行测试,它不仅可以评估材料非线性光学特性的强弱和种类,还能揭示不同非线性过程的产生机理,从而为找到性能优异、符合新型微纳光器件要求的非线性材料提供重要的实验依据。本文对贵金属纳米颗粒阵列以及和ZnO纳米线中的三阶非线性光学特性进行了系统地研究：
(1)采用脉冲激光沉积技术结合纳米球蚀刻技术,在石英基片上制备了一系列不同尺寸的贵金属(金和银)纳米颗粒阵列,利用扫描电子显微镜观测了纳米球掩膜板和贵金属纳米颗粒阵列的表面形貌。其中,纳米球掩膜板呈大面积、无缺陷的密排；三角形的贵金属纳米颗粒呈周期性排布。另外,采用气相传输法制备了高质量的单晶ZnO纳米线。通过扫描电子显微镜的观测,ZnO纳米线呈高质量的六棱柱结构,并将单根ZnO纳米线转移到空白石英基片上。
(2)通过紫外-可见吸收光谱仪在200nm到900nm波长范围内对贵金属纳米颗粒的线性光吸收特性进行了测量,分别观测到了金、银纳米颗粒的表面等离子体共振吸收峰。研究了尺寸为70 nm的金纳米颗粒阵列在不同的激发光强度下的非线性光学特性：随着激发光强度的增大,其非线性吸收特性由双光子吸收转变为饱和吸收,并且其非线性折射特性由自散焦效应转变为自聚焦效应。
(3)研究了一系列不同尺寸的金纳米颗粒阵列的三阶非线性光学特性,讨化了纳米颗粒的尺寸对其非线性光学特性的影响：随着纳米颗粒尺寸不断变大,其非线性吸收特性由双光子吸收占据主导变为饱和吸收,还观测到双光子吸收和饱和吸收效应竞争的现象。
(4)研究了尺寸为60 nm的银纳米颗粒阵列在四种不同激发光波长(400 nm,600 nm,650 nm和800 nm)激发下的非线性光学特性：随着激发光光强增大,在共振区域(400 nm),其非线性吸收特性由饱和吸收转变为反饱和吸收；非共振区域(800nm),其非线性光学吸收则由双光子吸收转变为饱和吸收；在共振区的边缘(600 nm,650 nml,发现即使在很高的激发光强下,其非线性吸收效应也很不明显。在共振区的非线性光学效应比非共振区的有两个数量级的提高。
(5)研究了单根ZnO纳米线的三阶非线性光学效应对激发光偏振特性的依赖关系：其双光子吸收和非线性折射特性的强度随着入射光偏振角呈周期为π/2的振动。还研究了ZnO纳米线入射面对其非线性光学特性的影响。结果表明,单根ZnO纳米线具有良好的非线性光学各向异性,在具有特定偏振特性的激光激发下,其非线性光学特性会有明显地提高。
In the 21st century, in the development of information society, the widely application of the fibre communication fits the requirement of a high speed transmission and high signal noise ratio. However, the optical-electronic conversation devices in the fibre communication system lead to a slow response time and a high noise, which significantly limits the development of the optical communications. Thus, people try to control and process the optical signal by light directly. Presently, it often uses an intensive laser to induce the third-optical nonlinearities in the medium of the signal, resulting in the changing of the refraction, absorption or the polarization properties of the medium to realize the all-optical switching. Such demands of the all-optical devices have driven people to search for a nonlinear material with a high nonlinear refraction index but a low nonlinear absorption. Furthermore, in the development of micromation and integration of the modern optical devices, kinds of the light resource in the micro-nano meter scales have drawn a lot of attentions. Especially, the optical pumped nanowire laser based on the optical nonlinearity of the materials demands for a high nonlinear absorption coefficient. Therefore, the study of the fabrication and the optical nonlinearity in nanostructures is one of the most interesting areas in studies of optical materials.
The measurement of the third-order optical nonlinearity in optical materials is an important method in the investigation of the optical nonlinearity. It is not only able to estimate the value and style of the nonlinear materials but also indicate the original mechanisms of the nonlinearity. It provides important experimental supports in order to find the nonlinear materials, meeting the requirement of new micro-nano optical devices with a high performance. In this dissertation, systematical investigations on the optical nonlinearity of the noble metals and ZnO in micro-nano scales are presented:
(1) Combined pulsed laser deposition technique with nanosphere lithography method, a serial of noble metals (Au and Ag) nanoparticle arrays with different size have been fabricated on quartz substrates. From scanning electron microscopy images, the well closed-packed nanosphere mask and periodical array of noble metals nanoprisms are observed. Besides, ZnO nanowires are synthesized by a high temperature thermal evaporation process, which has a hexagonal cross section in scanning electron microscopy images. And then, an individual ZnO nanowire is transferred to a quartz substrate for optical measurements.
(2) By measuring UV-visible absorption spectroscopy, the strong absorption band in the visible range caused by surface plasmon resonance of Ag and Au particles can be observed. The intensity-dependent optical nonlinearities in an Au nanoparticle array with a size of 60 nm are investigated. The results exhibit a sign reversal process in the nonlinear absorption and the nonlinear refraction properties as the intensity increases.
(3) The size effects on the optical nonlinearities of the Au nanoparticles are also investigated in a serial of Au nanoparticle arrays with four sizes (37 nm,70 nm,140 nm and 190 nm). It shows a reversal process from the two-photon absorption to the saturated absorption as the size of the nanoparticles increase. The competition of these two different mechanisms is also observed.
(4) The optical nonlinearities of an Ag nanoparticle array are investigated using the selected wavelengths (400 nm,600 nm,650 nm and 800 nm):as the intensities increase, the nonlinear absorption change over from the saturated absorption to the reversed saturated absorption process in the resonant region (400 nm); In the off-resonant region (800 nm), it is observed that optical nonlinearities change over from the two-photon absorption to the saturated absorption as the intensity increases; In the edge of the absorption band (600 nm and 650 nm), low nonlinear absorptions are observed even under high intensities. Furthermore, the nonlinear refraction index in the resonant region exhibits a large enhancement of the 2 orders larger than that in the off-resonant region.
(5) The anisotropy of the third-order optical nonlinearity of an individual ZnO nanowire is studied systematically. The two-photon absorption coefficient and the nonlinear refraction index exhibit oscillations with a period of n/2, the influence of the different incident crystal planes is also presented. The results indicate a highly polarized optical nonlinearity of the ZnO nanowire that a high nonlinear absorption property can be obtained under excitation laser with a proper polarization property.
研究材料非线性光学特性的一个重要手段就是对光学材料的三阶光学非线性特性进行测试,它不仅可以评估材料非线性光学特性的强弱和种类,还能揭示不同非线性过程的产生机理,从而为找到性能优异、符合新型微纳光器件要求的非线性材料提供重要的实验依据。本文对贵金属纳米颗粒阵列以及和ZnO纳米线中的三阶非线性光学特性进行了系统地研究：
(1)采用脉冲激光沉积技术结合纳米球蚀刻技术,在石英基片上制备了一系列不同尺寸的贵金属(金和银)纳米颗粒阵列,利用扫描电子显微镜观测了纳米球掩膜板和贵金属纳米颗粒阵列的表面形貌。其中,纳米球掩膜板呈大面积、无缺陷的密排；三角形的贵金属纳米颗粒呈周期性排布。另外,采用气相传输法制备了高质量的单晶ZnO纳米线。通过扫描电子显微镜的观测,ZnO纳米线呈高质量的六棱柱结构,并将单根ZnO纳米线转移到空白石英基片上。
(2)通过紫外-可见吸收光谱仪在200nm到900nm波长范围内对贵金属纳米颗粒的线性光吸收特性进行了测量,分别观测到了金、银纳米颗粒的表面等离子体共振吸收峰。研究了尺寸为70 nm的金纳米颗粒阵列在不同的激发光强度下的非线性光学特性：随着激发光强度的增大,其非线性吸收特性由双光子吸收转变为饱和吸收,并且其非线性折射特性由自散焦效应转变为自聚焦效应。
(3)研究了一系列不同尺寸的金纳米颗粒阵列的三阶非线性光学特性,讨化了纳米颗粒的尺寸对其非线性光学特性的影响：随着纳米颗粒尺寸不断变大,其非线性吸收特性由双光子吸收占据主导变为饱和吸收,还观测到双光子吸收和饱和吸收效应竞争的现象。
(4)研究了尺寸为60 nm的银纳米颗粒阵列在四种不同激发光波长(400 nm,600 nm,650 nm和800 nm)激发下的非线性光学特性：随着激发光光强增大,在共振区域(400 nm),其非线性吸收特性由饱和吸收转变为反饱和吸收；非共振区域(800nm),其非线性光学吸收则由双光子吸收转变为饱和吸收；在共振区的边缘(600 nm,650 nml,发现即使在很高的激发光强下,其非线性吸收效应也很不明显。在共振区的非线性光学效应比非共振区的有两个数量级的提高。
(5)研究了单根ZnO纳米线的三阶非线性光学效应对激发光偏振特性的依赖关系：其双光子吸收和非线性折射特性的强度随着入射光偏振角呈周期为π/2的振动。还研究了ZnO纳米线入射面对其非线性光学特性的影响。结果表明,单根ZnO纳米线具有良好的非线性光学各向异性,在具有特定偏振特性的激光激发下,其非线性光学特性会有明显地提高。
In the 21st century, in the development of information society, the widely application of the fibre communication fits the requirement of a high speed transmission and high signal noise ratio. However, the optical-electronic conversation devices in the fibre communication system lead to a slow response time and a high noise, which significantly limits the development of the optical communications. Thus, people try to control and process the optical signal by light directly. Presently, it often uses an intensive laser to induce the third-optical nonlinearities in the medium of the signal, resulting in the changing of the refraction, absorption or the polarization properties of the medium to realize the all-optical switching. Such demands of the all-optical devices have driven people to search for a nonlinear material with a high nonlinear refraction index but a low nonlinear absorption. Furthermore, in the development of micromation and integration of the modern optical devices, kinds of the light resource in the micro-nano meter scales have drawn a lot of attentions. Especially, the optical pumped nanowire laser based on the optical nonlinearity of the materials demands for a high nonlinear absorption coefficient. Therefore, the study of the fabrication and the optical nonlinearity in nanostructures is one of the most interesting areas in studies of optical materials.
The measurement of the third-order optical nonlinearity in optical materials is an important method in the investigation of the optical nonlinearity. It is not only able to estimate the value and style of the nonlinear materials but also indicate the original mechanisms of the nonlinearity. It provides important experimental supports in order to find the nonlinear materials, meeting the requirement of new micro-nano optical devices with a high performance. In this dissertation, systematical investigations on the optical nonlinearity of the noble metals and ZnO in micro-nano scales are presented:
(1) Combined pulsed laser deposition technique with nanosphere lithography method, a serial of noble metals (Au and Ag) nanoparticle arrays with different size have been fabricated on quartz substrates. From scanning electron microscopy images, the well closed-packed nanosphere mask and periodical array of noble metals nanoprisms are observed. Besides, ZnO nanowires are synthesized by a high temperature thermal evaporation process, which has a hexagonal cross section in scanning electron microscopy images. And then, an individual ZnO nanowire is transferred to a quartz substrate for optical measurements.
(2) By measuring UV-visible absorption spectroscopy, the strong absorption band in the visible range caused by surface plasmon resonance of Ag and Au particles can be observed. The intensity-dependent optical nonlinearities in an Au nanoparticle array with a size of 60 nm are investigated. The results exhibit a sign reversal process in the nonlinear absorption and the nonlinear refraction properties as the intensity increases.
(3) The size effects on the optical nonlinearities of the Au nanoparticles are also investigated in a serial of Au nanoparticle arrays with four sizes (37 nm,70 nm,140 nm and 190 nm). It shows a reversal process from the two-photon absorption to the saturated absorption as the size of the nanoparticles increase. The competition of these two different mechanisms is also observed.
(4) The optical nonlinearities of an Ag nanoparticle array are investigated using the selected wavelengths (400 nm,600 nm,650 nm and 800 nm):as the intensities increase, the nonlinear absorption change over from the saturated absorption to the reversed saturated absorption process in the resonant region (400 nm); In the off-resonant region (800 nm), it is observed that optical nonlinearities change over from the two-photon absorption to the saturated absorption as the intensity increases; In the edge of the absorption band (600 nm and 650 nm), low nonlinear absorptions are observed even under high intensities. Furthermore, the nonlinear refraction index in the resonant region exhibits a large enhancement of the 2 orders larger than that in the off-resonant region.
(5) The anisotropy of the third-order optical nonlinearity of an individual ZnO nanowire is studied systematically. The two-photon absorption coefficient and the nonlinear refraction index exhibit oscillations with a period of n/2, the influence of the different incident crystal planes is also presented. The results indicate a highly polarized optical nonlinearity of the ZnO nanowire that a high nonlinear absorption property can be obtained under excitation laser with a proper polarization property.
引文
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