金属合金材料光频介电性质及其表面等离激元性能研究
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摘要
表面等离激元学能够在纳米尺度下控制光的传播，因此近些年被广泛的应用在一大批新型器件中。但是由于表面等离激元学存在的必要条件之一即是需要具有负介电函数的金属单质材料，最常用的材料为银和金，材料种类相对单一，并且由于材料本身的欧姆损耗的存在极大限制了其发展。本论文主要利用反射式椭圆偏振法对金属合金薄膜材料的光频介电性质进行深入的研究，探索材料的介电性能可调行为，寻找更多能用于表面等离激元学的基本材料。论文的主要创新点如下：
提出了一种基于反射式椭圆偏振测量法来测量金属合金薄膜介电性能的测试方法，详细研究了铝银合金薄膜的光频介电函数和能带结构，并提出了合金成分、退火温度以及薄膜厚度等对介电函数的调节作用。随着铝银合金薄膜退火温度增加，薄膜的晶粒尺寸长大并呈现择优取向，而薄膜的介电函数虚部值也会逐渐减弱；铝银合金在1.5eV附近存在一个典型的带间跃迁过程，且该跃迁中心随退火温度升高而红移，而合金薄膜中银成分的增加将使其向高频移动，薄膜介电函数随着厚度增加而逐渐趋于稳定；铝银合金薄膜在可见光频段是一种很好的表面等离激元基本材料。
首次对银铂合金体系的光频介电性能进行测试，并提出了利用退火作用以及合金成分实现对其介电性能的调节。银铂合金薄膜介电函数实部和虚部分别随着波长增加而逐渐减小与增大；通过联合态密度函数谱以及拟合参数知道，银铂合金分别在1.9eV和3.1eV附近有带间跃迁峰存在，位于3.1eV处的跃迁峰随着铂含量的增加将出现红移，且银铂合金的介电函数损耗随着铂合金含量的增加而增加；经过300oC退火后的Ag-25at%Pt合金介电函数值明显小于其他退火温度下的值，因此，适当的退火作用可以极大提高银铂合金的表面等离激元品质因子。
探索了金属银铜以及铜锌合金体系的光频介电性能和内部能带结构，并且提出了薄膜厚度以及退火温度变化等对介电性能的调控作用。银铜合金中存在两个典型跃迁分别位于1.7eV和3.5eV附近，随着合金中铜含量增加，合金晶格常数逐渐减小，并且3.5eV处的峰值出现蓝移，随着退火温度增加薄膜晶粒尺寸增加，表面粗糙度增加；而铜锌合金体系中存在2.0eV和3.2eV附近带间跃迁，并且薄膜厚度的变化对铜锌合金体系介电函数有很大的影响。
Surface plasmon polariton phtonics or “Plasmonics” is considered for a promisingnew device technology that aims to exploit the unique optical properties of metallicnanostructures to enable routing and active manipulation of light at nanoscale. Thematerials with negative permittivity such as metals Ag and Au are the basic conditionfor the existence of plasmoncis. However, the large losses of metals arising from theohmic loss and interband transitions, seriously limit the applicability of plasmonics andmetamaterials. Therefore, more low-loss materials are needed for the development ofplasmonics. In this dissertation, the optical properties of metallic alloy films depositedby direct current magnetron sputtering are studied with variable angle spectroscopicellipsometry (VASE). The dielectric constants and band structure of metallic alloy flimsare analyzed in detail with the change of annealing temperature, composition and filmthickness, respectively. The key findings and conclusions of this dissertation are asfollows:
A new method based on variable angle spectroscopic ellipsometry is used to studythe optical dielectric properties of metallic alloy films. The dielectric properties ofAl-Ag alloy films in optical range were studied with different annealing temperatureand composition. We also investigated the band structure and the microstructure of thealloy films. The results show that the grain size and the imaginary part of the dielectricfunctions for the Al-Ag alloy films are increased and decreased with the increase of theannealing temperature, respectively. A typical interband transition around1.5eV of theAl-Ag alloy films separately shift to the low and high energy part with the increae of theannealing temperature and the silver concentrations in aluminum. The permittivity ofalloy films was slightly changed to the same with increasing the film thickness. TheAl-Ag alloy films are good candidate for plasmonics.
The optical dielectric constants of Ag-Pt alloy films were investigaged byellipsometry for the first time. The experiments show that the real and imaginary part ofdielectric constants are decreased and increased with improving the wavelength,respectively. By ananlyzing the joint density of states (JDOS) and fitting parameters ofthe model, we found that there are two typical interband transitions around1.9eV and3.1eV in the Ag-Pt alloy films. Furthermore, the centre of3.1eV transition shows a red shift and the imaginary part of permittivity is increased byincreasing the platinum addition in silver. The dielectric functions ofAg-25at%Pt alloy films annealed at300oC is clearly less than the one withother annealing temperature. Therefore, the quality factors of Ag-Pt alloy filmscan be greatly improved with the appropriate annealing effect.
The optical dielectric properties and band structures of the silver copperand copper zinc alloy films are tunable with the change of annealingtemperature and film thickness. It has been shown that two typical interbandtransitions around1.7eV and3.5eV are presented in Ag-Cu alloy films. Withincreasing the copper composition in silver, the lattice constants of Ag-Cualloys are decreased and the interband transition at3.5eV shifts to high energy.In addition, the grain size and surface roughness of Ag-Cu alloy films aresimultaneously increased by increasing the annealing temperature. For thecopper zinc alloy films, there are two interband transtions around2.0eV and3.2eV which arising from the top of the d band to the Fermi level in the vicinity ofthe L point in the reciprocal space. The dielectric functions of the Cu-Zn alloyfilms are relative to the film thickness.
提出了一种基于反射式椭圆偏振测量法来测量金属合金薄膜介电性能的测试方法，详细研究了铝银合金薄膜的光频介电函数和能带结构，并提出了合金成分、退火温度以及薄膜厚度等对介电函数的调节作用。随着铝银合金薄膜退火温度增加，薄膜的晶粒尺寸长大并呈现择优取向，而薄膜的介电函数虚部值也会逐渐减弱；铝银合金在1.5eV附近存在一个典型的带间跃迁过程，且该跃迁中心随退火温度升高而红移，而合金薄膜中银成分的增加将使其向高频移动，薄膜介电函数随着厚度增加而逐渐趋于稳定；铝银合金薄膜在可见光频段是一种很好的表面等离激元基本材料。
首次对银铂合金体系的光频介电性能进行测试，并提出了利用退火作用以及合金成分实现对其介电性能的调节。银铂合金薄膜介电函数实部和虚部分别随着波长增加而逐渐减小与增大；通过联合态密度函数谱以及拟合参数知道，银铂合金分别在1.9eV和3.1eV附近有带间跃迁峰存在，位于3.1eV处的跃迁峰随着铂含量的增加将出现红移，且银铂合金的介电函数损耗随着铂合金含量的增加而增加；经过300oC退火后的Ag-25at%Pt合金介电函数值明显小于其他退火温度下的值，因此，适当的退火作用可以极大提高银铂合金的表面等离激元品质因子。
探索了金属银铜以及铜锌合金体系的光频介电性能和内部能带结构，并且提出了薄膜厚度以及退火温度变化等对介电性能的调控作用。银铜合金中存在两个典型跃迁分别位于1.7eV和3.5eV附近，随着合金中铜含量增加，合金晶格常数逐渐减小，并且3.5eV处的峰值出现蓝移，随着退火温度增加薄膜晶粒尺寸增加，表面粗糙度增加；而铜锌合金体系中存在2.0eV和3.2eV附近带间跃迁，并且薄膜厚度的变化对铜锌合金体系介电函数有很大的影响。
Surface plasmon polariton phtonics or “Plasmonics” is considered for a promisingnew device technology that aims to exploit the unique optical properties of metallicnanostructures to enable routing and active manipulation of light at nanoscale. Thematerials with negative permittivity such as metals Ag and Au are the basic conditionfor the existence of plasmoncis. However, the large losses of metals arising from theohmic loss and interband transitions, seriously limit the applicability of plasmonics andmetamaterials. Therefore, more low-loss materials are needed for the development ofplasmonics. In this dissertation, the optical properties of metallic alloy films depositedby direct current magnetron sputtering are studied with variable angle spectroscopicellipsometry (VASE). The dielectric constants and band structure of metallic alloy flimsare analyzed in detail with the change of annealing temperature, composition and filmthickness, respectively. The key findings and conclusions of this dissertation are asfollows:
A new method based on variable angle spectroscopic ellipsometry is used to studythe optical dielectric properties of metallic alloy films. The dielectric properties ofAl-Ag alloy films in optical range were studied with different annealing temperatureand composition. We also investigated the band structure and the microstructure of thealloy films. The results show that the grain size and the imaginary part of the dielectricfunctions for the Al-Ag alloy films are increased and decreased with the increase of theannealing temperature, respectively. A typical interband transition around1.5eV of theAl-Ag alloy films separately shift to the low and high energy part with the increae of theannealing temperature and the silver concentrations in aluminum. The permittivity ofalloy films was slightly changed to the same with increasing the film thickness. TheAl-Ag alloy films are good candidate for plasmonics.
The optical dielectric constants of Ag-Pt alloy films were investigaged byellipsometry for the first time. The experiments show that the real and imaginary part ofdielectric constants are decreased and increased with improving the wavelength,respectively. By ananlyzing the joint density of states (JDOS) and fitting parameters ofthe model, we found that there are two typical interband transitions around1.9eV and3.1eV in the Ag-Pt alloy films. Furthermore, the centre of3.1eV transition shows a red shift and the imaginary part of permittivity is increased byincreasing the platinum addition in silver. The dielectric functions ofAg-25at%Pt alloy films annealed at300oC is clearly less than the one withother annealing temperature. Therefore, the quality factors of Ag-Pt alloy filmscan be greatly improved with the appropriate annealing effect.
The optical dielectric properties and band structures of the silver copperand copper zinc alloy films are tunable with the change of annealingtemperature and film thickness. It has been shown that two typical interbandtransitions around1.7eV and3.5eV are presented in Ag-Cu alloy films. Withincreasing the copper composition in silver, the lattice constants of Ag-Cualloys are decreased and the interband transition at3.5eV shifts to high energy.In addition, the grain size and surface roughness of Ag-Cu alloy films aresimultaneously increased by increasing the annealing temperature. For thecopper zinc alloy films, there are two interband transtions around2.0eV and3.2eV which arising from the top of the d band to the Fermi level in the vicinity ofthe L point in the reciprocal space. The dielectric functions of the Cu-Zn alloyfilms are relative to the film thickness.
引文
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