亚波长金属周期结构的负折射和局域场增强效应的研究
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摘要
对光与物质之间相互作用的理解以及对光及电磁波的操控,一直是人们梦寐追逐的目标,也是科技领域中至关重要的课题。随着工艺技术的长足进步,人们可以制造微米,甚至纳米级的具有任意形状或图案的金属周期结构。当电磁波与这些具有亚波长尺寸的金属周期结构发生作用时,出现一系列新现象和新效应,例如metamaterials(即电磁超介质)和表面等离子体。“电磁超介质”是通过周期排列某种几何结构单元获得的具有自然媒质所不具备的新型电磁特性的一种人工材料。电磁波能够在有效介电常数和有效磁导率同时为负值的电磁超介质中表现出后向波传输、负折射、倏逝波放大等奇异特性。电磁超介质的电磁性能高度依赖单元的几何结构,这为人们获得具有超常电磁性能的“新媒质”提供了一种全新的材料设计理念,为人们操纵、控制光及电磁波提供了新的途径。
电磁超介质通常基于金属的结构单元,采用金属便于实现形状或图案各异的周期结构,但金属的损耗问题是限制金属电磁超介质负折射性能及其应用的关键。结构简单,易于制备,且性能(低损耗、宽频带、固态的、均匀各向同性)良好的电磁超介质是科研工作者追求的目标。本论文设计并研究了几种工作在微波、太赫兹和红外波段的电磁超介质,探索可以实现“负折射”,且能有效降低损耗的结构和机制。同时,针对制约表面增强光谱技术实际广泛应用的瓶颈,即传统衬底结构可控性差导致的表面增强光谱重现性差的问题,对具有可控、稳定、高效的电磁场增强效果的电磁超介质结构在表面增强光谱衬底方面的应用进行了探索。
本文的研究工作和创新点如下：
1.研究了电磁波垂直入射时双闭合环和双劈裂环共振器的电磁响应及其微观机制。发现由于内外环电响应的共振耦合,双环共振器具有低频的反对称模和高频的对称模。利用外电场激发内外环“断续线”型电响应和反对称模贡献的负磁导率,双环共振器可以在电磁波垂直激发时实现负折射。
2.设计了一种工作在太赫兹波段的等方型十字孔渔网电磁超介质结构,研究了主要结构参数对其电磁响应以及左手性能的影响,并利用磁响应的LC有效电路模型解释左手频带对结构参数的依赖关系。与现有的矩形孔渔网状“金属／电介质／金属”电磁超介质相比,该结构的电磁响应可以不依赖入射电磁波的偏振,并且具有较高品质因数(FOM>4)和透射率(T>80%)。
3.探索分布有孔阵列的渔网电磁超介质结构在其左手通带发生的超强透射现象的起因,发现左手通带紧邻与波导谐振模式关联的超强透射峰,利用超强透射效应可以有效降低电磁超介质的损耗,提高品质因数。渔网结构中电介质层和金属层厚度对磁共振以及左手性能的影响主要源自于波导谐振模式对孔尺寸以及深度的依赖。
4.提出一种偏振可控的近红外双左手通带平面电磁超介质,即具有不对称十字孔(十字孔的两臂长或臂宽不同)阵列的“金属／电介质／金属”结构。详细讨论并利用理论模型解释改变臂长和臂宽对双左手通带的调制作用。进一步计算空间局域电场分布发现与等离子体模式关联的激发电场可以在两金属板中间区域引起12倍的电场增强,当探针分子处于这些“热点”位置时可以获得-104的拉曼信号增强。
5.系统研究了不对称双劈裂环阵列结构在光波垂直入射下的可调谐等离子体光学性能和不同共振模式激发时的场增强效应。该结构在近红外和可见光区域有两个强消光峰,分别对应等离子体的一阶共振(Ⅰ)和二阶共振(Ⅱ)。通过激发不同的共振模式,不对称双劈裂环阵列结构可以在近红外和可见光波段,在相同空间区域,即裂口位置获得显著增强的电场,电磁场热点位置位于金属弧的棱边和棱角附近,最大电场增强接近或超过-103,分别对应红外吸收和拉曼增强因子-105和1012-1013,并且增强效果可以通过缩小裂口宽度和优化金属弧顶端结构得到进一步提高。
Understanding the interaction between light and matter and manipulating light and electromagnetic waves at will have always been the people's pursuit, and also been the essential issues in science and technology. With the advance of technology, micron and even nano-scale metal periodic structures can be fabricated. When electromagnetic waves illuminate these structures with sub-wavelength size, there will appear a series of new phenomena or effects, such as "metamaterials" and surface plasmons. Metamaterials are artificial composite or structured materials constructed by periodically arranging special geometric elements, which exhibit properties not found in naturally occurring materials or compounds. Wave propagation in metamaterials with simultaneously negative dielectric permittivity and magnetic permeability can exhibit exotic properties, for instance backward-wave transmission, negative refraction, evanescent wave amplification etc. The electromagnetic properties of matematerials depend highly on the element's geometry. This flexibility provides a novel concept for us to design new materials with extraordinary electromagnetic properties, and also open a new channel to manipulate and control the light and electromagnetic waves.
Metamaterials are usually based on metallic structure units since it is convenient to use metal to realize structure with various shapes or patterns. However, conducting loss is the major drawback limiting their applications. Metamaterials with simple structures for easy preparation and excellent performance (low loss, broadband, solid, uniform isotropic) are desired. In this thesis, several novel structured metamaterials working respectively in microwave, terahertz and infrared frequencies are designed aiming at achieving negative refraction with lower losses and clarifying related mechanisms therein. Moreover, metallic structures based on metamaterials with tunable, stable and large local field enhancement are explored for possible applications as substrates of surface-enhanced spectroscopy, aiming at breaking the bottleneck hindering wide applications of surface-enhanced spectroscopy, namely, the poor reproducibility of signals with traditional substrates due to the lack of control in metal particles produced by chemical process.
The main progresses and innovation of this work are listed as follows:
(1) We investigated the electromagnetic responses and mechanisms of double split-and closed-ring resonators at normal-to-plane incidence. It is found that the double ring metamaterials exhibit respectively antisymmetric and symmetric modes in lower and higher frequencies due to the resonance coupling of the inner and outer rings. By combining the cut-wire type electric resonance in both outer and inner rings excited by external electric field and the negative magnetic response associated with antisymmetric mode, negative refraction can be achieved in the double-ring metamaterials at normal-to-plane incidence.
(2) We designed an isotropic-like fishnet metamaterial in terahertz frequencies. The influences of its main geometry parameters on both the electromagnetic response and the left-handed property are investigated. An effective LC circuit description for magnetic resonance is employed to explain the dependence of left-handed frequency band on geometry parameters. Compared to the current "metal/dielectric/metal" fishnet metamaterials with rectangular holes, this structure is insensitive to polarization configurations, exhibits a large figure of merit (FOM>4) and has a high transmission (T>80%).
(3) The physical mechanism that the left-handed behavior occurring together with the extraordinary optical transmission (EOT) in fishnet metamaterials is explored. It is found the left-handed band is adjacent to the EOT peak that is associated with waveguide resonant mode, and the EOT effect can be used to reduce the losses and improve the figure of merit in metamaterials. The influence of metal-layer thickness on magnetic resonance and left-handed performance in fishnet metamaterials with rectangular-hole or cross-hole originate mainly from the dependence of waveguide resonant mode on the hole's size and depth.
(4) A metal-dielectric-metal sandwich structure perforated by an array of asymmetric cross holes (i.e. both arms in cross hole have different length or width) is proposed and a novel planar metamaterial with dual left-handed bands is demonstrated. The tunability of dual left-handed bands by changing the arms' length or width is investigated, and the mechanism is elucidated with a theoretical model. Furthermore, by investigating the corresponding electric field distributions, the maximum field enhancement factor of 12 is achieved within the dielectric layer between two metal plates, meaning a Raman signal enhancement of～104 for probe molecules located at these positions.
(5) We investigated the plasmon resonance properties at normal incidence and the large field enhancement effects from different plasmon excitations in asymmetric double split rings (ADSRs) arrays. The ADSRs exhibit two intense excitation peaks in the near-infrared and visible regions, corresponding to first-and second-order resonance modes. By exciting different resonances, the electric field can be effectively localized and enhanced in the same area, i.e. the gap regions, in both the infrared and the visible for ADSRs with different asymmetries. The field "hotspots" are demonstrated to be at the tips or the edges with the maximum field enhancement close to or over 103, corresponding to a infrared absorption and Raman enhancement factor of about～105 and 1012～1013 respectively. The local field enhancement can be further enhanced by decreasing the gap's width and optimizing the tips'ends of split rings.
电磁超介质通常基于金属的结构单元,采用金属便于实现形状或图案各异的周期结构,但金属的损耗问题是限制金属电磁超介质负折射性能及其应用的关键。结构简单,易于制备,且性能(低损耗、宽频带、固态的、均匀各向同性)良好的电磁超介质是科研工作者追求的目标。本论文设计并研究了几种工作在微波、太赫兹和红外波段的电磁超介质,探索可以实现“负折射”,且能有效降低损耗的结构和机制。同时,针对制约表面增强光谱技术实际广泛应用的瓶颈,即传统衬底结构可控性差导致的表面增强光谱重现性差的问题,对具有可控、稳定、高效的电磁场增强效果的电磁超介质结构在表面增强光谱衬底方面的应用进行了探索。
本文的研究工作和创新点如下：
1.研究了电磁波垂直入射时双闭合环和双劈裂环共振器的电磁响应及其微观机制。发现由于内外环电响应的共振耦合,双环共振器具有低频的反对称模和高频的对称模。利用外电场激发内外环“断续线”型电响应和反对称模贡献的负磁导率,双环共振器可以在电磁波垂直激发时实现负折射。
2.设计了一种工作在太赫兹波段的等方型十字孔渔网电磁超介质结构,研究了主要结构参数对其电磁响应以及左手性能的影响,并利用磁响应的LC有效电路模型解释左手频带对结构参数的依赖关系。与现有的矩形孔渔网状“金属／电介质／金属”电磁超介质相比,该结构的电磁响应可以不依赖入射电磁波的偏振,并且具有较高品质因数(FOM>4)和透射率(T>80%)。
3.探索分布有孔阵列的渔网电磁超介质结构在其左手通带发生的超强透射现象的起因,发现左手通带紧邻与波导谐振模式关联的超强透射峰,利用超强透射效应可以有效降低电磁超介质的损耗,提高品质因数。渔网结构中电介质层和金属层厚度对磁共振以及左手性能的影响主要源自于波导谐振模式对孔尺寸以及深度的依赖。
4.提出一种偏振可控的近红外双左手通带平面电磁超介质,即具有不对称十字孔(十字孔的两臂长或臂宽不同)阵列的“金属／电介质／金属”结构。详细讨论并利用理论模型解释改变臂长和臂宽对双左手通带的调制作用。进一步计算空间局域电场分布发现与等离子体模式关联的激发电场可以在两金属板中间区域引起12倍的电场增强,当探针分子处于这些“热点”位置时可以获得-104的拉曼信号增强。
5.系统研究了不对称双劈裂环阵列结构在光波垂直入射下的可调谐等离子体光学性能和不同共振模式激发时的场增强效应。该结构在近红外和可见光区域有两个强消光峰,分别对应等离子体的一阶共振(Ⅰ)和二阶共振(Ⅱ)。通过激发不同的共振模式,不对称双劈裂环阵列结构可以在近红外和可见光波段,在相同空间区域,即裂口位置获得显著增强的电场,电磁场热点位置位于金属弧的棱边和棱角附近,最大电场增强接近或超过-103,分别对应红外吸收和拉曼增强因子-105和1012-1013,并且增强效果可以通过缩小裂口宽度和优化金属弧顶端结构得到进一步提高。
Understanding the interaction between light and matter and manipulating light and electromagnetic waves at will have always been the people's pursuit, and also been the essential issues in science and technology. With the advance of technology, micron and even nano-scale metal periodic structures can be fabricated. When electromagnetic waves illuminate these structures with sub-wavelength size, there will appear a series of new phenomena or effects, such as "metamaterials" and surface plasmons. Metamaterials are artificial composite or structured materials constructed by periodically arranging special geometric elements, which exhibit properties not found in naturally occurring materials or compounds. Wave propagation in metamaterials with simultaneously negative dielectric permittivity and magnetic permeability can exhibit exotic properties, for instance backward-wave transmission, negative refraction, evanescent wave amplification etc. The electromagnetic properties of matematerials depend highly on the element's geometry. This flexibility provides a novel concept for us to design new materials with extraordinary electromagnetic properties, and also open a new channel to manipulate and control the light and electromagnetic waves.
Metamaterials are usually based on metallic structure units since it is convenient to use metal to realize structure with various shapes or patterns. However, conducting loss is the major drawback limiting their applications. Metamaterials with simple structures for easy preparation and excellent performance (low loss, broadband, solid, uniform isotropic) are desired. In this thesis, several novel structured metamaterials working respectively in microwave, terahertz and infrared frequencies are designed aiming at achieving negative refraction with lower losses and clarifying related mechanisms therein. Moreover, metallic structures based on metamaterials with tunable, stable and large local field enhancement are explored for possible applications as substrates of surface-enhanced spectroscopy, aiming at breaking the bottleneck hindering wide applications of surface-enhanced spectroscopy, namely, the poor reproducibility of signals with traditional substrates due to the lack of control in metal particles produced by chemical process.
The main progresses and innovation of this work are listed as follows:
(1) We investigated the electromagnetic responses and mechanisms of double split-and closed-ring resonators at normal-to-plane incidence. It is found that the double ring metamaterials exhibit respectively antisymmetric and symmetric modes in lower and higher frequencies due to the resonance coupling of the inner and outer rings. By combining the cut-wire type electric resonance in both outer and inner rings excited by external electric field and the negative magnetic response associated with antisymmetric mode, negative refraction can be achieved in the double-ring metamaterials at normal-to-plane incidence.
(2) We designed an isotropic-like fishnet metamaterial in terahertz frequencies. The influences of its main geometry parameters on both the electromagnetic response and the left-handed property are investigated. An effective LC circuit description for magnetic resonance is employed to explain the dependence of left-handed frequency band on geometry parameters. Compared to the current "metal/dielectric/metal" fishnet metamaterials with rectangular holes, this structure is insensitive to polarization configurations, exhibits a large figure of merit (FOM>4) and has a high transmission (T>80%).
(3) The physical mechanism that the left-handed behavior occurring together with the extraordinary optical transmission (EOT) in fishnet metamaterials is explored. It is found the left-handed band is adjacent to the EOT peak that is associated with waveguide resonant mode, and the EOT effect can be used to reduce the losses and improve the figure of merit in metamaterials. The influence of metal-layer thickness on magnetic resonance and left-handed performance in fishnet metamaterials with rectangular-hole or cross-hole originate mainly from the dependence of waveguide resonant mode on the hole's size and depth.
(4) A metal-dielectric-metal sandwich structure perforated by an array of asymmetric cross holes (i.e. both arms in cross hole have different length or width) is proposed and a novel planar metamaterial with dual left-handed bands is demonstrated. The tunability of dual left-handed bands by changing the arms' length or width is investigated, and the mechanism is elucidated with a theoretical model. Furthermore, by investigating the corresponding electric field distributions, the maximum field enhancement factor of 12 is achieved within the dielectric layer between two metal plates, meaning a Raman signal enhancement of～104 for probe molecules located at these positions.
(5) We investigated the plasmon resonance properties at normal incidence and the large field enhancement effects from different plasmon excitations in asymmetric double split rings (ADSRs) arrays. The ADSRs exhibit two intense excitation peaks in the near-infrared and visible regions, corresponding to first-and second-order resonance modes. By exciting different resonances, the electric field can be effectively localized and enhanced in the same area, i.e. the gap regions, in both the infrared and the visible for ADSRs with different asymmetries. The field "hotspots" are demonstrated to be at the tips or the edges with the maximum field enhancement close to or over 103, corresponding to a infrared absorption and Raman enhancement factor of about～105 and 1012～1013 respectively. The local field enhancement can be further enhanced by decreasing the gap's width and optimizing the tips'ends of split rings.
引文
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