等离激元超构表面上的二次谐波产生与调控

光学超构表面是一种由亚波长尺度的超构单元在面内排布而构成的准二维人工结构材料。由于其具有对光场进行多维度调控的能力，且易于集成，超构表面近年来受到了广泛关注。通过引入非线性光学过程，超构表面也可以用于实现光学频率转换、光开关等功能。本论文聚焦等离激元超构表面上的二次谐波产生与调控机理的研究，通过设计等离激元纳米共振腔、超构单元的耦合效应和金属-晶体复合结构，探索调控二次谐波的振幅、偏振和相位的新原理和新方法。
纳米共振腔增强效应：在单层等离激元超构表面上，局域共振效应可以显著增强二次谐波的转换效率。然而，共振波长处存在较强的反射和散射导致泵浦光的耦合效率较低，从而限制了共振模式对局域光场的增强效果。本论文通过在超构表面上引入纳米共振腔设计，抑制了共振波长处的反射和散射损耗，从而大幅提高了二次谐波的转换效率。
耦合诱导增强效应：超构表面上的二次谐波的振幅和偏振调控主要基于对超构单元几何形状的设计而实现，而超构单元间的耦合效应通常被忽视。本论文将两组具有中心反演对称性的等离激元超构单元以六角晶格进行排列，借助超构单元间的耦合效应打破全局中心反演对称性，实现了对所产生的二次谐波的振幅和偏振的调控。
金属-晶体复合超构表面：超构表面上的手性非线性光学响应的实现主要依赖于超构单元的几何形状，难以在特定的工作波长对圆二向色性进行连续调控。本论文设计了一种由等离激元超构单元和非线性光学晶体组成的复合超构表面，借助超构单元和晶体的对称性，揭示了具有三种传播相位或几何相位的二次谐波转换通道。通过调控超构单元与晶体的面内扭转角，实现了复合超构表面上二次谐波的圆二向色性调控。
本论文系统地研究了等离激元超构表面上的二次谐波产生与调控机理。通过优化纳米共振腔的共振模式、设计超构表面的全局对称性、引入具有特定对称性的晶体材料等，不仅提高了二次谐波转换效率，而且实现了对其振幅、偏振和相位的调控。相关研究方法和结果有望为发展高效率、多功能非线性光学超构表面提供重要理论基础和技术方案。

Optical metasurfaces are quasi-two-dimensional artificial structural materials composed of sub-wavelength meta-atoms. For their advantages in multi-dimensional optical field manipulation and integration, metasurfaces have received widespread attention in recent years. By introducing nonlinear optical processes, optical functions like frequency conversion, switching can be realized on metasurfaces. This thesis focuses on the second harmonic generation and manipulation on plasmonic metasurfaces. By designing plasmonic nano-cavities, inter-meta-atom coupling effects and metal-crystal hybrid structures, new principles and methods are observed for controlling the amplitude, polarization, and phase of second harmonic waves.
Nano-cavity enhancement effect: On single-layer plasmonic metasurfaces, the conversion efficiency of second-harmonic waves can be enhanced by the local resonance modes. However, the significant reflection and scattering at the resonant wavelength lead to low coupling efficiency of the pump light, limiting the enhancement effect of the resonant mode on the local field. This research introduces nano-cavities onto the metasurfaces, which significantly suppress radiation losses at the resonant wavelength and greatly enhance the second-harmonic generation process.
Coupling-induced enhancement effect: The amplitude and polarization modulation of second-harmonic waves on metasurfaces are usually realized by designing the shape of meta-atoms, while the coupling of meta-atoms is usually neglected. This research arranges two groups of plasmonic meta-atoms with inversion symmetry into a hexagonal lattice, breaks the global inversion symmetry, and realizes the controlling of the amplitude and polarization of the second harmonics.
Metal-crystal hybrid metasurface: The realization of nonlinear optical chirality usually relies on the shape design of chiral meta-atoms, making it difficult to achieve a continuous chirality modulation at the certain wavelength. This research designs a hybrid metasurface composed of plasmonic meta-atoms and nonlinear optical crystals. Leveraging both symmetries of meta-atoms and crystals, three second-harmonic conversion channels with different propagation and geometric phases are observed. By using the interference between different channels and designing the in-plane twisting angle between the meta-atoms and the crystals, continuous modulation of the second-harmonic circular dichroism can be realized on the hybrid metasurface.
In summary, this thesis systematically studies the methods and mechanisms of the second-harmonic generation and manipulation on plasmonic metasurfaces. By optimizing the resonant mode of nano-cavities, designing the global symmetry-breaking effect of the metasurface, and introducing crystal materials with symmetries, not only improvements of the second-harmonic conversion efficiency achieved, but also precise modulation of the amplitude, polarization, and phase realized. The related methods and results of this thesis will provide a theoretical and practical guidance for the design of efficient multifunctional nonlinear optical metasurfaces.

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