纳米多孔光子超材料中生色团的各向异性限制引起的二阶非线性光学
Anisotropic Confinement of Chromophores Induces Second-Order Nonlinear Optics in a Nanoporous Photonic Metamaterial
摘要：
二阶非线性光学是各种旨在对光进行主动操纵的器件的基础。然而，物理原理限制它的发生非中心对称，各向异性物质。这显著地限制了表现出非线性光学的基础材料的数量。在这里，我们表明，嵌入发色团在一个阵列中的锥形通道13纳米在单片二氧化硅结果介观各向异性物质，从而在混合材料显示二次谐波产生（SHG）。这种非线性光学相比，在电晕极化聚合物薄膜中实现的含有相同的发色团。它起源于约束诱导的取向秩序的细长的客体分子在纳米通道。这导致了非中心对称偶极序，从而导致了在亚波长、单孔尺度上的非线性光-物质相互作用。我们的研究表明，大规模的，自组织的纳米多孔性的整体固体的出现，以及在单孔尺度上的生色团的限制可控的取向顺序提供了一个可靠的和可访问的工具来设计具有非线性元光学材料。
英文摘要：
Second-order nonlinear optics is the base for a large variety of devices aimed at the active manipulation of light. However, physical principles restrict its occurrence to non-centrosymmetric, anisotropic matter. This significantly limits the number of base materials exhibiting nonlinear optics. Here, we show that embedding chromophores in an array of conical channels 13 nm across in monolithic silica results in mesoscopic anisotropic matter and thus in a hybrid material showing second-harmonic generation (SHG). This non-linear optics is compared to the one achieved in corona-poled polymer films containing the identical chromophores. It originates in confinement-induced orientational order of the elongated guest molecules in the nanochannels. This leads to a non-centrosymmetric dipolar order and hence to a non-linear light-matter interaction on the sub-wavelength, single-pore scale. Our study demonstrates that the advent of large-scale, self-organised nanoporosity in monolithic solids along with confinement-controllable orientational order of chromophores at the single-pore scale provides a reliable and accessible tool to design materials with a nonlinear meta-optics.
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