由结构涡旋实现的光学涡旋
Optical vortices enabled by structural vortices
AI总结：
本文利用自组装有机球晶的自发涡旋极性与结构对称性破缺，实现强各向异性及非线性响应，并在基频、倍频和三倍频产生可定制拓扑荷的光学涡旋。
摘要：
固体的结构对称性在决定其线性和非线性光学性质方面发挥着重要作用。数十年来，人们一直在寻求通用、低成本、大规模且无缺陷的方法与材料平台，以按需调控结构和光学性质。我们通过实验展示了一种基于自下而上自组装的有机工程材料：该材料由具有大偶极矩的合成分子组成，这些分子结晶形成球晶结构。分子沿方位角方向排列，产生对称性自发破缺的涡旋极性，从而导致强光学各向异性和非线性光学响应。精心设计的有机球晶所具有的这些独特偏振性质，与结构化光束的对称性相结合，可实现大量新的线性和非线性光—物质相互作用，包括在基频、二倍频和三倍频处生成具有复杂自旋态和按需拓扑荷的光学涡旋光束。本工作结果有望在高容量、高安全性的高维量子信息处理等领域实现众多应用。所展示的球晶晶体有助于构建依赖独特微尺度自发涡旋极性的独立微尺度器件，这可能在未来用于高维量子信息处理、时空光学涡旋，以及作为光学操控和捕获的新型平台。
英文摘要：
The structural symmetry of solids plays an important role in defining their linear and nonlinear optical properties. The quest for versatile, cost-effective, large-scale, and defect-free approaches and materials platforms for tailoring structural and optical properties on demand has been underway for decades. We experimentally demonstrate a bottom-up self-assembly-based organic engineered material comprised of synthesized molecules with large dipole moments that are crystallized into a spherulite structure. The molecules align in an azimuthal direction, resulting in a vortex polarity with spontaneously broken symmetry leading to strong optical anisotropy and nonlinear optical responses. These unique polarization properties of the judiciously designed organic spherulite combined with the symmetry of structured optical beams enable a plethora of new linear and nonlinear light-matter interactions, including the generation of optical vortex beams with complex spin states and on-demand topological charges at the fundamental, doubled, and tripled frequencies. The results of this work are likely to enable numerous applications in areas such as high-dimensional quantum information processing, with large capacity and high security. The demonstrated spherulite crystals facilitate stand-alone micro-scale devices that rely on the unique micro-scale spontaneous vortex polarity that is likely to enable future applications for high-dimensional quantum information processing, spatiotemporal optical vortices, and a novel platform for optical manipulation and trapping.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
