Liu Yuanfeng, Zhou Le, Guo Mengfan, Xu Zongqi, Ma Jing, Wen Yongzheng, Litchinitser Natalia M, Shen Yang, Sun Jingbo, Zhou Ji
State Key Laboratory of New Ceramics and Fine Processing, School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.
Department of Electrical and Computer Engineering, Duke University, Durham, NC, 27705, USA.
Adv Mater. 2024 Nov;36(45):e2412007. doi: 10.1002/adma.202412007. Epub 2024 Sep 23.
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 is underway since decades. A self-assembled spherulite material comprised of synthesized molecules with large dipole moments aligned azimuthally, forming a vortex polarity with spontaneously broken symmetry, is experimentally demonstrated. This unique self-assembled structure enables new linear and nonlinear light-matter interactions, including generating optical vortex beams with complex spin states and on-demand topological charges at the fundamental, doubled, and tripled frequencies. This work will likely enable numerous applications in areas such as high-dimensional quantum information processing with large capacity and high security, spatiotemporal optical vortices, and a novel optical manipulation and trapping platform.
固体的结构对称性在定义其线性和非线性光学性质方面起着重要作用。几十年来，人们一直在探索通用、经济高效、大规模且无缺陷的方法和材料平台，以便按需定制结构和光学性质。实验证明了一种由具有沿方位角排列的大偶极矩的合成分子组成的自组装球晶材料，形成了具有自发破缺对称性的涡旋极性。这种独特的自组装结构实现了新的线性和非线性光与物质相互作用，包括在基频、倍频和三倍频下产生具有复杂自旋态和按需拓扑电荷的光学涡旋光束。这项工作可能会在诸如大容量、高安全性的高维量子信息处理、时空光学涡旋以及新型光学操纵和捕获平台等领域带来众多应用。
