可编程应变诱导的全无机钙钛矿纳米晶玻璃本征圆偏振发射

中文摘要 AI 辅助

产生圆偏振发光（CPL）对于手性光子学和高密度光学信息存储具有重要意义。目前，在半导体纳米材料中实现CPL的方法通常采用手性有机分子，这阻碍了将不同手性态逐像素集成到单一单片衬底上。在此，我们实现了无手性分子的、可编程的CPL，其来源于通过玻璃中直接激光写入合成的全无机钙钛矿纳米晶。高分辨率透射电子显微镜揭示了晶面间距的核-壳状变化，这与扭转晶格畸变一致。密度泛函理论计算进一步表明，扭转晶格畸变提升了带边电子态的自旋简并性。功率依赖的CPL测量揭示了从双折射介导的圆偏振到本征CPL的转变。此外，通过系统地调节入射线性偏振角和焦深，我们确定性地编程了CPL的手性和幅度，|glum|约为4 x 10^-3。通过展示直接激光写入对本征手性光学功能的确定性控制，我们的工作为在单片材料中实现空间集成的手性发射体建立了一种策略。

英文摘要

Circularly polarized luminescence (CPL) is central to chiral photonics, yet programming circularly polarized emission at the nanoscale remains challenging. Here, we program intrinsic CPL at its microscopic origin in laser-written all-inorganic perovskite nanocrystals embedded in glass. High-resolution transmission electron microscopy reveals a core-shell-like variation in interplanar spacing associated with intrinsic CPL, consistent with torsional lattice distortion. The torsional lattice distortion breaks inversion symmetry, while density functional theory calculations show that it lifts the spin degeneracy of the band-edge electronic states. Power-dependent measurements further reveal a transition from birefringence-mediated circular polarization to intrinsic CPL, accompanied by the emergence of a distinct core-shell-like lattice distortion in the nanocrystals. By tuning the incident linear polarization angle and focal depth, we deterministically control both the handedness and magnitude of the intrinsic CPL, with |glum| of approximately 4 ^ 10^-3. These results show that programmable intrinsic CPL originates from the structural and electronic properties of the emitting nanocrystals, enabling circularly polarized emission to be controlled at its microscopic origin and spatially encoded within a monolithic material.

发表机构

• Zhejiang University（浙江大学）
• Westlake University（西湖大学）
• Shanghai Jiao Tong University（上海交通大学）
• Westlake Institute for Optoelectronics（西湖光电子研究院）

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