发表机构
Max-Born-Institut; Department of Chemistry, New York University; Instituto de Ciencia de Materiales de Madrid (ICMM-CSIC); Department of Chemistry, Molecular Sciences Research Hub, Imperial College London; Technion–Israel Institute of Technology; Department of Physics, Humboldt Universität zu Berlin; Technische Universität Berlin; University of Ottawa, Faculty of Science（马克斯·玻恩研究所; 纽约大学化学系; 马德里材料科学研究所（CSIC）; 帝国理工学院分子科学研究中心化学系; 以色列理工学院; 柏林洪堡大学物理系; 柏林工业大学; 渥太华大学理学院）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本文提出光子架构产生合成手性光，通过空芯波导增强手性光-物质相互作用，实现高效灵敏的手性传感，并预测了皮焦级三次谐波发射与200%二色性。
AI 中文摘要
分子手性产生左旋和右旋对映体，其平衡支撑着生化功能。偏离这种对映体过量是疾病的有前景的生物标志物。尽管其重要性，快速灵敏地检测痕量小手性分子中的对映体过量仍然是一个突出的挑战。合成手性光为手性光谱学引入了新的机会，有潜力将光-物质相互作用增强几个数量级。在这里，我们提出了一类新的用于合成手性光的光子架构，其中光子结构产生、引导和优化手性光-物质相互作用。作为首次实现，我们展示了空芯介质波导支持多色场的相位匹配传播，使得对映体敏感的非线性响应在厘米级距离上相干累积。通过将微观量子响应模拟与麦克斯韦方程组相结合，我们预测，在仅2厘米的传播距离上，约1微焦的入射脉冲能量可从仅皮摩尔量的香芹酮气体（50毫巴）产生数百皮焦的三次谐波发射，对映体敏感对比度接近5%。相位分辨傅里叶分析分离出无背景的手性信号，展现出200%的最大可能二色性。除了高效的手性传感，用于合成手性光的光子架构为集成非线性手性光谱学、基于超快电子动力学的分子指纹识别以及拓扑鲁棒的手性光学可观测量建立了一个可扩展的平台。
英文摘要
Molecular chirality gives rise to left- and right-handed enantiomers whose balance underpins biochemical function. Deviations from this enantiomeric excess are promising biomarkers of disease. Despite its importance, rapid and sensitive detection of enantiomeric excess in trace amounts of small chiral molecules remains an outstanding challenge. Synthetic chiral light introduces new opportunities for chiroptical spectroscopy, with the potential to enhance light-matter interactions by several orders of magnitude. Here we propose a new class of photonic architectures for synthetic chiral light, in which photonic structures generate, guide and optimize chiral light-matter interactions. As a first realization, we show that hollow dielectric waveguides support phase-matched propagation of multicolor fields enabling coherent accumulation of the enantio-sensitive nonlinear response over centimeter-scale distances. By combining microscopic quantum-response simulations with Maxwell's equations, we predict that incident pulse energies of around 1 uJ produce hundreds of picojoules of third-harmonic emission from only picomole quantities of carvone gas at 50 mbar over just 2 cm of propagation, with enantio-sensitive contrast approaching 5%. Phase-resolved Fourier analysis isolates a background-free chiral signal exhibiting the maximum possible dichroism of 200%. Beyond efficient chiral sensing, photonic architectures for synthetic chiral light establish a scalable platform for integrated nonlinear chiral spectroscopy, molecular fingerprinting based on ultrafast electron dynamics, and topologically robust chiroptical observables.
