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arXiv 2602.19617cond-mat.mtrl-sci
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旋转各向异性拉曼光谱仪用于高灵敏度晶体对称性分析

Rotational anisotropy Raman spectrometer for high-sensitivity crystallographic symmetry analysis

National University of Singapore(新加坡国立大学)

Di Cheng, Junxiang Li, Shizhuo Luo, Zehao Chen, Xinwei Li

AI总结:

旋转各向异性拉曼光谱仪通过高灵敏度分析晶体对称性,揭示量子材料中拓扑激发和对称破缺相的特性。

摘要:

拉曼光谱学是探测固体中集体激发和涌现量子相的基石技术。尽管极化分辨拉曼散射已被广泛用于提取本征模的对称性信息,但其传统几何结构存在显著限制:它只能访问拉曼张量元素的一部分,强制π周期性的强度模式,掩盖了内在晶体对称性,并缺乏对波矢依赖的各向异性灵敏度。为克服这些限制,我们引入了旋转各向异性拉曼光谱(RA-Raman)。通过在斜射入射下测量光学散射平面的全圆周旋转期间的散射强度,这种几何结构能够完整重建拉曼张量,并揭示丰富的旋转各向异性模式,这对于访问传统方法难以获取的细微对称性信息至关重要。我们开发了一台原型仪器来验证这种方法。对于中心对称晶体,RA-Raman能够无歧义地识别声子对称性表示并确定晶格轴。在非中心对称晶体中,它能够解析方向各向异性及声子极化子的角色散,使定量确定Faust-Henry系数以及分离变形势和电光散射贡献成为可能。通过在标准基准晶体中展示前所未有的对称性解析能力,我们确立了RA-Raman作为一种强大工具的潜力,其在量子材料中发现和表征对称破缺相和拓扑激发方面具有广阔前景。

英文摘要:

Raman spectroscopy stands as a cornerstone technique for probing collective excitations and emergent quantum phases in solids. While polarization-resolved Raman scattering has been widely used to extract symmetry information of eigenmodes, its conventional geometry suffers from significant limitations: it accesses only a subset of Raman tensor elements, enforces π-periodic intensity patterns that obscure intrinsic crystalline symmetries, and lacks sensitivity to wavevector-dependent anisotropy. To overcome these constraints, here we introduce rotational-anisotropy Raman spectroscopy (RA-Raman). By measuring scattering intensity during full azimuthal rotation of the optical scattering plane at oblique incidence, this geometry enables complete reconstruction of the Raman tensor and reveals rich rotational anisotropy patterns essential for accessing subtle symmetry information elusive to conventional methods. We developed a prototype instrument to validate this approach experimentally. For centrosymmetric crystals, RA-Raman unambiguously identifies phonon symmetry representations and determines crystallographic axes. In noncentrosymmetric crystals, it resolves directional anisotropy and angular dispersion of phonon-polaritons, enabling quantitative determination of the Faust-Henry coefficient and the separation of deformation-potential and electro-optic scattering contributions. By demonstrating unprecedented symmetry-resolving power in standard benchmark crystals, we establish RA-Raman as a powerful tool with far-reaching potential to discover and characterize symmetry-breaking phases and topological excitations in quantum materials.

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。

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