美国哈佛大学Sascha Feldmann团队近日研究了宽带瞬态全斯托克斯发光光谱。该研究于2025年6月25日发表在《自然》杂志上。

发射圆偏振光（CPL）的材料在从高效显示器到量子信息技术的应用中备受追捧。然而，已建立的时间分辨CPL（TRCPL）表征方法存在明显的局限性，通常需要在灵敏度、可访问的时间尺度和光谱信息之间权衡。这限制了材料开发所需的深入光物理见解的获取。

研究组演示了一种高灵敏度（噪声水平为10⁻⁴量级）、宽带（约400–900 nm），瞬态（纳秒分辨率，毫秒范围）全斯托克斯（CPL和线性偏振）光谱设置。所实现的高灵敏度、宽波长响应和灵活时间范围的结合代表了与之前的TRCPL方法相比有重大进步。因此，TRCPL测量被证明适用于迄今为止无法访问的材料系统和光物理过程，包括具有低（10⁻³）不对称因子和跨越纳秒到毫秒时间范围的发光途径的系统。最后，全斯托克斯测量允许跟踪线性偏振分量的时间演变，这些分量本身就很重要，但在时域中控制相关CPL伪影的背景下尤其重要。 

附：英文原文

Title: Broadband transient full-Stokes luminescence spectroscopy

Author: Reponen, Antti-Pekka M., Mattes, Marcel, VanOrman, Zachary A., Estaque, Lilian, Pieters, Grgory, Feldmann, Sascha

Issue&Volume: 2025-06-25

Abstract: Materials emitting circularly polarized light (CPL) are highly sought after for applications ranging from efficient displays to quantum information technologies1,2,3,4,5,6,7. However, established methods for time-resolved CPL (TRCPL) characterization have notable limitations8,9,10,11,12,13,14,15,16,17, generally requiring a compromise between sensitivity, accessible timescales and spectral information. This has limited the acquisition of in-depth photophysical insight necessary for materials development. Here we demonstrate a high-sensitivity (noise level of the order of 104), broadband (about 400–900nm), transient (nanosecond resolution, millisecond range) full-Stokes (CPL and linear polarizations) spectroscopy setup. The achieved combination of high-sensitivity, broad wavelength response and flexible time ranges represents a substantial advancement over previous TRCPL approaches. As a result, TRCPL measurements are shown to be applicable to hitherto inaccessible material systems and photophysical processes, including systems with low (103) dissymmetry factors and luminescence pathways spanning nanosecond to millisecond time ranges. Finally, full-Stokes measurements allow tracking the temporal evolution of linear polarization components, of interest by themselves, but especially relevant in the context of controlling for associated CPL artefacts18,19 in the time domain.

DOI: 10.1038/s41586-025-09197-3

Source: https://www.nature.com/articles/s41586-025-09197-3