近日，南京工业大学彭其明团队研究了Diradial系统中亮暗自由基配对实现的自旋相关发光。2025年8月11日，《德国应用化学》杂志发表了这一成果。

自旋光调制是自旋电子学、基于自旋的光电子学和量子材料等新兴技术的核心。开壳发光双自由基，具有两个不配对和合成可调的自旋，提供了一个分子平台来实现这种控制。然而，先前的研究仅限于对称系统，其中自旋相互作用发生在两个相同的发光自由基之间。

研究组证明了非发光（暗）自由基可以有效地调节不对称双自由基框架内发光（亮）自由基的自旋和光物理行为。所得分子在低温下表现出独特的三级磁致发光（ML）响应，由超精细偶联（HFC）引起(B <0.05 T)、Δg-induced自旋混合（0.05 ~ 0.8 T）和自旋极化（0.8 ~ 7 T）。值得注意的是，该系统在超低磁场下表现出明显的ML增强（>14%），这是一种在分子自旋光学系统中从未报道过的现象。这些发现确立了不对称明暗双基作为自旋光子界面设计的强大新基序，为开壳系统的基本光物理学提供了新的见解。

附：英文原文

Title: Spin-Correlated Luminescence Enabled by Bright–Dark Radical Pairing in a Diradical System

Author: Xing Wang, Shengjie Wang, Zhaoze Ding, Li Shen, Zihao Zhu, Alim Abdurahman, Geyu Lu, Qiming Peng

Issue&Volume: 2025-08-11

Abstract: Spin-optical modulation lies at the core of emerging technologies in spintronics, spin-based optoelectronics, and quantum materials. Open-shell luminescent diradicals, featuring two unpaired and synthetically tunable spins, offer a molecular platform to achieve such control. However, previous studies have been restricted to symmetric systems, where spin interactions occur between two identical, luminescent radicals. Here, we demonstrate that a non-luminescent (dark) radical can effectively modulate the spin and photophysical behavior of a luminescent (bright) radical within an asymmetric diradical framework. The resulting molecule exhibits a unique three-stage magnetoluminescence (ML) response at low temperatures, arising from hyperfine coupling (HFC) (B < 0.05 T), the Δg-induced spin mixing (0.05–0.8 T), and spin polarization (0.8–7 T). Notably, the system exhibits pronounced ML enhancement (>14%) under ultra-low magnetic fields (B < 0.05 T), a previously unreported phenomenon in molecular spin-optical systems. These findings establish asymmetric bright–dark diradicals as a powerful new motif for spin-photon interface design, providing fresh insights into the fundamental photophysics of open-shell systems.

DOI: 10.1002/anie.202513593

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202513593