Enabling Thermally Stimulated Delayed Phosphorescence in Cu(I) Cyclic Trinuclear Complexes with Near-Unity Quantum Yield.

Guo-Quan Huang,Ri-Qin Xia,Xu Chen,Hu Yang,Yong-Liang Huang,Kun Wu,Ji Zheng,Weigang Lu,Dan Li

pubmed（2025）

Department of Chemistry

Cited 0|Views2

Abstract

Thermally stimulated delayed phosphorescence (TSDP) emission has recently been discovered in several Au(I)/Au(III) complexes, featuring thermally enhanced emission intensities and notable quantum yields (QYs). Developing earth-abundant metal-based TSDP emitters with further increased QYs holds significant promise for practical applications. Herein, we present a halogen bonding approach to achieve TSDP emission in bromo-substituted Cu(I) cyclic trinuclear complexes (CTCs). Photophysical analysis and theoretical calculations reveal the crucial role of halogen bonding in suppressing the excited-state distortions and reducing energy differences between the first and second triplet excited states (T1 and T2). This enables efficient spin-allowed reverse internal conversion, leading to the TSDP behavior. Additionally, the low internal reorganization energy and rigid halogen-bonded network in bromo-substituted Cu(I) CTCs result in significantly suppressed nonradiative decay and high QYs, with one approaching near-unity. This work provides an innovative approach to extend the TSDP behavior from Au(I)/Au(III) to Cu(I) complexes with high QYs.

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【要点】：本研究通过溴代铜(I)环状三核配合物中的卤素键合方法，实现了热刺激延迟磷光发射，并获得了接近 unity 的量子产率，为开发高效地球丰饶金属基 TSDP 发光材料提供了新途径。

【方法】：作者利用光物理分析和理论计算揭示了卤素键合在抑制激发态畸变和减小第一和第二三重激发态（T1 和 T2）之间的能量差异中的作用，从而实现高效的逆向内部转换并导致 TSDP 行为。

【实验】：研究在溴代 Cu(I) 环状三核配合物（CTCs）中进行了实验，实验结果表明，低内重组能和刚性的卤素键合网络显著抑制了非辐射衰减，使得量子产率显著提高，接近 unity。论文中未明确提及使用的数据集名称。