Yang Qing, Wang Weibin, Yang Yunfeng, Li Pengyuan, Yang Xinyi, Bai Fuquan, Zou Bo
State Key Laboratory of Superhard Materials, Synergetic Extreme Condition High-Pressure Science Center, College of Physics, Jilin University, Changchun, China.
International Joint Research Laboratory of Nano-Micro Architecture Chemistry, Institute of Theoretical Chemistry and College of Chemistry, Jilin University, Changchun, China.
Nat Commun. 2025 Jan 15;16(1):696. doi: 10.1038/s41467-025-55978-9.
Metal-organic frameworks that feature hybrid fluorescence and phosphorescence offer unique advantages in white-emitting communities based on their multiple emission centers and high exciton utilization. However, it poses a substantial challenge to realize superior white-light emission in single-component metal-organic frameworks without encapsulating varying chromophores or integrating multiple phosphor subunits. Here, we achieve a high-performance white-light emission with photoluminescence quantum yield of 81.3% via boosting triplet excitons distribution through pressure treatment in single-component Zn-IPA metal-organic frameworks. A novel metal-ligand asymmetrical chelate coordination is successfully integrated into the Zn-IPA after a high-pressure treatment over ~20.0 GPa. This modification unexpectedly endows the targeted sample with a new emergent electronic state to narrow the singlet-triplet energy gap, which effectively accelerates the spin-flipping process for boosted triplet excitons population. Time delay phosphor-converted light-emitting diodes are fabricated with long emission time up to ~7 s after switching off, providing significant advancements for white-light and time-delay lighting applications.
具有混合荧光和磷光特性的金属有机框架，基于其多个发射中心和高激子利用率，在白光发射领域具有独特优势。然而，在不封装不同发色团或整合多个磷光亚基的情况下，要在单一组分金属有机框架中实现优异的白光发射是一项巨大挑战。在此，我们通过在单一组分Zn-IPA金属有机框架中进行压力处理来促进三重态激子分布，实现了光致发光量子产率达81.3%的高性能白光发射。在超过约20.0 GPa的高压处理后，一种新型的金属-配体不对称螯合配位成功整合到Zn-IPA中。这种修饰意外地赋予目标样品一种新出现的电子态，以缩小单重态-三重态能隙，从而有效加速自旋翻转过程，促进三重态激子的产生。制备了时间延迟磷光转换发光二极管，关闭后发光时间长达约7秒，为白光和时间延迟照明应用带来了显著进展。
