基态和激发态的协同构象调控实现刺激响应和宽调谐室温磷光,Journal of the American Chemical Society

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基态和激发态的协同构象调控实现刺激响应和宽调谐室温磷光
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-07-20 , DOI: 10.1021/jacs.3c04725
Zhu Chen ₁ , Xiaojie Chen ₁ , Dongyu Ma ₁ , Zhu Mao ₂ , Juan Zhao ₃ , Zhenguo Chi ₁

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了解分子构象的变化对于在室温磷光（RTP）材料中实现多个发射三重态至关重要。在这项工作中，我们报告了两种具有构象依赖性发光的分子，4,4'-二甲基苯偶酰（DMBZ）和4,4'-二叔丁基苯偶酰（DBBZ），并证明了刺激响应和宽调节RTP发射可以通过基态和激发态的协同构象调节来实现。由于构象变化，DMBZ 和 DBBZ 在外部刺激（包括光、力、热和熏蒸）下表现出丰富的 RTP 变化。值得注意的是，DBBZ 在基态和激发态下均表现出多种构象变化，这赋予了 DBBZ 多种发射态和独特的刺激响应行为。DBBZ在过冷液态和不同固态之间呈现多种相变，并伴有不同的磷光跃迁，其中激发态构象得到有效调节。此外，DBBZ的单组件和主客体系统都实现了宽范围的RTP调节（青色、绿色和黄色之间），显示出在温度传感、多色动态显示和信息加密方面的潜在应用。这些结果可能为理解聚集状态下复杂的构象变化提供新的视角，并为分子构象、RTP发射和刺激响应之间的关系提供独特的见解。

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Synergetic Conformational Regulations in Ground and Excited States for Realizing Stimulus-Responsive and Wide-Tuning Room-Temperature Phosphorescence

Understanding the changes of molecular conformations is crucial for realizing multiple emissive triplet states in room-temperature phosphorescence (RTP) materials. In this work, we report two molecules, 4,4′-dimethylbenzil (DMBZ) and 4,4′-di-tert-butylbenzil (DBBZ) with conformation-dependent luminescence, and demonstrate that stimulus-responsive and wide-tuning RTP emissions can be realized via synergetic conformational regulations in ground and excited states. Due to conformational changes, DMBZ and DBBZ show abundant RTP variations upon external stimuli, including light, force, heat, and fumigation. Notably, DBBZ exhibits multiple conformational changes in both ground and excited states, which endow DBBZ with multiple emissive states and unique stimulus-responsive behaviors. DBBZ presents multiple phase transitions between the supercooled liquid state and different solid states accompanied by different phosphorescence transitions, in which the excited-state conformations are effectively regulated. Moreover, wide-range RTP regulations (between cyan, green, and yellow) are realized in both single component and host–guest systems of DBBZ, showing potential applications in temperature sensing, multicolor dynamic displays, and information encryption. These results may provide new visions for understanding the complicated conformational changes in the aggregated state, as well as unique insights into the relationship between molecular conformations, RTP emissions, and stimulus responsiveness.

更新日期：2023-07-20

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