两种新型杂化金属卤化物玻璃的制备和光学性能研究

零维有机-无机杂化金属卤化物是由有机阳离子和无机多面体组成，具 有独特的“主-客体”结构，在光电领域受到广泛的关注。这种杂化材料具 有晶格较软、量子限域效应强等特征，表现出优异的光学性质。晶相的杂 化金属卤化物可以通过熔融淬火转变为玻璃相，结构的转变导致了新颖的 光化学性质，在 X 射线探测和防伪等光学领域有潜在的应用价值。本文设 计合成了两种杂化金属卤化物，研究了其晶态和玻璃态的结构和光学性质， 并且探究了结构转变导致的电荷转移（CT）激子作用对玻璃态发光性质的 影响。研究总结如下： 具有弱 CT 激子相互作用的杂化锡基晶体转变为玻璃后，导致 CT 作用 增强，实现发光效率的提升。具体而言，利用甲基三苯基磷阳离子与二价 锡离子分别构筑了杂化锡基金属卤化物晶体和玻璃。其中，晶体展示了弱 的近红外发射，而相应的玻璃具有增强的近红外发射，并且出现了新的发 射峰，总荧光量子产率从小于 1%增大至 82.7%。研究发现，晶体和玻璃中 的近红外发射来源于结构中无机多面体向有机配体的 CT 激子跃迁，而玻璃 中新的发射峰是源于玻璃态结构中刚性增强导致的自陷态激子发射。 锌基晶体玻璃化后激活了 CT 相互作用，提升了发光效率，并且产生了 新颖的发光性质。将手性 R/S-3-氨基哌啶阳离子与锌离子结合制备了手性 锌基杂化卤化物晶体和玻璃。其中，晶体展现出蓝光发射，荧光量子产率 为 8.5%；而玻璃展现出增强的白光发射，荧光量子产率增大至 31.5%，延 迟寿命延长了 25 倍。研究表明，玻璃中刚性的增强诱导了 CT 激子的产生， 导致了热活化延迟荧光、反热猝灭磷光以及高效的圆偏振发光。 本论文研究了两种新型的杂化金属卤化物玻璃，实现了晶体转变为玻 璃后荧光量子产率的增强，丰富了发光杂化玻璃材料体系，对设计下一代 光学材料具有重要的参考价值。

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