Halogenated Terephthalic Acid "Antenna Effects" in Lanthanide-SURMOF Thin Films.
Halogenated Terephthalic Acid "Antenna Effects" in Lanthanide-SURMOF Thin Films.
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DOI：
10.1021/acsami.0c15392
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发表时间：
2020-11
影响因子：
9.5
通讯作者：
Jaciara C C Santos-Jaciara-C-C-Santos-153706724;Y. Pramudya;M. Krstić;Dong-Hui Chen;B. Neumeier;C. Feldmann;W. Wenzel;E. Redel
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作者：
Jaciara C C Santos-Jaciara-C-C-Santos-153706724;Y. Pramudya;M. Krstić;Dong-Hui Chen;B. Neumeier;C. Feldmann;W. Wenzel;E. Redel
基于镧系元素的晶体涂层在能量转换器件中具有很大的潜力，但到目前为止，发光的表面锚定材料很难制造。薄膜，称为镧系表面安装金属有机框架（SURMOFs）与四取代卤化物（氟，氯和溴）对苯二甲酸衍生物连接作为光学器件的基本平台，在环境光下表现出肉眼可见的高荧光量子产率。我们表明，我们可以通过卤化物取代来调整薄膜中的发光特性，从而可以控制材料的分子结构。我们利用实验和理论技术，将“天线效应”对镧系元素光物理性质的调制机制进行了理顺，“天线效应”控制着镧系元素的能量转移和量子产率，并将其作为苯基环上原子取代的类型以及苯基环与羧酸基之间的二面角的函数。
Lanthanide-based crystalline coatings have a great potential for energy-conversion devices, but until now luminescent surface-anchored materials were difficult to fabricate. Thin films, called lanthanides surface-mounted metal-organic frameworks (SURMOFs) with tetrasubstituted halide (fluorine, chlorine, and bromine) terephthalic acid derivative linkers as a basic platform for optical devices, exhibit a high quantum yield of fluorescence visible to the naked eyes under ambient light. We show that we can tune the luminescent properties in thin films by halide substitution, which affords control over the molecular structure of the material. We rationalize the mechanism for the modulation of the photophysical properties by "antenna effect", which controls the energy transfer and quantum yields using experimental and theoretical techniques for chelated lanthanides as a function of the type of atom substitutions at the phenyl rings and the resulting dihedral angle between phenyl rings in the linkers and carboxylate groups.