Coordination Geometrical Effect on Ligand-to-Metal Charge Transfer-Dependent Energy Transfer Processes of Luminescent Eu(III) Complexes

Pedro Paulo  Ferreira da Rosa; Shiori  Miyazaki; Haruna  Sakamoto; Yuichi  Kitagawa; Kiyoshi  Miyata; Tomoko  Akama; Masato  Kobayashi; Koji  Fushimi; Ken  Onda; Tetsuya  Taketsugu; Yasuchika  Hasegawa

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Coordination Geometrical Effect on Ligand-to-Metal Charge Transfer-Dependent Energy Transfer Processes of Luminescent Eu(III) Complexes

机译：对致发光EU（III）复合物配体 - 金属电荷转移依赖能量转移过程的协调几何效应

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Photophysical properties of europium (Eu(III)) complexes are affected by ligand-to-metal charge transfer (LMCT) states. Two luminescent Eu(III) complexes with three tetramethylheptadionates (tmh) and pyridine (py), [Eu(tmh)_(3)(py)_(1)] (seven-coordinated monocapped-octahedral structure) and [Eu(tmh)_(3)(py)_(2)] (eight-coordinated square antiprismatic structure), were synthesized for geometrical-induced LMCT level control. Distances between Eu(III) and oxygen atoms of tmh ligands were estimated using single-crystal X-ray analyses. The contribution percentages of π–4f mixing in HOMO and LUMO at the optimized structure in the ground state were calculated using DFT (LC-BLYP). The Eu–O distances and their π–4f mixed orbitals affect the energy level of LMCT states in Eu(III) complexes. The LMCT energy level of an eight-coordinated Eu(III) complex was higher than that of a seven-coordinated Eu(III) complex. The energy transfer processes between LMCT and Eu(III) ion were investigated using temperature-dependent and time-resolved emission lifetime measurements of ~(5)D_(0) → ~(7)F_(J ) transitions of Eu(III) ions. In this study, the LMCT-dependent energy transfer processes of seven- and eight-coordinated Eu(III) complexes are demonstrated for the first time.

机译：铕（Eu（III））配合物的光物理性质受配体-金属电荷转移（LMCT）状态的影响。合成了三种四甲基七碘酸盐（tmh）和吡啶（py）[Eu（tmh）（3）（py）（1）]（七配位单帽八面体结构）和[Eu（tmh）（3）（py）（2）]（八配位方形反rismatic结构）的发光Eu（III）配合物，用于几何诱导的LMCT水平控制。使用单晶X射线分析估计了Eu（III）和tmh配体的氧原子之间的距离。利用DFT（LC-BLYP）计算了基态优化结构下HOMO和LUMO中π-4f混合的贡献率。Eu-O距离及其π-4f混合轨道影响Eu（III）配合物中LMCT态的能级。八配位Eu（III）复合体的LMCT能级高于七配位Eu（III）复合体。利用~（5）D_0）的温度相关和时间分辨发射寿命测量，研究了LMCT与Eu（Ⅲ）离子之间的能量转移过程→ ~（7） Eu（III）离子的F_J（J）跃迁。在这项研究中，七配位和八配位铕（III）配合物的LMCT依赖性能量转移过程首次得到证实。

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《The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory》 |2021年第1期|共9页
作者
Pedro Paulo Ferreira da Rosa; Shiori Miyazaki; Haruna Sakamoto; Yuichi Kitagawa; Kiyoshi Miyata; Tomoko Akama; Masato Kobayashi; Koji Fushimi; Ken Onda; Tetsuya Taketsugu; Yasuchika Hasegawa;
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Graduate School of Chemical Sciences and Engineering Hokkaido University;

Department of Chemistry Kyushu University;

Department of Chemistry Kyushu University;

Faculty of Engineering Hokkaido University;

Department of Chemistry Kyushu University;

Faculty of Science Hokkaido University;

Institute for Chemical Reaction Design and Discovery (WPI-ICReDD) Hokkaido University;

Faculty of Engineering Hokkaido University;

Department of Chemistry Kyushu University;

Institute for Chemical Reaction Design and Discovery (WPI-ICReDD) Hokkaido University;

Faculty of Engineering Hokkaido University;

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中图分类物理化学（理论化学）、化学物理学;
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Coordination Geometrical Effect on Ligand-to-Metal Charge Transfer-Dependent Energy Transfer Processes of Luminescent Eu(III) Complexes

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