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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Bidirectional Singlet and Triplet Energy Transfer via the 2-Ureido-4[1H]-pyrimidinone Quadruple Hydrogen-Bonded Module
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Bidirectional Singlet and Triplet Energy Transfer via the 2-Ureido-4[1H]-pyrimidinone Quadruple Hydrogen-Bonded Module

机译：通过2-Ureido-4 [1H]-嘧啶酮四氢键合模块进行双向单重态和三重态能量转移

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摘要

The bidirectional singlet-singlet and triplet-triplet energy transfer processes were observed for the first time within a noncovalent hydrogen-bonded module. For this purpose, 2-ureido-4[1H]-pyrimidinone quadruple hydrogen-bonds (UPy) functionalized BF2-chelated dipyrromethene (BODIPY-UPy) and iodinated BODIPY (I-BODIPY-UPy) were synthesized. These molecules formed energy donor-acceptor assembly through quadruple self-complementary hydrogen bonds, which demonstrated interesting photophysical properties. Spectroscopic studies in toluene solution revealed that selective excitation of BODIPY-UPy in the assembly resulted in efficient intra-assembly singlet energy transfer from excited BODIPY-UPy to I-BODIPY-UPy. This was followed by intersystem crossing of I-BODIPY-UPy from S-1 to T-1 and the backward triplet energy transfer from the I-BODIPY to BODIPY part. Time-resolved transient absorption spectroscopy confirmed that the triplet excited-state energy was distributed on both chromophores in the assembly. Density functional theory (DFT) calculations further validated the feasibility of energy transfer as well as two degenerate triplet states in the assembly. The present studies revealed that the bidirectional singlet-singlet and triplet-triplet energy transfer processes could be manipulated through the noncovalent quadruple hydrogen bonds. Studies on such a process in supramolecular assembly are of considerable importance in the elucidation of their possible function in natural photosystems and inspire applications in various fields such as luminescent materials, optoelectronic devices, photocatalysis, and photodynamic therapy.
机译：在非共价氢键模块中首次观察到双向单重态-单重态和三重态-三重态的能量转移过程。为此目的，合成了2-脲基-4 [1H]-嘧啶酮四氢键（UPy）功能化的BF2-螯合的二吡咯亚甲基（BODIPY-UPy）和碘化的BODIPY（I-BODIPY-UPy）。这些分子通过四重自补氢键形成能量供体-受体组装体，这表明了有趣的光物理性质。在甲苯溶液中的光谱研究表明，装配体中BODIPY-UPy的选择性激发导致装配体内部单线态能量从激发的BODIPY-UPy高效传递到I-BODIPY-UPy。随后是I-BODIPY-UPy从S-1到T-1的系统间交叉，以及从I-BODIPY到BODIPY部分的向后三重态能量转移。时间分辨瞬态吸收光谱法证实三重态激发态能量分布在组件中的两个生色团上。密度泛函理论（DFT）的计算进一步验证了能量转移以及组件中两个简并三重态的可行性。目前的研究表明，双向单重态-单重态和三重态-三重态的能量转移过程可以通过非共价四重氢键进行控制。对超分子组装中这种方法的研究对于阐明其在自然光系统中的可能功能具有重要意义，并激发在各种领域中的应用，例如发光材料，光电器件，光催化和光动力疗法。

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