菲咪唑-硼二吡甲烷供体-受体二价体中的分子内光诱导能量和电子转移反应,The Journal of Physical Chemistry A

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菲咪唑-硼二吡甲烷供体-受体二价体中的分子内光诱导能量和电子转移反应
The Journal of Physical Chemistry A ( IF 2.7 ) Pub Date : 2023-08-04 , DOI: 10.1021/acs.jpca.3c04141
Swathi Nenavath _{1,

2} , Naresh Duvva _{1,

3} , Ram R Kaswan ₄ , Gary N Lim ₄ , Francis D'Souza ₄ , Lingamallu Giribabu _{1,

2}

Affiliation

供体菲咪唑 (PhI) 直接连接到 BODIPY 受体 ( Dyad1 ) 并通过 PhI 和 BODIPY ( Dyad2 )之间的乙炔桥分隔的供体-受体系统已通过各种光谱和电化学技术进行设计、合成和表征。两个二元体与组成个体的光学吸收和^{1 H NMR 特征表明，菲并咪唑和 BODIPY 之间存在最小的 π-π 相互作用。}在所有三种研究的溶剂中，当在苯并咪唑吸收最大值或 BODIPY 吸收最大值激发时，观察到两个二元组的猝灭发射。详细的光谱分析为从菲并咪唑的单重激发态到 BODIPY 的分子内光致激发能量转移（PEnT）和从菲并咪唑的基态到 BODIPY 的光致电子转移（PET）提供了证据。瞬态吸收研究表明，对于二元体Dyad1和 (5.15 ± 0.03 ) × 10 ⁸ s ，电荷分离物质 (PhI ^•+ - BODIPY ^•– ) 的生成速率常数为 (1.16 ± 0.01) × 10 ⁸ s ^–1^–1和Dyad2 ，而Dyad1和Dyad2的能量转移速率常数要高得多，分别约为 (1.1 ± 0.02) × 10 ¹⁰ s ^–1和 (1.6 ± 0.02) × 10 ¹⁰ s ^–1，这意味着它们在光能收集应用中的有用性。

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Intramolecular Photoinduced Energy and Electron Transfer Reactions in Phenanthroimidazole–Boron Dipyromethane Donor–Acceptor Dyads

Donor–acceptor systems in which a donor phenanthroimidazole (PhI) is directly connected to a BODIPY acceptor (Dyad1) and separated by an ethynyl bridge between PhI and BODIPY (Dyad2) have been designed, synthesized, and characterized by various spectroscopic and electrochemical techniques. Optical absorption and ¹H NMR characteristics of both dyads with those of constituent individuals suggest that there exists a minimum π–π interaction between phenanthroimidazole and BODIPY. Quenched emission of both the dyads was observed when excited either at phenthaoimidazole absorption maxima or at BODIPY absorption maxima in all three investigated solvents. The detailed spectral analysis provided evidence for an intramolecular photoinduced excitation energy transfer (PEnT) from the singlet excited state of phenanthroimidazole to BODIPY and photoinduced electron transfer (PET) from the ground state of phenanthroimidazole to BODIPY. Transient absorption studies suggest that charge-separated species (PhI^•+ - BODIPY^•–) are generated at a rate constant of (1.16 ± 0.01) × 10⁸ s^–1 for the dyads Dyad1 and (5.15 ± 0.03) × 10⁸ s^–1 and for Dyad2 whereas energy transfer rate constants were much higher and were on the order of (1.1 ± 0.02) × 10¹⁰ s^–1 and (1.6 ± 0.02) × 10¹⁰ s^–1 for Dyad1 and Dyad2, respectively, signifying their usefulness in light energy harvesting applications.

更新日期：2023-08-04

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