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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Broadband Visible Light-Harvesting Naphthalenediimide (NDI) Triad: Study of the Intra-/Intermolecular Energy/Electron Transfer and the Triplet Excited State
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Broadband Visible Light-Harvesting Naphthalenediimide (NDI) Triad: Study of the Intra-/Intermolecular Energy/Electron Transfer and the Triplet Excited State

机译：宽带可见光收集萘二酰亚胺（NDI）三元组：分子内/分子间能量/电子转移和三重态激发态的研究

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摘要

A triad based on naphthalenediimides (NDI) was prepared to study the intersystem crossing (ISC), the fluorescence-resonance-energy-transfer (FRET), as well as the photoinduced electron transfer (PET) processes. In the triad, the 2-bromo-6-alkylaminoNDI moiety was used as singlet energy donor and the spin converter, whereas 2,6-dialkylaminoNDI was used as the singlet/triplet energy acceptor. This unique structural protocol and thus alignment of the energy levels ensures the competing ISC and FRET in the triad. The photophysical properties of the triad and the reference compounds were studied with steady-state UV-vis. absorption spectra, fluorescence spectra, nanosecond transient absorption spectra, cyclic voltammetry, and DFT/TDDFT calculations. FRET was confirmed with steady-state UV-vis absorption and fluorescence spectroscopy. Intramolecular electron transfer was observed in polar solvents, demonstrated by the quenching of both the fluorescence and triplet state of the energy acceptor. Nanosecond transient absorption spectroscopy shows that the T-1 state of the triad is exclusively localized on the 2,6-dialkylaminoNDI moiety in the triad upon selective photoexcitation into the energy donor, which indicates the intramolecular triplet state energy transfer. The intermolecular triplet state energy transfer between the two reference compounds was investigated with nanosecond transient absorption spectroscopy. The photophysical properties were rationalized by TDDFT calculations.
机译：制备了基于萘二甲酰亚胺（NDI）的三元组，以研究系统间穿越（ISC），荧光共振能量转移（FRET）以及光致电子转移（PET）过程。在三元组中，将2-溴-6-烷基氨基NDI部分用作单线态能量供体和自旋转换器，而将2,6-二烷基氨基NDI用作单线态/三重态能量受体。这种独特的结构方案，从而使能级保持一致，从而确保三联体中相互竞争的ISC和FRET。用稳态紫外可见光谱研究了三单元组和参考化合物的光物理性质。吸收光谱，荧光光谱，纳秒瞬态吸收光谱，循环伏安法和DFT / TDDFT计算。通过稳态紫外可见吸收和荧光光谱法确认了FRET。在极性溶剂中观察到分子内电子转移，这通过能量受体的荧光和三重态的猝灭证明。纳秒瞬态吸收光谱法显示，在选择性光激发进入能量供体中后，三合体的T-1状态仅局限在三合体中的2,6-二烷基氨基NDI部分上，这表明分子内三重态的能量转移。用纳秒瞬态吸收光谱研究了两种参考化合物之间的分子间三重态能量转移。通过TDDFT计算使光物理性质合理化。

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