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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Ultrafast intramolecular charge transfer of formyl perylene observed using femtosecond transient absorption spectroscopy
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Ultrafast intramolecular charge transfer of formyl perylene observed using femtosecond transient absorption spectroscopy

机译：飞秒瞬态吸收光谱法观察甲酰per的超快分子内电荷转移

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摘要

The excited-state photophysics of formylperylene (FPe) have been investigated in a series of nonpolar, polar aprotic, and polar protic solvents. A variety of experimental and theoretical methods were employed including femtosecond transient absorption (fs-TA) spectroscopy with 130 fs temporal resolution. We report that the ultrafast intramolecular charge transfer from the perylene unit to the formyl (CHO) group can be facilitated drastically by hydrogen-bonding interactions between the carbonyl group oxygen of FPe and hydrogen-donating solvents in the electronically excited state. The excited-state absorption of FPe in methanol (MeOH) is close to the reported perylene radical cation produced by bimolecular quenching by an electron acceptor. This is a strong indication for a substantial charge transfer in the S_1 state in protic solvents. The larger increase of the dipole moment change in the protic solvents than that in aprotic ones strongly supports this observation. Relaxation mechanisms including vibrational cooling and solvation coupled to the charge-transfer state are also discussed.
机译：甲酰基per（FPe）的激发态光物理性质已在一系列非极性，非质子惰性和质子惰性溶剂中进行了研究。采用了各种实验和理论方法，包括飞秒瞬态吸收（fs-TA）光谱法，时间分辨率为130 fs。我们报告说，从Pe单元到甲酰基（CHO）基团的超快分子内电荷转移可以通过FPe的羰基氧与供氢溶剂在电子激发态之间的氢键相互作用而大大促进。 FPe在甲醇（MeOH）中的激发态吸收接近所报道的通过电子受体进行双分子淬灭而生成的per自由基阳离子。这强烈表明在质子溶剂中处于S_1状态时大量电荷转移。质子传递溶剂中偶极矩变化的增加幅度大于非质子传递溶剂中偶极矩变化的幅度，强烈支持了这一观察结果。还讨论了包括振动冷却和与电荷转移状态耦合的溶剂化的弛豫机制。

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