Lifetime Broadening and Impulsive Generation of Vibrational Coherence Triggered by Ultrafast Electron Transfer,The Journal of Physical Chemistry Letters

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Lifetime Broadening and Impulsive Generation of Vibrational Coherence Triggered by Ultrafast Electron Transfer
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2021-01-20 , DOI: 10.1021/acs.jpclett.0c03641
Alexander Aster ₁ , Anna-Bea Bornhof ₂ , Naomi Sakai ₂ , Stefan Matile ₂ , Eric Vauthey ₁

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The absorption band shape of chromophores in liquid solution at room temperature is usually dominated by pure electronic dephasing dynamics, which occurs on the sub-100 fs time scale. Herein, we report on a series of dyads consisting of a naphthalenediimide (NDI) electron acceptor with one or two phenyl-based donors for which photoinduced intramolecular electron transfer is fast enough to be competitive with pure electronic dephasing. As a consequence, the absorption band of the π–π* transition of these dyads is broader than that of the NDI alone to an extent that scales with the electron transfer rate. Additionally, this reaction is so fast that it leads to the impulsive excitation of a low-frequency vibrational mode of the charge-separated product. Quantum-chemical calculations suggest that this vibration involves the C–N donor–acceptor bond, which shortens considerably upon electron transfer.

中文翻译：

超快电子转移触发的振动相干的终身扩展和脉冲生成

室温下发色团在液体溶液中的吸收带形状通常由纯电子移相动力学决定，该动力学发生在低于100 fs的时间范围内。本文中，我们报道了一系列由萘二酰亚胺（NDI）电子受体与一个或两个基于苯基的供体组成的二元组，其光诱导分子内电子转移足够快，足以与纯电子移相竞争。结果，这些二重体的π–π *跃迁的吸收带比单独的NDI吸收带更宽，其吸收带与电子传输速率成比例。另外，该反应非常快，以至于导致电荷分离产物的低频振动模式的脉冲激发。量子化学计算表明，这种振动涉及C–N供体-受体键，

更新日期：2021-01-28

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