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Excited State Molecular Dynamics of Photoinduced Proton-Coupled Electron Transfer in Anthracene-Phenol-Pyridine Triads.
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-08-05 , DOI: 10.1021/acs.jpclett.0c02012 Elvira R Sayfutyarova 1 , Sharon Hammes-Schiffer 1
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2020-08-05 , DOI: 10.1021/acs.jpclett.0c02012 Elvira R Sayfutyarova 1 , Sharon Hammes-Schiffer 1
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Photoinduced proton-coupled electron transfer (PCET) in anthracene–phenol–pyridine triads exhibits inverted region behavior, where the more thermodynamically favorable process is slower. The long-lived transient charge-separated state (CSS) associated with electron transfer from phenol to anthracene and inverted region behavior were only observed experimentally for certain triads. Herein, excited state molecular dynamics simulations were performed on four different triads to simulate the nonequilibrium dynamics following photoexcitation to the locally excited state (LES) of anthracene. These simulations identified two distinct PCET pathways: the triads exhibiting inverted region behavior transitioned from the LES to the CSS, whereas the other triads transitioned to a local electron–proton transfer (LEPT) state within phenol and pyridine. The simulations suggest that PCET to the LEPT state is slower than PCET to the CSS and provides an alternative relaxation pathway. The mechanistic pathways, as well as the time scales of the electron and proton transfers, can be controlled by tuning the substituents.
中文翻译：
蒽-苯酚-吡啶三联体中光诱导质子偶联电子转移的激发态分子动力学。
蒽-苯酚-吡啶三联体中的光诱导质子偶联电子转移（PCET）表现出反向区域行为，其中热力学更有利的过程较慢。仅从某些三元组实验观察到与从苯酚到蒽的电子转移和反向区域行为相关的长寿命瞬态电荷分离状态（CSS）。本文中，对四个不同的三单元组进行了激发态分子动力学模拟，以模拟光激发蒽的局部激发态（LES）后的非平衡动力学。这些模拟确定了两种不同的PCET途径：三元组显示出从LES到CSS的反向区域行为转变，而其他三元组在苯酚和吡啶内转变为局部电子-质子转移（LEPT）状态。模拟表明，PCET到LEPT状态比PCET到CSS慢，并且提供了另一种松弛路径。可以通过调节取代基来控制机械途径以及电子和质子转移的时间尺度。
更新日期：2020-09-03
中文翻译：
蒽-苯酚-吡啶三联体中光诱导质子偶联电子转移的激发态分子动力学。
蒽-苯酚-吡啶三联体中的光诱导质子偶联电子转移（PCET）表现出反向区域行为，其中热力学更有利的过程较慢。仅从某些三元组实验观察到与从苯酚到蒽的电子转移和反向区域行为相关的长寿命瞬态电荷分离状态（CSS）。本文中，对四个不同的三单元组进行了激发态分子动力学模拟，以模拟光激发蒽的局部激发态（LES）后的非平衡动力学。这些模拟确定了两种不同的PCET途径：三元组显示出从LES到CSS的反向区域行为转变，而其他三元组在苯酚和吡啶内转变为局部电子-质子转移（LEPT）状态。模拟表明，PCET到LEPT状态比PCET到CSS慢，并且提供了另一种松弛路径。可以通过调节取代基来控制机械途径以及电子和质子转移的时间尺度。
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