On the proton transfer mechanism in ammonia-bridged 7-hydroxyquinoline: a TDDFT molecular dynamics study.
On the proton transfer mechanism in ammonia-bridged 7-hydroxyquinoline: a TDDFT molecular dynamics study.
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DOI：
10.1039/b903136g
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发表时间：
2009-05
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影响因子：
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通讯作者：
M. Guglielmi;I. Tavernelli;U. Rothlisberger
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文献类型：
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作者：
M. Guglielmi;I. Tavernelli;U. Rothlisberger
本文研究了7-羟基喹啉最低光激发态的质子转移机理。（NH3）3使用TDDFT为基础的分子动力学。我们观察到一个协调一致的机制，根据该机制，所有质子同时转移在一个快速的过程（约100 fs），相当于一个质子从氧到氮的7-羟基喹啉的净运输。此外，观察到的质子转移途径涉及所有三个氨分子，而不是之前提出的只有两个。这些差异来自于有限温度下发生的动力学效应。我们的模拟提供了一个详细的时间分辨的质子转移反应机制的一个原型分子簇的描述，从而有助于进一步阐明这个重要的和普遍存在的过程的性质。
We have investigated the mechanism of proton transfer in the lowest photoexcited state of 7-hydroxyquinoline.(NH3)3 using TDDFT based molecular dynamics. We observe a concerted mechanism according to which all protons are transferred simultaneously in a fast process (approximately 100 fs) that amounts to the net transport of one proton from the oxygen to the nitrogen of 7-hydroxyquinoline. In addition, the observed proton transfer pathway involves all three ammonia molecules and not only two as previously proposed. These differences arise from dynamical effects that occur at finite temperature. Our simulations provide a detailed time-resolved description of the proton transfer reaction mechanism for a prototypical molecular cluster and thus help to shed further light on the nature of this important and ubiquitous process.