论文标题
胞嘧啶的电子附件：水的作用
Electron attachment to Cytosine: The Role of Water
论文作者
论文摘要
我们提出了基于EOM-CCSD的QM/MM研究，该研究对在水中溶剂化的电子附着过程进行了电子附着过程。微水合研究无法捕获大量水环境对电子附着过程的影响，并且需要在计算中包括大量水分子以获得融合结果。散装溶剂化胞嘧啶中的电子附件发生在门口机构中，初始电子位于水上。电子随后通过在超快时间尺度上的电子和核自由度混合而转移到胞嘧啶。大量的水环境通过广泛的氢键网络稳定了胞嘧啶结合的阴离子，并通过在气相观察到的歧管提高了电子传递速率。从我们的QM/mm计算获得的预测的绝热电子亲和力和电子传递率与可用的实验结果一致。
We present an EOM-CCSD based QM/MM study on the electron attachment process to cytosine, solvated in water. The microhydration studies cannot capture the effect of bulk water environment on the electron attachment process and one need to include large number of water molecules in the calculation to get converged results. The electron attachment in the bulk solvated cytosine happened through a doorway mechanism, where the initial electron is localized on water. The electron subsequently gets transferred to cytosine by mixing of electronic and nuclear degrees of freedom which happens at an ultrafast time scale. The bulk water environment stabilizes the cytosine bound anion by an extensive hydrogen-bonding network and enhances the electron transfer rate by manifold from that observed in the gas phase. The predicted adiabatic electron affinity and electron transfer rate obtained from our QM/MM calculations are consistent with the available experimental results.
