Vendrell Oriol, Meyer Hans-Dieter
Theoretische Chemie, Physikalisch-Chemisches Institut, Universität Heidelberg, INF 229, D-69120 Heidelberg, Germany.
J Chem Phys. 2005 Mar 8;122(10):104505. doi: 10.1063/1.1859274.
Proton transfer along a chain of water molecules is discussed. A linear model for such a chain is developed and its parameters are determined by comparison to quantum chemistry calculations. Fully quantum mechanical dynamical simulations on the translocation process are performed for different chain lengths, with up to five water molecules. We found that tunneling is important for the proton-transfer process. Furthermore, translocation is accomplished through a strongly correlated motion involving both hydrogen and oxygen atoms. An approximate treatment, which limits or even neglects this correlation, may lead to severely incorrect results.
讨论了质子沿水分子链的转移。建立了这样一条链的线性模型，并通过与量子化学计算结果进行比较来确定其参数。针对不同链长（最多包含五个水分子）的转移过程进行了全量子力学动力学模拟。我们发现隧穿对于质子转移过程很重要。此外，转移是通过涉及氢原子和氧原子的强关联运动来完成的。一种限制甚至忽略这种关联的近似处理可能会导致严重错误的结果。
