论文标题
使用环聚合物分子动力学的漫游反应H + MGH的速率系数
Rate coefficients of a roaming reaction H + MgH using the ring polymer molecular dynamics
论文作者
论文摘要
使用环聚合物分子动力学（RPMD）来计算两通道漫游反应H + MGH的热速率系数。明确考虑了两个紧密和漫游的反应通道。这是将RPMD方法用于多通道反应的开创性尝试。借助新开发的优化交互协议，以准备选择力常数的初始结构和自适应方案，我们成功地获得了热速率系数。结果与其他理论方法的结果一致，例如变化过渡状态理论（VTST）和量子动力学（QD）。特别是，RPMD结果表现出负温度依赖性，这与VTST的结果相似，但与基态QD计算的结果不同。
The ring-polymer molecular dynamics (RPMD) was used to calculate the thermal rate coefficients of the two-channel roaming reaction H + MgH. Both reaction channels, tight and roaming, are explicitly considered. This is a pioneering attempt of exerting RPMD method to multi-channel reactions. With the help of a newly developed optimization-interpolation protocol for preparing the initial structures and adaptive protocol for choosing the force constants, we have successfully obtained the thermal rate coefficients. The results are consistent with those from other theoretical methods, such as variational transition state theory (VTST) and quantum dynamics (QD). Especially, RPMD results exhibit negative temperature dependence, which is similar to results from VTST but different from ones from ground state QD calculations.
