Multiply Accelerated ReaxFF Molecular Dynamics: Coupling Parallel Replica Dynamics with Collective Variable Hyper Dynamics
Multiply Accelerated ReaxFF Molecular Dynamics: Coupling Parallel Replica Dynamics with Collective Variable Hyper Dynamics
复制标题
乘法加速 ReaxFF 分子动力学：将并行复制动力学与集体变量超动力学耦合
DOI：
10.1080/08927022.2019.1646911
复制
发表时间：
2019
影响因子：
2.1
通讯作者：
Ganeshan, Karthik
Hossain
中科院分区：
文献类型：
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作者：
Ganeshan, Karthik
Hossain
为了解决研究复杂化学反应所需的时间尺度，即使在高性能计算方面取得了最新进展，执行加速分子动力学的方法也是必要的。许多不同的加速技术是可用的。在这里，我们通过分析正十二烷热解获得的加速，探讨了两种流行的加速方法——平行复制动力学（PRD）和集体变量超动力学（CVHD）之间的潜在协同作用。我们观察到PRD + CVHD通过在更早的壁钟时间达到反应所需的时间尺度，为CVHD提供了额外的加速。虽然额外的副本可以获得一些加速，但我们发现，在CVHD诱导的反应速率急剧增加的系统中，包含PRD的有效性降低了。在碳酸乙烯/锂体系的模拟中也得到了类似的观察结果，该体系本身比热解反应性更强，表明通过两种加速方法的组合获得的加速可以推广到大多数实际的化学体系。
To tackle the time scales required to study complex chemical reactions, methods performing accelerated molecular dynamics are necessary even with the recent advancement in high-performance computing. A number of different acceleration techniques are available. Here we explore potential synergies between two popular acceleration methods – Parallel Replica Dynamics (PRD) and Collective Variable Hyperdynamics (CVHD), by analysing the speedup obtained for the pyrolysis of n-dodecane. We observe that PRD + CVHD provides additional speedup to CVHD by reaching the required time scales for the reaction at an earlier wall-clock time. Although some speedup is obtained with the additional replicas, we found that the effectiveness of the inclusion of PRD is depreciated for systems where there is a dramatic increase in reaction rates induced by CVHD. Similar observations were made in the simulation of ethylene-carbonate/Li system, which is inherently more reactive than pyrolysis, indicate that the speedup obtained via the combination of the two acceleration methods can be generalised to most practical chemical systems.