Adaptive accelerated reactive molecular dynamics driven by parallel collective variables overcoming dimensionality explosion.
文献类型:期刊论文
作者 | Zhou R(周锐)1,2,3,4; Bao LY(鲍路瑶)1,3![]() ![]() |
刊名 | The Journal of Chemical Physics
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出版日期 | 2024-07-14 |
期号 | 161页码:054103 |
DOI | 10.1063/5.0222514 |
英文摘要 | ReaxFF reactive molecular dynamics has significantly advanced the exploration of chemical reaction mechanisms in complex systems. How ever, it faces several challenges: (1) the prevalent use of excessively high temperatures (>2000 K), (2) a time scale considerably shorter than the experimental timeframes (nanoseconds vs seconds), and (3) the constraining impact of dimensionality growth due to collective variables on the expansiveness of research systems. To overcome these issues, we introduced Parallel Collective Variable-Driven Adaptive Accelerated Reaction Molecular Dynamics (PCVR), which integrates metadynamics with ReaxFF. This method incorporates bond distortion based on each bond type for customized Collective Variable (CV) parameterization, facilitating independent parallel acceleration. Simultaneously, the sampling was confined to fixed cutoff ranges for distinct bond distortions, effectively overcoming the challenge of the CV dimensionality explosion. This extension enhances the applicability of ReaxFF to non-strongly coupled systems with numerous reaction energy barriers and mitigates the system size limitations. Using accelerated reactive molecular dynamics, the oxidation of ester-based oil was simulated with 31 808 atoms at 500 K for 64 s. This achieved 61% efficiency compared to the original ReaxFF and was ∼37 times faster than previous methods. Unlike ReaxFF’s high-temperature constraints, PCVR accurately reveals the pivotal role of oxygen in ester oxidation at industrial temperatures, pro ducing polymers consistent with the sludge formation observed in ester degradation experiments. This method promises to advance reactive molecular dynamics by enabling simulations at lower temperatures, extending to second-level timescales, and accommodating systems with millions of atoms. |
URL标识 | 查看原文 |
语种 | 英语 |
源URL | [http://ir.licp.cn/handle/362003/31138] ![]() |
专题 | 兰州化学物理研究所_固体润滑国家重点实验室 |
通讯作者 | Zhou R(周锐); Weifeng Bu,; Zhou F(周峰) |
作者单位 | 1.中国科学院兰州化学物理研究所 2.兰州大学 3.烟台先进材料与绿色制造山东省实验室 4.中国科学院大学 |
推荐引用方式 GB/T 7714 | Zhou R,Bao LY,Weifeng Bu,,et al. Adaptive accelerated reactive molecular dynamics driven by parallel collective variables overcoming dimensionality explosion.[J]. The Journal of Chemical Physics,2024(161):054103. |
APA | Zhou R,Bao LY,Weifeng Bu,,&Zhou F.(2024).Adaptive accelerated reactive molecular dynamics driven by parallel collective variables overcoming dimensionality explosion..The Journal of Chemical Physics(161),054103. |
MLA | Zhou R,et al."Adaptive accelerated reactive molecular dynamics driven by parallel collective variables overcoming dimensionality explosion.".The Journal of Chemical Physics .161(2024):054103. |
入库方式: OAI收割
来源:兰州化学物理研究所
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