中国科学院机构知识库网格
Chinese Academy of Sciences Institutional Repositories Grid
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; Weifeng Bu,1,2,4; Zhou F(周峰)1,3
刊名The Journal of Chemical Physics
出版日期2024-07-14
期号161页码:054103
DOI10.1063/5.0222514
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.

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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
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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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