使用PBE0精度机器学习潜力的分子动力学模拟的CO2-I/III相图
Benkun Hong1, Guoao Li1, Pei Liu1
1State Key Laboratory of Coordination Chemistry, Key Laboratory of Mesoscopic Chemistry of Ministry of Education, New Cornerstone Science Laboratory, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210093, China.
The Journal of chemical physics
|October 1, 2025
概括
我们开发了一种机器学习潜力,用于绘制二氧化碳 (CO2) 晶相图,揭示了CO2-III的新Cmca结构,并表明它与CO2-VII相同.
科学领域:
- 计算材料科学 计算材料科学
- 化学物理 化学物理
- 固态化学 固态化学
背景情况:
- 了解二氧化碳 (CO2) 的相位图对于各种科学和工业应用至关重要.
- 之前的研究报告了不同的二氧化碳晶体结构和过渡压力,导致相位识别的模两可.
- 准确的二氧化碳相变的理论建模需要高准确度的潜能和高效的模拟方法.
研究的目的:
- 使用 PBE0-D3 ((BJ) / aug-cc-pVDZ 理论水平,构建一个高度准确的二氧化碳 (CO2) 机器学习潜力 (MLP).
- 在广泛的温度和压力范围内研究CO2分子晶相图.
- 阐明过渡机制,并为CO2-III阶段提出一个最终的结构.
主要方法:
- 采用PBC-GEBF-AL工作流程,将主动学习 (AL) 与周期边界条件下的基于能源的一般化碎片化方法 (PBC-GEBF) 整合在一起.
- 利用多TPU-OPES增强采样进行分子动力学模拟,达到高达170 ns的轨迹长度.
- 产生了一种机器学习潜力 (MLP),准确度为PBE0-D3{\displaystyle PBE0-D3{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}{\displaystyle PBE0-D3}}
主要成果:
- 从250-700 K和10.5-14.0 GPa获得了CO2相位图,确定了一个CO2-I/III共存线,峰值在~12.3 GPa和525 K.
- 揭示了一种协调的CO2-I/III过渡机制,涉及分子旋转,晶格变形和非单调的体积变化.
- 为CO2-III提出了一个新的Cmca空间组结构,其特点是倾斜的分子和a > b格子参数,非常类似CO2-VII.
结论:
- 拟议的CO2-III倾斜的Cmca结构表明它可能与CO2-VII相同的相位,实验中的差异归因于热效应.
- 该研究提供了对二氧化碳相变和不同晶体结构的共存更深入的见解.
- 为复杂的罕见事件系统开发高精度MLP制定了可通用策略.
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