在来自分子模拟的中度超冷时均的冰核形成
1Departamento de Química Física, Facultad de Ciencias Químicas, Universidad Complutense de Madrid , 28040 Madrid, Spain.
Journal of the American Chemical Society
|September 10, 2013
概括
这项研究使用计算机模拟来探索水中的均质冰核形成. 结果表明,在化下20K以上,水结必须是异质的,而不是同质的.
科学领域:
- 物理 物理学 物理
- 化学 化学 化学
- 地质地质地质地质地质地
背景情况:
- 水结成冰是跨越多个科学学科的关键转变.
- 了解同质冰核是解释自然结现象的关键.
研究的目的:
- 通过计算机模拟来研究水中均质冰核的形成.
- 在各种零度以下温度下确定关键集群大小和核化速率.
主要方法:
- 使用TIP4P/2005和TIP4P/冰水模型进行模拟.
- 运用古典核化理论 (CNT) 来分析自由能源障碍.
- 在核化屏障的顶部模拟了关键集群.
主要成果:
- 临界大小从~8000个分子 (4纳米) 减少到~600个分子 (1.7纳米),因为温度从化点以下的15K降至35K.
- 计算的冰水界面自由能量为29(3) mN/m,与实验数据一致.
- 模拟的核化速率与实验测量结果一致,特别是在较低的温度下.
结论:
- 在低于融化的20K以上的温度下,均的冰核形成速度变得极其缓慢.
- 预测所有温度值以上的水结都必须通过异质核化发生.
- 这些发现使模拟结果与对水结行为的实验观测结果相协调.
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