Abstract This paper compares ReaxFF, SPC/E, TIP4P/2005 and TIP4P/Ice with Density Functional Theory (DFT) to identify which one should be used to model both the microstructures and mechanical properties of large size hexagonal Ice (Ih) over a long time scale (~10−9–10−6 s). According to the model performances with regards to determining the microstructure, surface energy and fracture toughness, the limitations and validities of ReaxFF and the three other potential models are discussed. It is found that hydrogen bond density determines the surface energy on the same surface. TIP4P/Ice has the smallest error and the ReaxFF force field has the largest error, up to 27.21% for the aforementioned quantities. If only modeling the microstructure of ice Ih, TIP4P/2005 and SPC/E are the most suitable water models. Moreover, the secondary prism face 11 2 ¯ 0 , with the lowest hydrogen bond density and fracture toughness, is the first cleavage plane of ice Ih. The primary prism face 1 ¯ 100 is the second cleavage plane, as shown by the surface energy and fracture toughness results of DFT and molecular dynamics (MD).

中文翻译：

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ReaxFF 和势模型与密度泛函理论模拟六边形冰的比较研究

摘要 本文将 ReaxFF、SPC/E、TIP4P/2005 和 TIP4P/Ice 与密度泛函理论 (DFT) 进行了比较，以确定应该使用哪一种来模拟大尺寸六边形冰 (Ih) 的微观结构和机械性能。时间尺度（~10−9–10−6 s）。根据模型在确定微观结构、表面能和断裂韧性方面的性能，讨论了 ReaxFF 和其他三个潜在模型的局限性和有效性。发现氢键密度决定了同一表面的表面能。TIP4P/Ice 的误差最小，ReaxFF 力场的误差最大，上述量的误差高达 27.21%。如果仅模拟冰 Ih 的微观结构，TIP4P/2005 和 SPC/E 是最合适的水模型。而且，次棱面 11 2¯ 0 具有最低的氢键密度和断裂韧性，是冰 Ih 的第一解理面。主棱面 1~100 是第二解理面，如 DFT 和分子动力学 (MD) 的表面能和断裂韧性结果所示。