氮笼形水合物中笼形占位的蒙特卡罗模拟
Cage occupancies in nitrogen clathrate hydrates from Monte Carlo simulations
摘要：
将吉布斯系综蒙特卡罗模拟与N2笼形水合物中笼占据率的实验数据进行比较，以评估此类模拟的准确性，改进所采用的有效势，并帮助解释最近测量的大笼相对于小笼占据率的比率[Petuya等人，J. Phys. Chem. C 122，566（2018）]。考虑了N2-N2、N2-H2O和H2O-H2O相互作用的不同相互作用势。其中一些未能再现已知的实验事实，即一些大笼在273 K和高压下被双重占据。当使用一个新的N-O相互作用势在这项工作中获得的平均从头计算势能面的N2-H2O二聚体的模拟和实验之间的最佳协议。
英文摘要：
Comparisons of Gibbs ensemble Monte Carlo simulations with experimental data for the cage occupancies in N2 clathrate hydrates are performed to assess the accuracy of such simulations, to refine the effective potentials employed, and to help interpret recently measured large cage over small cage occupancy ratios [Petuya et al., J. Phys. Chem. C 122, 566 (2018)]. Different sets of interaction potentials for N2-N2, N2-H2O and H2O-H2O interactions are considered. Some of them fail to reproduce the known experimental fact that some large cages are doubly occupied at 273 K and high pressures. The best agreement between simulations and experiments is obtained when using a new N-O interaction potential derived in this work by averaging an ab-initio potential energy surface for the N2-H2O dimer.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
