Ribeiro Mauro C C
Laboratório de Espectroscopia Molecular, Instituto de Química, Universidade de São Paulo, C.P. 26077, CEP 05513-970, São Paulo, SP, Brazil.
J Phys Chem B. 2006 May 4;110(17):8789-97. doi: 10.1021/jp060518a.
A previously proposed model for molecular dynamics (MD) simulation of liquid sulfur dioxide, SO(2), has been reviewed. Thermodynamic, structural, and dynamical properties were calculated for a large range of thermodynamic states. Predicted (P,V,T) of simulated system agrees with an elaborated equation of state recently proposed for liquid SO(2). Calculated heat capacity, expansion coefficient, and isothermal compressibility are also in good agreement with experimental data. Calculated equilibrium structure agrees with X-ray and neutron scattering measurements on liquid SO(2). The model also predicts the same (SO(2))(2) dimer structure as previously determined by ab initio calculations. Detailed analysis of equilibrium structure of liquid SO(2) is provided, indicating that, despite the rather large dipole moment of the SO(2) molecule, the structure is mainly determined by the Lennard-Jones interactions. Both single-particle and collective dynamics are investigated. Temperature dependency of dynamical properties is given. The MD results are compared with previous findings obtained from the analysis of inelastic neutron scattering spectra of liquid SO(2), including wave-vector dependent structural relaxation, tau(k), and viscosity, eta(k).
之前提出的用于液态二氧化硫（SO₂）分子动力学（MD）模拟的模型已被综述。针对大范围的热力学状态计算了热力学、结构和动力学性质。模拟系统的预测（P，V，T）与最近提出的用于液态SO₂的精细状态方程相符。计算得到的热容、膨胀系数和等温压缩率也与实验数据高度吻合。计算得到的平衡结构与液态SO₂的X射线和中子散射测量结果一致。该模型还预测了与之前通过从头算确定的相同的（SO₂）₂二聚体结构。提供了对液态SO₂平衡结构的详细分析，表明尽管SO₂分子的偶极矩相当大，但结构主要由 Lennard-Jones 相互作用决定。研究了单粒子动力学和集体动力学。给出了动力学性质的温度依赖性。将MD结果与之前通过分析液态SO₂的非弹性中子散射光谱获得的结果进行了比较，包括与波矢相关的结构弛豫时间τ(k)和粘度η(k)。
