ABEEM浮动电荷分子力场在含离子体系中的发展和应用

离子水合及生物分子体系内离子选择性的微观作用机制是人们长期探索的重要课题,其难点在于如何合理精确地描述上述体系内的离子-水、离子-生物分子等各种相互作用.本文主要总结近年来原子-键电负性均衡浮动电荷分子力场（ABEEM/MM）在含离子体系中的发展和应用,包括离子水溶液、金属蛋白、离子-核酸碱基体系的研究.我们优选相关参数,构建上述体系的势能函数,并对气相水合离子团簇、离子水溶液、金属蛋白、离子-核酸碱基体系进行研究,模拟其结构、活性、热力学和动力学等性质.研究和比较结果表明,我们的ABEEM浮动电荷力场总体上优于其它力场方法,其精度可达到或接近高水平从头计算MP2方法.这为进一步探讨生物分子体系内的离子选择性、金属酶及其它含离子体系的结构和性质奠定了基础.

Development and applications of the ABEEM fluctuating charge molecular force field in the ion-containing systems

The microscopic mechanisms of ion hydration and ion selectivity in biomolecular systems are prolonged research topics, in which the difficulty is how to reasonably and accurately describe the interactions of ion-water, ion-biomolecule, etc. In this paper, the development and applications of the atom-bond electronegativity equalization fluctuating charge force field model, ABEEM/MM in the investigations of ion hydration, metalloproteins and ion-DNA bases systems were summarized. Based on high-level quantum chemistry calculations, the parameters were optimized and then the molecular potential functions were constructed and applied to studies of structures, activities, energetics and thermodynamic and kinetic properties of these ion-containing systems. The results show that the performance of ABEEM/MM is generally better than the common popular force fields, and its accuracy can achieve or approach those of the high-level ab initio MP2 method. These studies provide a solid basis for further investigations of ion selectivity in biomolecular systems, the structures and properties of metalloproteins and other related ion-containing systems.