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Accurate SCC-DFTB Parametrization for Bulk Water.
Journal of Chemical Theory and Computation ( IF 5.7 ) Pub Date : 2020-02-10 , DOI: 10.1021/acs.jctc.9b00816
Maicon Pierre Lourenço 1 , Egon Campos Dos Santos 2, 3 , Lars G M Pettersson 3 , Hélio Anderson Duarte 2
Affiliation  

The SCC-DFTB repulsion parameters based on the material science set (matsci) were redesigned to describe the structure and dynamic properties of bulk liquid water. The iterative Boltzman inversion (IBI) approach was applied by simultaneously correcting the O-H and O-O SCC-DFTB repulsion energy contribution to develop the new water-matsci and water-matsci-UFF set of parameters. The water-matsci parameters provide O-O and O-H radial distribution functions in excellent agreement with available state-of-the-art experimental data. The parametrization is applied to compute binding energies of a set of water clusters with 2-10 molecules and compared to other DFTB parameters and reference data. The self-diffusion coefficients of ambient and supercooled (254 K) water have been estimated and compared to other SCC-DFTB calculated values and experiment. The performance of the new parameters for describing the density of ambient water and reactions involving water dissociation into H3O+ and OH-, the self-diffusion coefficient, and neutralization energy were investigated. Finally, we show that the new parametrization can be reliably applied to adsorption of water on the mineral pyrite by combining the new water-matsci parameters with the available matsci set of parameters for pyrite. This opens opportunities for investigating materials and phenomena of increasing complexity involving water.

中文翻译:

批量水的准确SCC-DFTB参数化。

重新设计了基于材料科学集(matsci)的SCC-DFTB排斥参数,以描述散装液态水的结构和动力学特性。通过同时校正OH和OO SCC-DFTB排斥能的贡献,应用了迭代Boltzman反演(IBI)方法,以开发新的water-matsci和water-matsci-UFF参数集。水质参数提供了OO和OH径向分布函数,与可用的最新实验数据高度吻合。将参数化应用于计算具有2-10个分子的一组水簇的结合能,并将其与其他DFTB参数和参考数据进行比较。已估算了环境和过冷(254 K)水的自扩散系数,并将其与其他SCC-DFTB计算值和实验进行了比较。研究了用于描述环境水密度和涉及水分解成H3O +和OH-的反应,自扩散系数和中和能的新参数的性能。最后,我们表明,通过将新的水-物性参数与黄铁矿的可用物性参数集相结合,可以将新的参数化可靠地应用于水在矿物黄铁矿上的吸附。这为研究材料和涉及水的复杂性增加的现象提供了机会。我们表明,通过将新的水-物性参数与黄铁矿的可用物性参数集相结合,可以将新的参数化可靠地应用于水在矿物黄铁矿上的吸附。这为研究材料和涉及水的复杂性增加的现象提供了机会。我们表明,通过将新的水-物性参数与黄铁矿的可用物性参数集相结合,可以将新的参数化可靠地应用于水在矿物黄铁矿上的吸附。这为研究材料和涉及水的复杂性增加的现象提供了机会。
更新日期:2020-02-23
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