Comparison between Gaussian-type orbitals and plane wave ab initio density functional theory modeling of layer silicates: talc [Mg3Si4O10(OH)2] as model system.
Comparison between Gaussian-type orbitals and plane wave ab initio density functional theory modeling of layer silicates: talc [Mg3Si4O10(OH)2] as model system.
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DOI：
10.1063/1.4830405
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发表时间：
2013-11
期刊：
影响因子：
--
通讯作者：
G. Ulian;S. Tosoni;G. Valdrè
中科院分区：
文献类型：
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作者：
G. Ulian;S. Tosoni;G. Valdrè
固态系统的量子化学表征有多种不同的方法，其中采用周期性边界条件来处理三维无限凝聚系统。该方法与密度泛函理论 (DFT) 相结合，已被证明可以成功模拟各种固体。直到最近几年，这种从头算的量子力学方法才被用于层状硅酸盐结构和矿物的研究。在目前的工作中，系统比较了不同的 DFT 泛函（GGA-PBEsol 和混合 B3LYP）和基组（平面波和全电子高斯型轨道）对模型层硅酸盐滑石 [Mg3Si4O10(OH)2] 的几何、能量和声子特性的影响。 DFT+D方法考虑了长程色散。结果与文献报道的实验数据一致，GTO∕B3LYP-D* 方法给出的关于轴向晶格参数和相互作用能的偏差最小，PW/PBE-D 给出的晶胞体积和角度值的偏差最小。所有考虑的方法都充分描述了实验滑石粉红外光谱。
The quantum chemical characterization of solid state systems is conducted with many different approaches, among which the adoption of periodic boundary conditions to deal with three-dimensional infinite condensed systems. This method, coupled to the Density Functional Theory (DFT), has been proved successful in simulating a huge variety of solids. Only in relatively recent years this ab initio quantum-mechanic approach has been used for the investigation of layer silicate structures and minerals. In the present work, a systematic comparison of different DFT functionals (GGA-PBEsol and hybrid B3LYP) and basis sets (plane waves and all-electron Gaussian-type orbitals) on the geometry, energy, and phonon properties of a model layer silicate, talc [Mg3Si4O10(OH)2], is presented. Long range dispersion is taken into account by DFT+D method. Results are in agreement with experimental data reported in literature, with minimal deviation given by the GTO∕B3LYP-D* method regarding both axial lattice parameters and interaction energy and by PW/PBE-D for the unit-cell volume and angular values. All the considered methods adequately describe the experimental talc infrared spectrum.