利用库仑核截断方法对带电分子和表面进行高效周期性密度泛函理论计算
Efficient periodic density functional theory calculations of charged molecules and surfaces using Coulomb kernel truncation
AI总结：
本文通过库仑核截断方法在VASP中实现0D和2D周期性边界条件，并结合高效填充策略消除真空非物理电势，从而高效计算带电分子和表面，并在NaCl表面氯缺陷形成能及金（211）|水界面分子动力学模拟中验证了计算效率。
摘要：
带电分子和表面的密度泛函理论（DFT）计算对于电催化、能源材料及相关材料科学领域的应用至关重要。诸如维也纳从头计算模拟程序包（VASP）等DFT实现是在三维周期性边界条件下计算静电势的，因此必须满足电荷中性条件。在本工作中，我们实现了零维和二维周期性边界条件，以分别便于对带电分子和表面进行DFT计算。我们采用库仑核截断方法来实现这些边界条件。我们的实现通过选择性地减去在三维边界条件下计算所得电势中不想要的长程相互作用，来计算零维和二维边界条件下的电势。通过将库仑核截断方法与计算上高效的填充方法相结合，我们消除了零维和二维体系中来自真空的非物理电势。为了说明我们方法的计算效率，我们对氯化钠（001）表面上带电氯缺陷的形成能进行了大超胞计算，并对阶梯状金（211）|水电极-电解质界面进行了长时间尺度的分子动力学模拟。
英文摘要：
Density functional theory (DFT) calculations of charged molecules and surfaces are critical to applications in electro-catalysis, energy materials and related fields of materials science. DFT implementations such as the Vienna ab-initio Simulation Package (VASP) compute the electrostatic potential under 3D periodic boundary conditions, necessitating charge neutrality. In this work, we implement 0D and 2D periodic boundary conditions to facilitate DFT calculations of charged molecules and surfaces respectively. We implement these boundary conditions using the Coulomb kernel truncation method. Our implementation computes the potential under 0D and 2D boundary conditions by selectively subtracting unwanted long-range interactions in the potential computed under 3D boundary conditions. By combining the Coulomb kernel truncation method with a computationally efficient padding approach, we remove nonphysical potentials from vacuum in 0D and 2D systems. To illustrate the computational efficiency of our method, we perform large supercell calculations of the formation energy of a charged chlorine defect on a sodium chloride (001) surface and perform long time-scale molecular dynamics simulations on a stepped gold (211) | water electrode-electrolyte interface.
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