基于Daubechies小波的约束密度泛函理论计算的片段方法
Fragment Approach to Constrained Density Functional Theory Calculations using Daubechies Wavelets
摘要：
在最近的一篇论文中，我们提出了一个线性标度Kohn-Sham密度泛函理论（DFT）代码的基础上Daubechies小波，其中最小的一组本地化的支持函数在原位优化，因此适应的分子系统的化学性质。由于基本基组的系统可控精度，这种方法能够为给定的系统提供最佳的收缩基：基态能量和原子力的精度与非收缩的立方标度方法具有相同的质量。通过构造，该基组提供了系统的密度矩阵可以被投影的自然子集。在本文中，我们证明了这种最小的基础形式主义的灵活性，提供了一个基础集，可以重复使用的是，即没有重新优化，在一个片段的方法内的电荷约束的DFT计算。支持功能，表示在底层小波网格中，模板片段的旋转平移具有高数值精度的所需的位置，并用作投影仪的电荷权重函数。我们证明了这种方法的兴趣，以表达高精度和高效率的计算准备非绝热状态和复杂环境中的系统的计算设置。
英文摘要：
In a recent paper we presented a linear scaling Kohn-Sham density functional theory (DFT) code based on Daubechies wavelets, where a minimal set of localized support functions is optimized in situ and therefore adapted to the chemical properties of the molecular system. Thanks to the systematically controllable accuracy of the underlying basis set, this approach is able to provide an optimal contracted basis for a given system: accuracies for ground state energies and atomic forces are of the same quality as an uncontracted, cubic scaling approach. This basis set offers, by construction, a natural subset where the density matrix of the system can be projected. In this paper we demonstrate the flexibility of this minimal basis formalism in providing a basis set that can be reused as-is, i.e. without reoptimization, for charge-constrained DFT calculations within a fragment approach. Support functions, represented in the underlying wavelet grid, of the template fragments are roto-translated with high numerical precision to the required positions and used as projectors for the charge weight function. We demonstrate the interest of this approach to express highly precise and efficient calculations for preparing diabatic states and for the computational setup of systems in complex environments.
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