Auxiliary Density Matrix Methods for Hartree-Fock Exchange Calculations
Auxiliary Density Matrix Methods for Hartree-Fock Exchange Calculations
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DOI：
10.1021/ct1002225
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发表时间：
2010-08-01
影响因子：
5.5
通讯作者：
VandeVondele, Joost
中科院分区：
文献类型：
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作者：
Guidon, Manuel;Hutter, Jurg;VandeVondele, Joost
Hartree-Fock交换（HFX）的计算对于用高质量基组描述的大型系统是计算上要求很高的。在这项工作中，我们表明，仍然可以获得优异的性能和良好的精度，如果采用辅助密度矩阵的HFX计算几个方案，以获得一个辅助密度矩阵从一个高品质的密度矩阵进行了讨论的辅助密度矩阵方法（ADMM）的准确性的关键是使用一个校正的基础上标准的广义梯度近似HFX。ADMM无缝集成在现有的HFX代码，特别是，可以采用线性缩放实现。为了证明该方法的性能，使用64个分子的系统的Born-Oppenheimer分子动力学模拟（300 ps）详细研究了HFX对液态水结构的影响。对于大型系统，代表性的是对溶剂化蛋白质（Rubredoxin）的计算，对于该系统，ADMM比相应的标准HFX实现好大约20倍。
The calculation of Hartree-Fock exchange (HFX) is computationally demanding for large systems described with high-quality basis sets. In this work, we show that excellent performance and good accuracy can nevertheless be obtained if an auxiliary density matrix is employed for the HFX calculation Several schemes to derive an auxiliary density matrix from a high-quality density matrix are discussed Key to the accuracy of the auxiliary density matrix methods (ADMM) is the use of a correction based on standard generalized gradient approximations for HFX. ADMM integrates seamlessly in existing HFX codes and, in particular, can be employed in linear scaling implementations. Demonstrating the performance of the method, the effect of HFX on the structure of liquid water is investigated in detail using Born-Oppenheimer molecular dynamics simulations (300 ps) of a system of 64 molecules Representative for large systems are calculations on a solvated protein (Rubredoxin), for which ADMM outperforms the corresponding standard HFX implementation by approximately a factor 20