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首页> 外文期刊>The Journal of Chemical Physics >Linear-scaling atomic orbital-based second-order Moller-Plessetperturbation theory by rigorous integral screening criteria
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Linear-scaling atomic orbital-based second-order Moller-Plessetperturbation theory by rigorous integral screening criteria

机译：通过严格的积分筛选准则线性定标基于原子轨道的二阶Moller-Plesset摄动理论

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摘要

A Laplace-transformed second-order Moller–Plesset perturbation theory (MP2) method ispresented, which allows to achieve linear scaling of the computational effort with molecular size forelectronically local structures. Also for systems with a delocalized electronic structure, a cubic oreven quadratic scaling behavior is achieved. Numerically significant contributions to the atomicorbital (AO)-MP2 energy are preselected using the so-called multipole-based integral estimates(MBIE) introduced earlier by us [J. Chem. Phys. 123, 184102 (2005)]. Since MBIE providesrigorous upper bounds, numerical accuracy is fully controlled and the exact MP2 result is attained.While the choice of thresholds for a specific accuracy is only weakly dependent upon the molecularsystem, our AO-MP2 scheme offers the possibility for incremental thresholding: for only littleadditional computational expense, the numerical accuracy can be systematically converged. Weillustrate this dependence upon numerical thresholds for the calculation of intermolecular interactionenergies for the S22 test set. The efficiency and accuracy of our AO-MP2 method is demonstratedfor linear alkanes, stacked DNA base pairs, and carbon nanotubes: e.g., for DNA systems thecrossover toward conventional MP2 schemes occurs between one and two base pairs. In this way,it is for the first time possible to compute wave function-based correlation energies for systemscontaining more than 1000 atoms with 10 000 basis functions as illustrated for a 16 base pair DNAsystem on a single-core computer, where no empirical restrictions are introduced and numericalaccuracy is fully preserved.
机译：提出了一种拉普拉斯变换的二阶Moller-Plesset扰动理论（MP2）方法，该方法可以实现计算工作量与电子局部结构的分子大小的线性比例缩放。同样对于具有离域电子结构的系统，也可以获得立方或偶数二次缩放行为。使用我们先前介绍的所谓的基于多极子的积分估计（MBIE），可以预先选择出对原子轨道（AO）-MP2能量具有重要意义的数值。化学物理123，184102（2005）]。由于MBIE提供了严格的上限，因此可以完全控制数值精度并获得准确的MP2结果。虽然为特定精度选择阈值的方法仅与分子系统有很小的依赖关系，但我们的AO-MP2方案为增量阈值化提供了可能性：很少的额外计算开销，就可以系统地收敛数值精度。我们说明了这种对数值阈值的依赖性，用于计算S22测试集的分子间相互作用能。对于线性烷烃，堆叠的DNA碱基对和碳纳米管，我们证明了AO-MP2方法的效率和准确性：例如，对于DNA系统，在一个和两个碱基对之间发生了与常规MP2方案的交叉。这样，对于单核计算机上的16个碱基对的DNA系统而言，首次有可能为包含1000个以上原子且具有1万个基函数的系统计算基于波动函数的相关能量。引入并完全保留数值精度。

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