We seek correlation‐consistent diffuse‐augmented double‐zeta and triple‐zeta basis sets that perform optimally in extrapolating the correlation energy to the one‐electron complete basis set limit, denoted oAVXZ and oAV(X + d)Z. The novel basis sets are method‐dependent in that they are trained to perform optimally for the correlation energy at each specific level of theory. They are shown to yield accurate results in calculating both the energy and tensorial properties such as polarizabilities while not significantly altering the Hartree‐Fock energy. Quantitatively, complete basis set limit (CBS)‐/(oAVdZ,oAVtZ)‐extrapolated correlation energies typically outperform, by 3‐ to 5‐fold, the ones calculated with traditional ansatzes of similar flexibility. Attaining energies of CBS/(AVtZ,AVqZ) type or better accuracy, they frequently outperform expensive raw explicitly correlated ones. Promisingly, a limited test on CBS‐extrapolated energies based on conventional basis sets has shown that they compare well even with extrapolated explicitly correlated ones. Calculated atomization and dissociation energies, molecular geometries, ionization potentials, and electron affinities also tend to outperform the ones obtained with traditional Dunning's ansatzes from which the new basis sets have been determined. The method for basis set generation is simple, and there is no reason of principle why the approach could not be adapted for handling other bases in the literature.

中文翻译：

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用于相关能量外推的最优扩散增强原子基集

我们寻求相关一致的弥散增强的double-zeta和Triple-zeta基集，它们在将相关能量外推到单电子完整基集限制（以oAV X Z和oAV（X  +  d）Z表示）中表现最佳。新的基础集依赖于方法，因为它们经过训练，可以在每个特定的理论水平上针对相关能量最佳地执行。在计算能量和张量特性（例如极化率）时，它们显示出了准确的结果，而不会显着改变Hartree-Fock能量。定量的完整基准集限制（CBS）-/（oAV d Z，oAV tZ）推算出的相关能量通常比使用具有类似灵活性的传统方法计算出的相关能量高3到5倍。达到CBS /（AV t Z，AV q的能量Z）类型或更高的精度，它们通常胜过昂贵的原始显式关联的。很有可能，对基于常规基集的CBS外推能量的有限测试表明，即使与外推明确相关的能量进行比较，它们也能很好地进行比较。计算出的雾化和离解能，分子几何形状，电离势和电子亲和力也往往优于传统的邓宁分析所确定的新基础。用于基础集生成的方法很简单，并且没有原理上的理由为什么该方法不能适用于文献中的其他基础。