近化学精度：来自尺寸一致的Padé重求和Møller-Plesset微扰理论
Near Chemical Accuracy From Size-Consistent Padé Resummed Møller-Plesset Perturbation Theory
AI总结：
本文提出尺寸一致的轨道Padé重求和MP2/MP3方法，通过阻尼三阶同自旋贡献，实现近化学精度（MAE约1 kcal/mol），成本同MP3，填补波函数方法精度-成本空白。
AI中文摘要：
Møller-Plesset（MP）微扰理论相关能的Padé重求和不具有尺寸一致性，因此很少被使用。我们提出了一种基于轨道的MP2和MP3自能算符的Padé重求和，其迹可产生尺寸一致的相关能。我们发现，对三阶同自旋贡献进行阻尼可显著提高精度，由此得到的同自旋阻尼轨道Padé重求和（SSD-OPMP3）方法在W4-17数据集中非多参考分子的总原子化能上，相对于金标准CCSD(T)方法达到了近化学精度（平均绝对误差约1 kcal/mol）。对于其他分子数据集，如包含势垒高度、非共价相互作用、偶极矩、静态极化率和过渡金属化学的数据集，也获得了超越CCSD的优异性能。因此，SSD-OPMP3是一种高精度的电子结构方法，其非迭代O(N^6)成本与MP3相同，填补了波函数方法成本/精度层级中的一个空白。
英文摘要：
Padé resummation of the correlation energy from Møller-Plesset (MP) perturbation theory is not size-consistent and is therefore seldom used. We present an orbital-based Padé resummation of the MP2 and MP3 self-energy operators, whose trace yields a size-consistent correlation energy. We find that damping the third-order same-spin contribution leads to substantially increased accuracy, with the resulting same-spin damped orbital Padé resummed (SSD-OPMP3) approach attaining near-chemical accuracy (mean absolute error $\sim$ 1 kcal/mol) for total atomization energies of non-multireference molecules in the W4-17 dataset against the gold standard CCSD(T) method. Excellent performance surpassing CCSD is also obtained for other molecular datasets such as those containing barrier heights, noncovalent interactions, dipole moments, static polarizabilities, and transition-metal chemistry. SSD-OPMP3 is thus a highly accurate electronic structure method with the same noniterative $O(N^6)$ cost as MP3, filling a gap in the cost/accuracy hierarchy of wavefunction methods.
