Virtual Orbital Many-Body Expansions: A Possible Route towards the Full Configuration Interaction Limit,The Journal of Physical Chemistry Letters

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Virtual Orbital Many-Body Expansions: A Possible Route towards the Full Configuration Interaction Limit
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-09-13 00:00:00 , DOI: 10.1021/acs.jpclett.7b02075
Janus J. Eriksen ₁ , Filippo Lipparini ₁ , Jürgen Gauss ₁

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It is demonstrated how full configuration interaction (FCI) results in extended basis sets may be obtained to within sub-kJ/mol accuracy by decomposing the energy in terms of many-body expansions in the virtual orbitals of the molecular system at hand. This extension of the FCI application range lends itself to two unique features of the current approach, namely, that the total energy calculation can be performed entirely within considerably reduced orbital subspaces and may be so by means of embarrassingly parallel programming. Facilitated by a rigorous and methodical screening protocol and further aided by expansion points different from the Hartree–Fock solution, all-electron numerical results are reported for H₂O in polarized core-valence basis sets ranging from double-ζ (10 e, 28 o) to quadruple-ζ (10 e, 144 o) quality.

中文翻译：

虚拟轨道多主体扩展：通往完整配置交互限制的可能途径

它证明了如何通过在手边的分子系统的虚拟轨道中以多体膨胀的方式分解能量，从而获得在扩展的基集中产生的完整构型相互作用（FCI），精确度在亚kJ / mol以内。FCI应用范围的这种扩展使其自身具有当前方法的两个独特特征，即总能量计算可以完全在大大减少的轨道子空间内执行，并且可以通过令人尴尬的并行编程来实现。在严格而系统的筛选方案的协助下，再加上与Hartree-Fock解决方案不同的扩展点，进一步报道了H ₂ O在极化核价基集中双电子（10 e，28 o）到四倍（10 e，144 o）的质量。

更新日期：2017-09-13

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