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arXiv · 2303.16957

Averting the infrared catastrophe in the gold standard of quantum chemistry

Nikolaos Masios·Andreas Irmler·Tobias Schäfer·Andreas Grüneis
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Abstract

Coupled-cluster theories can be used to compute ab initio electronic correlation energies of real materials with systematically improvable accuracy. However, the widely-used coupled cluster singles and doubles plus perturbative triples (CCSD(T)) method is only applicable to insulating materials. For zero-gap materials the truncation of the underlying many-body perturbation expansion leads to an infrared catastrophe. Here, we present a novel perturbative triples formalism that yields convergent correlation energies in metallic systems. Furthermore, the computed correlation energies for the three dimensional uniform electron gas at metallic densities are in good agreement with quantum Monte Carlo results. At the same time the newly proposed method retains all desirable properties of CCSD(T) such as its accuracy for insulating systems as well as its low computational cost compared to a full inclusion of the triples. This paves the way for ab initio calculations of real metals with chemical accuracy.

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Nikolaos Masios, Andreas Irmler, Tobias Schäfer, Andreas Grüneis. 2023-03-29. Averting the infrared catastrophe in the gold standard of quantum chemistry. https://doi.org/10.1103/physrevlett.131.186401

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