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arXiv · 2508.15744

Regularized Perturbation Theory for Ab initio Solids

Meng-Fu Chen·Jinghong Zhang·Hieu Q. Dinh·Adam Rettig·Joonho Lee
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Abstract

Second-order Moller-Plesset perturbation theory (MP2) for ab initio simulations of solids is often limited by divergence or over-correlation issues, particularly in metallic, narrow-gap, and dispersion-stabilized systems. We develop and assess three regularized second-order perturbation theories: $\kappa$-MP2, $\sigma$-MP2, and the size-consistent Brillouin-Wigner approach (BW-s2), across metals, semiconductors, molecular crystals, and rare gas solids. BW-s2 achieves high accuracy for cohesive energies, lattice constants, and bulk moduli in metals, semiconductors, and molecular crystals, rivaling or surpassing coupled-cluster with singles and doubles at lower cost. In rare gas solids, where MP2 already underbinds, $\kappa$-MP2 does not make the results much worse while BW-s2 struggles. These results illustrate both the potential and the limitations of regularized perturbation theory for efficient and accurate solid-state simulations. While broader testing is warranted, BW-s2($\alpha$ = 2) appears particularly promising, with possible advantages over modern random-phase approximations and coupled-cluster theory.

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Meng-Fu Chen, Jinghong Zhang, Hieu Q. Dinh, Adam Rettig, Joonho Lee. 2025-08-21. Regularized Perturbation Theory for Ab initio Solids. https://doi.org/10.1021/acs.jpclett.5c02731

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