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Putting PASPT2 on a Firmer Basis

2026/07/24 by Chunzhang Liu, Ning Zhang, Wenjian Liu
Physics and Astronomy · #physics.chem-ph

paper · pdf

3 figures,1 table

arxiv created 2026/07/29 · arxiv updated 2026/07/31

Abstract

The recently proposed partial-active-space (PAS) multi-state second-order perturbation theory (PASPT2) [Precis. Chem. 4, 997 (2026)] features connected amplitudes and a connected, closed intermediate Hamiltonian. Despite these hallmarks, PASPT2 (denoted as PASPT2H from now on) is not strictly size-extensive, as originally thought (and numerically confirmed), albeit strictly size-consistent. Nevertheless, PASPT2 is near-extensive for the states with major projections on the chosen PAS M0. This becomes more transparent upon introducing PASPT2X, a strictly size-extensive variant. Compared with the intruder-prone PASPT2X, the intruder-free PASPT2H merely neglects the second-order corrections that are important only for those states with major projections on the orthogonal complement RX of M0 within the closed space MX (=M0\oplusRX); however, such states are not supported by the chosen finite one-particle basis set. The weak violation of size-extensivity is therefore numerically insignificant for the target states supported by M0, reinforcing the theoretical basis of PASPT2H.

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