A new family of seniority-restricted coupled cluster methods

Ram贸n Alain Miranda-Quintana, Rugwed Lokhande, Carlos E. V. de Moura, Krisztina Zsigmond, Paul W. Ayers

Published: 2025/9/18

Abstract

We introduce a novel class of coupled cluster (CC) methods that leverage the seniority concept to enhance efficiency and accuracy in electronic structure calculations. While existing approaches, such as the pair coupled cluster doubles (pCCD) method, are limited to seniority-zero ({\Omega} = 0) wavefunctions,1 we propose a more flexible framework: seniority-restricted coupled cluster (sr-CC). This new methodology selectively constrains the seniority sectors accessible through excitation operators in the cluster expansion, enabling a more systematic exploration of electron correlation effects. By balancing computational cost and accuracy, sr-CC provides a promising pathway for advancing electronic structure theory, particularly in strongly correlated systems.

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