Improvement on the screening of nonlinear commutator operations in selective coupled-cluster using Lagrangian.

Abstract

We introduce a Lagrangian implementation of the full coupled-cluster reduction [Xu et al., Phys. Rev. Lett. 121, 113001 (2018)], that is, a selected coupled-cluster (CC) based on an arbitrary-order full CC expansion using direct commutator expansions. In this method, the screening for the products of cluster amplitudes plays a central role to reduce the computational cost for the nonlinear commutator operations, while the convergence of the total energy in the standard energy expression is not rapid with tightening the threshold. The new implementation using Lagrangian is robust, containing error only quadratic to those of amplitudes, allowing a much larger screening threshold. We demonstrate the performance of the new implementation by investigating the calculations of N2 and C6H6. The accuracy and applicability are also demonstrated for the potential energy curve of H2O in comparison with conventional quantum chemical methods.