Modular Construction of Jastrow Factors for the Transcorrelated Method

TL;DR

This paper introduces a modular approach to constructing Jastrow factors in the transcorrelated method, enabling reuse of atom-specific terms to reduce optimization complexity and improve energy accuracy.

Contribution

It proposes a workflow for reusing atom-optimized Jastrow terms in molecules, reducing parameters and enhancing energy calculation accuracy.

Findings

Reduces the number of parameters to optimize in the Jastrow factor.

Improves the accuracy of xTC-CCSD(T) energy calculations.

Maintains performance while simplifying the optimization process.

Abstract

In this work, we explore the reuse of terms in the Jastrow factor between systems for use in the transcorrelated method, to reduce the number of optimisable parameters for a given system. In particular, we propose a workflow in which atom-specific parts of Jastrow factors, optimised in atoms, may be reused in the molecule, with only a few parameters in the electron-electron part of the Jastrow left to optimise, while maintaining performance. We find that the modified workflow not only reduces the number of terms needing to be optimised, but also improves the accuracy of xTC-CCSD(T) energies.