Modular construction of Jastrow factors for the transcorrelated method

Area of Science:

• Quantum chemistry
• Computational physics
• Electronic structure theory

Background:

• The transcorrelated method is a powerful tool for electronic structure calculations.
• Optimizing parameters in the Jastrow factor is crucial but computationally intensive.
• Current methods require extensive parameter optimization for each new system.

Purpose of the Study:

• To reduce the number of optimizable parameters in the transcorrelated method.
• To develop a workflow for reusing Jastrow factor components between different systems.
• To maintain or improve the accuracy of calculations using the modified approach.

Main Methods:

• Exploration of Jastrow factor term reuse between atomic and molecular systems.
• Development of a workflow for optimizing atom-specific Jastrow factors.
• Application of the modified workflow within the extended transcorrelated coupled cluster singles and doubles with perturbative triples (xTC-CCSD(T)) method.

Main Results:

• Successful reuse of atom-specific Jastrow factors in molecular calculations.
• Significant reduction in the number of optimizable parameters.
• Demonstrated improvement in the accuracy of xTC-CCSD(T) energies compared to standard methods.

Conclusions:

• The proposed workflow offers an efficient strategy for parameter optimization in the transcorrelated method.
• Reusing Jastrow factors enhances computational efficiency without sacrificing accuracy.
• This approach advances the application of high-accuracy quantum chemical methods.