Optimizing Jastrow factors for the transcorrelated method

• DOI: 10.48550/arxiv.2302.13683
• Publication Date: 2023-01-01
• Authors: J. Philip Haupt; Seyed MohammadRez...; Pablo López Ríos; Werner Dobrautz; Aron J. Cohen; Ali Alavi
• Keywords: Basis (linear algebra); Quantum chemical

We investigate the optimization of flexible tailored real-space Jastrow factors for use in transcorrelated (TC) method combination with highly accurate quantum chemistry methods such as initiator full configuration interaction Monte Carlo (FCIQMC). obtained by minimizing variance TC reference energy are found to yield better, more consistent results than those variational energy. compute all-electron atomization energies challenging first-row molecules C2 , CN, N2 and O2 find that yields chemically using only cc-pVTZ basis set, roughly matching accuracy non-TC calculations much larger cc-pV5Z set. also an approximation which pure three-body excitations neglected from TC-FCIQMC dynamics, saving storage computational cost, show it affects relative negligibly. Our demonstrate multi-configurational provides a route obtaining chemical modest sets, obviating need basis-set extrapolation composite techniques.