Max Planck Institute for Solid State Research, Heisenbergstraße 1, 70569 Stuttgart, Germany.
Yusuf Hamied Department of Chemistry, University of Cambridge, Lensfield Road, Cambridge CB2 1EW, United Kingdom.
J Chem Phys. 2023 Jun 7;158(21). doi: 10.1063/5.0151412.
We demonstrate the accuracy of ground-state energies of the transcorrelated Hamiltonian, employing sophisticated Jastrow factors obtained from variational Monte Carlo, together with the coupled cluster and distinguishable cluster methods at the level of singles and doubles excitations. Our results show that already with the cc-pVTZ basis, the transcorrelated distinguishable cluster method gets close to the complete basis limit and near full configuration interaction quality values for relative energies of over thirty atoms and molecules. To gauge the performance in different correlation regimes, we also investigate the breaking of the nitrogen molecule with transcorrelated coupled cluster methods. Numerical evidence is presented to further justify an efficient way to incorporate the major effects coming from the three-body integrals without explicitly introducing them into the amplitude equations.
我们通过变分蒙特卡罗方法得到了复杂的 Jastrow 因子，结合单激发和双激发的耦合簇和可区分簇方法，展示了关联哈密顿量基态能量的准确性。我们的结果表明，仅使用 cc-pVTZ 基，关联可区分簇方法就接近完全基限制，并且对于三十多个原子和分子的相对能量，接近完全组态相互作用质量值。为了衡量不同相关区域的性能，我们还研究了关联耦合簇方法对氮分子的断裂。给出了数值证据，进一步证明了一种有效的方法来结合来自三体积分的主要影响，而无需将它们显式地引入振幅方程中。
