优化用于转关联方法的Jastrow因子
Optimizing Jastrow factors for the transcorrelated method
AI总结：
本研究优化了转关联方法中的实空间Jastrow因子，通过最小化参考能量方差获得更优因子，使TC-FCIQMC仅用cc-pVTZ基组即可对第一行分子达到化学精度，媲美cc-pV5Z基组的非TC计算，并证明忽略三体激发影响极小。
摘要：
我们研究了在转关联（TC）方法中，与高精度量子化学方法（如引发子完全组态相互作用量子蒙特卡洛（FCIQMC））结合使用的灵活定制实空间Jastrow因子的优化问题。通过最小化TC参考能量方差获得的Jastrow因子，比通过最小化变分能量获得的因子能产生更好、更一致的结果。我们计算了具有挑战性的第一行双原子分子C2、CN、N2和O2的全电子原子化能，发现TC方法仅使用cc-pVTZ基组即可获得化学精度结果，其精度大致与使用大得多的cc-pV5Z基组的非TC计算相当。我们还研究了一种近似，即在TC-FCIQMC动力学中忽略纯三体激发，以节省存储和计算成本，并表明该近似对相对能量的影响可忽略不计。我们的结果表明，定制实空间Jastrow因子与多组态TC-FCIQMC方法的结合，为使用适度基组获得化学精度提供了一条途径，从而无需进行基组外推和复合技术。
英文摘要：
We investigate the optimization of flexible tailored real-space Jastrow factors for use in the transcorrelated (TC) method in combination with highly accurate quantum chemistry methods such as initiator full configuration interaction quantum Monte Carlo (FCIQMC). Jastrow factors obtained by minimizing the variance of the TC reference energy are found to yield better, more consistent results than those obtained by minimizing the variational energy. We compute all-electron atomization energies for the challenging first-row molecules C2 , CN, N2 , and O2 and find that the TC method yields chemically accurate results using only the cc-pVTZ basis set, roughly matching the accuracy of non-TC calculations with the much larger cc-pV5Z basis set. We also investigate an approximation in which pure three-body excitations are neglected from the TC-FCIQMC dynamics, saving storage and computational cost, and show that it affects relative energies negligibly. Our results demonstrate that the combination of tailored real-space Jastrow factors with the multi-configurational TC-FCIQMC method provides a route to obtaining chemical accuracy using modest basis sets, obviating the need for basis-set extrapolation and composite techniques.
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