用定域原子轨道精确计算总能量的系统收敛方法
Systematically convergent method for accurate total energy calculations with localized atomic orbitals
摘要：
我们介绍了一种方法，用于解决自洽的电子计算在本地化的原子轨道，使我们能够收敛到完整的基组（CBS）限制在一个稳定的，受控的，和系统的方式。我们将我们的结果与简单苯分子的标准量子化学包所获得的结果进行比较。我们发现完美的协议，小基集，并表明，在我们的计划，它是可能的工作与一个非常大的基础上，在一个有效的和稳定的方式。因此，我们可以避免引入任何外推以达到CBS极限。在我们的研究中，我们还进行了变分蒙特卡罗（VMC）和晶格正则化扩散蒙特卡罗（LRDMC）与一个标准的多体波函数（WF）定义的斯莱特行列式和Jastrow因子的产品。一旦Jastrow因子通过保持我们的新方案提供的Slater行列式不变而得到优化，我们得到了一个很好的描述苯分子的原子化能，只有当原子轨道的基础足够大，并接近CBS极限，产生最低的变分能量。
英文摘要：
We introduce a method for solving a self consistent electronic calculation within localized atomic orbitals, that allows us to converge to the complete basis set (CBS) limit in a stable, controlled, and systematic way. We compare our results with the ones obtained with a standard quantum chemistry package for the simple benzene molecule. We find perfect agreement for small basis set and show that, within our scheme, it is possible to work with a very large basis in an efficient and stable way. Therefore we can avoid to introduce any extrapolation to reach the CBS limit. In our study we have also carried out variational Monte Carlo (VMC) and lattice regularized diffusion Monte Carlo (LRDMC) with a standard many-body wave function (WF) defined by the product of a Slater determinant and a Jastrow factor. Once the Jastrow factor is optimized by keeping fixed the Slater determinant provided by our new scheme, we obtain a very good description of the atomization energy of the benzene molecule only when the basis of atomic orbitals is large enough and close to the CBS limit, yielding the lowest variational energies.
机构、总结、中文摘要均由AI分析而来，可能存在错误，请以论文正文为准。
