论文标题

在4C相关域中迈向DMRG量化的耦合群集方法

Towards DMRG-tailored coupled cluster method in the 4c-relativistic domain

论文作者

Brandejs, Jan, Višňák, Jakub, Veis, Libor, Mihály, Maté, Legeza, Örs, Pittner, Jiří

论文摘要

计算相对论化学中有三个基本问题:电子以相对论速度移动,近距离状态和动态相关性。当前可用的量子化学方法能够解决其中一个或两个问题的系统。但是,存在很大的分子,其中所有三个效应都存在。这些是带有开放D或F壳的较重的过渡金属化合物,灯笼和肌动剂。对于此类系统,无法使用足够准确的数值方法,这阻碍了理论化学在该领域的应用。在本文中,我们结合了两种数值方法,以解决这一具有挑战性的分子类别。这些是耦合群集方法和密度基质重新归一化组(DMRG)方法的相对论版本。据我们所知,这是通过DMRG外部校正的耦合聚类方法的第一个相对论实现。正如我们在TLH,ASH和SBH系统上所证明的那样,该方法带来了大幅降低计算成本。

There are three essential problems in computational relativistic chemistry: electrons moving at relativistic speeds, close lying states and dynamical correlation. Currently available quantum-chemical methods are capable of solving systems with one or two of these issues. However, there is a significant class of molecules, in which all the three effects are present. These are the heavier transition metal compounds, lanthanides and actinides with open d or f shells. For such systems, sufficiently accurate numerical methods are not available, which hinders the application of theoretical chemistry in this field. In this paper, we combine two numerical methods in order to address this challenging class of molecules. These are the relativistic versions of coupled cluster methods and density matrix renormalization group (DMRG) method. To the best of our knowledge, this is the first relativistic implementation of the coupled cluster method externally corrected by DMRG. The method brings a significant reduction of computational costs, as we demonstrate on the system of TlH, AsH and SbH.

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