耦合集团理论在平面波随机相位近似中的局部嵌入
Local embedding of Coupled Cluster theory into the Random Phase Approximation using plane-waves
摘要：
提出了一种处理周期环境中局域电子关联效应的嵌入方法。在一个单一、一致的框架中，我们的基于平面波的方案将采用局部轨道的局部高级相关性计算（这里是耦合簇理论，CC）嵌入到低级相关性计算（这里是直接随机相位近似，RPA）中。这种选择允许精确和有效地处理长程色散效应。加速收敛相对于本地片段的大小，可以观察到，如果低级别和高级别的远程分散是定量相似的，是在RPA的CC的情况下。为了证明引入嵌入方法的能力，我们计算表面上和菱沸石晶体笼中的分子的吸附能，以及在高度精确的多电子微扰理论的水平上的固体中的晶格杂质的形成能。例如，沸石菱沸石中的甲烷分子的吸收能量在CC水平下以远低于20 meV的误差收敛。作为我们最大的周期性基准系统，我们将我们的计划应用于含有超过1000个电子的超级电池中的二氧化钛上的水分子的吸附。
英文摘要：
We present an embedding approach to treat local electron correlation effects in periodic environments. In a single, consistent framework, our plane-wave based scheme embeds a local high-level correlation calculation (here Coupled Cluster Theory, CC), employing localized orbitals, into a low-level correlation calculation (here the direct Random Phase Approximation, RPA). This choice allows for an accurate and effcient treatment of long-range dispersion effects. Accelerated convergence with respect to the local fragment size can be observed if the low-level and high-level long-range dispersion are quantitatively similar, as is the case for CC in RPA. To demonstrate the capabilities of the introduced embedding approach, we calculate adsorption energies of molecules on a surface and in a chabazite crystal cage, as well as the formation energy of a lattice impurity in a solid at the level of highly accurate many-electron perturbation theories. The absorption energy of a methane molecule in a zeolite chabazite, for instance, is converged with an error well below 20 meV at the CC level. As our largest periodic benchmark system, we apply our scheme to the adsorption of a water molecule on titania in a supercell containing more than 1000 electrons.
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