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arXiv 2302.05367cond-mat.mtrl-sci
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低维无机/有机界面的电子结构：混合密度泛函理论、$G_0W_0$和静电模型

Electronic structure of low-dimensional inorganic/organic interfaces: Hybrid density functional theory, $G_0W_0$, and electrostatic models

Jannis Krumland, Caterina Cocchi

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摘要：

混合无机/有机界面的电子性质的第一性原理模拟是具有挑战性的，因为常见的密度泛函理论（DFT）近似针对特定的材料类别，如块状半导体或气相分子。作为一个典型的例子，蒽物理吸附在单层钼$_2$，我们评估的能力，不同的\textit{ab initio}计划描述的电子结构，使用半本地和混合DFT。对于后者，采用无约束的三参数距离分离格式。与多体微扰理论结果的比较表明，DFT基本上无法对界面性质做出可靠的预测。混合泛函，虽然提高了准确性的MoS $_2$能带结构，不系统地增强描述的混合系统相对于半本地泛函。这两种方法都没有为$G_0W_0$提供良好的起点，因此，除了正确的能级对准之外，$G_0W_0$不能提供很多信息。我们表明，非经验参数化的静电屏蔽模型可以完成相同的任务，在可以忽略不计的计算成本。这样的计划可以包括基板的混合界面与实验数据吻合良好。我们的研究结果表明，目前，完全原子，多体模拟弱相互作用的混合系统是不值得所需的计算资源。相比之下，从头算参数化的有效模型模仿环境提供了一个可扩展的替代方案，而不影响准确性和预测性。

英文摘要：

First-principles simulations of electronic properties of hybrid inorganic/organic interfaces are challenging, as common density-functional theory (DFT) approximations target specific material classes like bulk semiconductors or gas-phase molecules. Taking as a prototypical example anthracene physisorbed on monolayer MoS$_2$, we assess the ability of different \textit{ab initio} schemes to describe the electronic structure using semi-local and hybrid DFT. For the latter, an unconstrained three-parameter range-separation scheme is employed. Comparisons against many-body perturbation theory results indicate that DFT is substantially unable to make reliable predictions about interfacial properties. Hybrid functionals, while improving the accuracy of the MoS$_2$ band structure, do not systematically enhance the description of hybrid systems with respect to semi-local functionals. Neither approach provides a good starting point for $G_0W_0$, which, consequently, cannot provide much information beyond the correct energy level alignment. We show that non-empirically parametrized electrostatic screening models can accomplish the same task at negligible computational costs. Such schemes can include substrates of hybrid interfaces in good agreement with experimental data. Our results indicate that currently, fully atomistic, many-body simulations of weakly interacting hybrid systems are not worth the required computational resources. In contrast, ab-initio-parametrized effective models mimicking the environment offer a scalable alternative without compromising accuracy and predictivity.

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