论文标题

杂交密度功能计算的可重复性,用于状态方程性能和带隙

Reproducibility of Hybrid Density Functional Calculations for Equation-of-State Properties and Band Gaps

论文作者

Ji, Yuyang, Lin, Peize, Ren, Xinguo, He, Lixin

论文摘要

杂交密度功能(HDF)近似通常比局部和半近似值具有更高的准确性,而交换相关功能的精度则大大提高了计算成本。 HDF的实际实现不可避免地涉及数值近似值 - 由于处理精确交换组件产生的其他数值复杂性,其局部和半局部性近似值甚至比其局部和半属性对应物更重要。这就提出了有关HDF结果的可重复性的问题,该问题由不同的实现产生。在这项工作中,我们基于流行的Heyd-Scuseria-Ernzerhof(HSE)范围分隔的HDF的四个独立实现的数值精度,用于描述关键材料的属性,包括源自状态方程(EOS)的方程(EOS)和20晶体固体的带隙。我们发现,这四个代码获得的能量频段差距相互满意。但是,对于晶格常数和大量模量,由不同代码计算的结果之间的偏差与计算结果和实验结果之间的偏差相同。一方面,这意味着HSE功能非常准确地描述了简单绝缘固体的内聚特性。另一方面,这也表明,当前主要的HSE实施实现的数值精度不足以明确评估HDF的身体准确性。发现核心电子的伪电势治疗是导致这种不确定性的主要因素。

Hybrid density functional (HDF) approximations usually deliver higher accuracy than local and semilocal approximations to the exchange-correlation functional, but this comes with drastically increased computational cost. Practical implementations of HDFs inevitably involve numerical approximations -- even more so than their local and semilocal counterparts due to the additional numerical complexity arising from treating the exact-exchange component. This raises the question regarding the reproducibility of the HDF results yielded by different implementations. In this work, we benchmark the numerical precision of four independent implementations of the popular Heyd-Scuseria-Ernzerhof (HSE) range-separated HDF on describing key materials' properties, including both properties derived from equations of states (EOS) and band gaps of 20 crystalline solids. We find that the energy band gaps obtained by the four codes agree with each other rather satisfactorily. However, for lattice constants and bulk moduli, the deviations between the results computed by different codes are of the same order of magnitude as the deviations between the computational and experimental results. On the one hand, this means that the HSE functional is rather accurate for describing the cohesive properties of simple insulating solids. On the other hand, this also suggests that the numerical precision achieved with current major HSE implementation is not sufficiently high to unambiguously assess the physical accuracy of HDFs. It is found that the pseudopotential treatment of the core electrons is a major factor that contributes to this uncertainty.

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