Accurate prediction of electronic and optical excitations in van der Waals (vdW) materials is a long-standing challenge for density functional theory. The recent Wannier-localized optimally-tuned screened range-separated hybrid (WOT-SRSH) functional has proven successful in non-empirical determination of electronic band gaps and optical absorption spectra for covalent and ionic crystals. However, for vdW materials the tuning of the material- and structure-dependent functional parameters has only been attained semi-empirically. Here, we present a non-empirical WOT-SRSH approach applicable to vdW materials, with the optimal functional parameters transferable between monolayer and bulk. We apply this methodology to prototypical vdW materials: black phosphorus, molybdenum disulfide, and hexagonal boron nitride (in the latter case including zero-point renormalization). We show that the WOT-SRSH approach consistently achieves accuracy levels comparable to experiments and many-body perturbation theory (MBPT) calculations for band structures and optical absorption spectra, both on its own and as an optimal starting point for MBPT calculations.

准确预测范德华 （vdW） 材料中的电子和光学激发是密度泛函理论面临的一个长期挑战。最近的 Wannier 定位优化调谐筛选范围分离混合 （WOT-SRSH） 功能已被证明在共价和离子晶体的电子带隙和光吸收光谱的非经验测定中取得了成功。然而，对于 vdW 材料，材料和结构依赖性功能参数的调整只能半凭经验实现。在这里，我们提出了一种适用于 vdW 材料的非经验 WOT-SRSH 方法，其最佳功能参数可在单层和块体之间转移。我们将这种方法应用于原型 vdW 材料：黑磷、二硫化钼和六方氮化硼（在后一种情况下包括零点重整化）。我们表明，WOT-SRSH 方法始终达到与能带结构和光吸收光谱的实验和多体扰动理论 （MBPT） 计算相当的精度水平，无论是作为 MBPT 计算的最佳起点。