2D binary transition‐metal chalcogenides (TMCs) such as molybdenum disulfide exhibit excellent properties required for energy conversion applications. Alloying binary TMCs can form 2D compositionally complex TMC alloys (CCTMCAs) that possess remarkable properties from the constituent TMCs. High‐throughput workflow performing density functional theory (DFT) calculations based on the virtual crystal approximation (VCA) model (VCA‐DFT) is designed. The workflow is tested by predicting properties including in‐plane lattice constants, band gaps, effective masses, spin–orbit coupling, and band alignments of the Mo‐W‐S‐Se, Mo‐W‐S‐Te, and Mo‐W‐Se‐Te 2D CCTMCAs. The VCA‐DFT results are validated by computing the same properties using unit cells and supercells of selected compositions. The VCA‐DFT results of the abovementioned five properties are comparable to that of DFT calculations, with some inaccuracies in several properties of MoSTe and WSTe. Moreover, 2D CCTMCAs can form type II heterostructures as used in photovoltaics. Finally, Mo_0.5W_0.5SSe, Mo_0.5W_0.5STe, and Mo_0.5W_0.5SeTe 2D CCTMCAs are used to demonstrate the room‐temperature entropy‐stabilized alloys. They also exhibit high electrical conductivities at 300 K, promising for light adsorption devices. This work shows that the high‐throughput workflow using VCA‐DFT calculations provides a tradeoff between efficiency and accuracy, opening up opportunities in the computational design of other 2D CCTMCAs for various applications.

中文翻译：

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二维成分复杂的过渡金属硫属化物合金的高通量计算表征

二维二元过渡金属硫属元素化物（TMC），例如二硫化钼表现出能量转换应用所需的优异性能。使二元TMC合金化可以形成2D成分复杂的TMC合金（CCTMCA），这些合金具有来自组成TMC的卓越性能。设计了基于虚拟晶体近似（VCA）模型（VCA-DFT）进行密度泛函理论（DFT）计算的高通量工作流程。通过预测包括平面内晶格常数，带隙，有效质量，自旋轨道耦合以及Mo‐W‐S‐Se，Mo‐W‐S‐Te和Mo‐W的谱带对齐的属性来测试工作流程-Se-Te 2D CCTMCA。通过使用选定成分的晶胞和超晶胞计算相同的属性，可以验证VCA-DFT结果。上述五个属性的VCA-DFT结果可与DFT计算的结果相媲美，但MoSTe和WSTe的一些属性有些不准确。而且，二维CCTMCA可以形成光伏中使用的II型异质结构。最后，莫_使用0.5 W _0.5 SSe，Mo _0.5 W _0.5 STe和Mo _0.5 W _0.5 SeTe 2D CCTMCA来证明室温熵稳定的合金。它们还具有300 K的高电导率，有望用于光吸收装置。这项工作表明，使用VCA-DFT计算的高通量工作流提供了效率和准确性之间的折衷，这为各种应用提供了其他2D CCTMCA的计算设计机会。