High-Throughput Design Method Based On Anderson’s Rule For Two-Dimentional Heterostructures And Its Appliaction

The rapid expansion of modern emerging industries has increased the urgency of developing novel and advanced materials.As an emerging field of condensed matter physics and materials science,high-throughput calculation and design accelerate the discovery and application of novel functional materials.The high-throughput design method based on Anderson’s rule（AR）has been applied in a preliminary manner to the design of non-polar two-dimensional（2D）van der Waals（vd W）heterostructures.However,the applicability and design flaw of the method remain obscure.Through large-scale density functional theory（DFT）calculations,this papersystematically investigate the limitations of the AR-based high-throughput design method,explore the physical mechanism of the high-throughput design error,and propose strategies to improve the method and expand its application.The primary findings of the research are as follows:（1）We found that the classification of band alignment by AR-based high-throughput design method is incomplete.The AR-based high-throughput design method typically classifies the band alignments of 2D vd W heterostructures as type-I,type-II,and type-III.Theoretically,there are three additional types of band alignments:type-IV,type-V,and type-VI（Type-other）.Based on a high-throughput calculation of53 2D A₂B₂ heterostructures with hexagonal honeycomb structure（A and B are group IV and V elements,respectively）,we investigated the distribution of type-other band alignments,their physical mechanisms and their responses to external modulation.According to the findings,the proportion of type-V and type-VI band alignments in 2D vd W heterostructures with hexagonal honeycomb structure is apparoximately 20%.In the presence of a weak applied strain and external electric field,the type-VI band alignment is stable.The incomplete classification of band alignments implies that the AR-based high-throughput design method would misclassify the band alignment types of 2D vd W heterostructures.（2）We discovered the misclassification of band alignment types by the AR-based high-throughput design method and the underlying physical mechanism of this phenomenon.Based on a large-scale calculation of 1231 nonpolar 2D vd W heterojunctions with hexagonal phase,we systematically investigate the prediction accuracy of the AR-based high-throughput design method on the band alignment types,and explore the effect of various interface factors on the misclassification of band alignment types.The results indicate that the AR-based high-throughput design method is incapable of predicting type-other band alignment and misclassifies a number of type-II band alignments as type-III.The misclassification of type-other and type-III band alignment by AR are attributed to the neglect of interlayer orbital coupling effect and charge redistribution effect,respectively.The incorrect classification of the band alignment type suggests that the AR-based high-throughput design method would generate erroneous design results.（3）We reveal the omission behavior of the AR-based high-throughput design method for the design of functional heterostructures.Based on the high-throughput design results of nonpolar A₂B₂（A are group III and IV elements;B are group V and VI elements）2D vd W heterostructures,we investigated the reliability of AR-based high-throughput design method for designing solar energy conversion materials,and explored the correlation between the omission behavior in the design results and the electronic properties of heterostructures.The results demonstrate that the AR-based high-throughput design method can reasonably screen the candidate heterostructures applied to water splitting photocatalyst,but omits approximately half of the candidate heterostructures applied to solar cells.The omission behavior can be attributed to the inaccurate predictions for the power conversion efficiency（PCE）.Based on the AR and a large-scale calculation of 474 hexagonal-phase unpolarized 2D vd W heterojunctions,we found that an appropriate relaxation of the screening criteria can effectively reduce the omission of candidate heterostructures applied to solar cells.Using the relaxed screening criteria,we screened approximately 70 solar cell materials with PCE>20%from more than 8000 2D vd W heterostructures.（4）We developed the high-throughput design method for polar 2D vd W heterostructures.Based on large-scale calculations of more than 3000 nonpolar transition group metal sulfides（TMDs）and polar Janus-TMD heterojunctions,we investigated the effect of the intrinsic dipole in polar heterostructures on the interfacial electrostatic potential and electronic properties,explored the feasibility of the AR-based high-throughput design method applied in Janus-TMD heterojunctions,and proposed an improved high-throughput design strategy for Janus-TMD heterostructures.The results show that the AR-based high-throughput design method has similar prediction errors of the band alignment types,band edge positions and PCEs for TMD and polar Janus-TMD heterostructures,which demonstrate that the AR-based high-throughput design method and related conclusions can be extended to polar 2D vd W heterostructures.Using this high-throughput design method,we identified approximately 130 solar cell materials with PCE>20%from 12,000 polar 2D heterostructures.Based on the AR,the electrostatic potential compensation strategy can partially describes the effect of charge redistribution,thereby increasing the precision of the AR-based high-throughput design method.