High-throughput computational design for 2D van der Waals functional heterostructures: Fragility of Anderson's rule and beyond

The heart of current high-throughput computational design for two-dimensional (2D) van der Waals (vdW) functional heterostructures is Anderson's rule (AR). This non-interacting model, however, inevitably introduces error and uncertainty in design results, problems which remain neglected. We report that, even for a non-magnetic system, the current high-throughput design framework commonly omits potential candidates in specific fields, such as heterostructure solar cell research. Therefore, this framework is fragile to extend to all subfields of functional vdW heterostructures. Through the analysis of several factors, such fragility is found to arise mainly from interlayer orbital coupling. This effect is omitted by AR and causes statistical deviation in the prediction of electronic properties. In the absence of a more advanced and universal physical model for describing interlayer orbital coupling, we propose a robust high-throughput design framework to reduce the omission of potential candidates. This work deepens the understanding of high-throughput design for 2D vdW functional heterostructures and provides insight into their development.