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Two-dimensional (2D) materials van der Waals heterostructures (vdWHs)provides a revolutionary route towards high-performance solar energy conversiondevices beyond the conventional silicon-based pn junction solar cells. Despitetremendous research progress accomplished in recent years, the searches ofvdWHs with exceptional excitonic solar cell conversion efficiency and opticalproperties remain an open theoretical and experimental quest. Here we show thatthe vdWH family composed of MoSi$_2$N$_4$ and WSi$_2$N$_4$ monolayers providesa compelling material platform for developing high-performance ultrathinexcitonic solar cells and photonics devices. Using first-principlecalculations, we construct and classify 51 types of MoSi$_2$N$_4$ andWSi$_2$N$_4$-based [(Mo,W)Si$_2$N$_4$] vdWHs composed of various metallic,semimetallic, semiconducting, insulating and topological 2D materials.Intriguingly, MoSi$_2$N$_4$/(InSe, WSe$_2$) are identified as Type-II vdWHswith exceptional excitonic solar cell power conversion efficiency reaching wellover 20%, which are competitive to state-of-art silicon solar cells. The(Mo,W)Si$_2$N$_4$ vdWH family exhibits strong optical absorption in both thevisible and ultraviolet regimes. Exceedingly large peak ultraviolet absorptionsover 40%, approaching the maximum absorption limit of a free-standing 2Dmaterial, can be achieved in (Mo,W)Si$_2$N$_4$/$\alpha_2$-(Mo,W)Ge$_2$P$_4$vdWHs. Our findings unravel the enormous potential of (Mo,W)Si$_2$N$_4$ vdWHsin designing ultimately compact excitonic solar cell device technology.

Cataloguing MoSi$_2$N$_4$ and WSi$_2$N$_4$ van der Waals Heterostructures: An Exceptional Material Platform for Excitonic Solar Cell Applications