Two dimensional transition metal dichalcogenide based bilayer heterojunctions for efficient solar cells and photocatalytic applications

This work presents a first-principles study of the optoelectronic properties of vertically-stacked bilayer heterostructures composed of 2D transition-metal dichalcogenides (TMDs). The calculations are performed using the density-functional theory (DFT) and many-body perturbation theory within $G_0W_0$-BSE methodology. We aim to propose these TMD heterostructures for solar cell applications. The TMD monolayers comprising the heterojunctions considered in this work are $MoS_2$, $WS_2$, $MoSe_2$, and $WSe_2$ due to their favorable band gaps, high carrier mobility, robust absorption in the visible region, and excellent stability. These four TMD monolayers provide the basis for six heterostructures. Consequently, we have examined the structural, electronic, and optical properties of six heterostructures ($WS_2/MoS_2$, $MoSe_2/MoS_2$, $MoSe_2/WS_2$, $WSe_2/MoS_2$, $WSe_2/MoSe_2$, and $WSe_2/WS_2$). At the DFT level, all the six considered TMD heterostructures meet the essential criterion of type II band alignment, a critical factor in extending carrier lifetime. However, according to $G_0W_0$ results, $MoSe_2/WS_2$ does not exhibit the type II band alignment, instead it shows type I band alignment. The large quasiparticle gaps obtained from $G_0W_0$ approximation suggest the presence of strong electron-correlation effects. The quality of these heterojunction solar cells is estimated by computing their power conversion efficiencies (PCE). The PCEs are calculated at both the HSE06 and $G_0W_0$ levels, and the maximum PCE predicted by HSE06 calculations on our designed solar cells can reach up to 19.25% for the $WSe_2/WS_2$ heterojunction. In addition, all six TMD heterostructures are examined for their potential applications in photocatalysis for hydrogen evolution reaction, and the three of them, namely, $WS_2/MoS_2$, $MoSe_2/MoS_2$, and $WSe_2/MoS_2$ heterostructures qualify for the same.
Comment: 49 pages (40 pages Manuscript and 9 pages Supporting Material), 9 figures and 11 tables in the manuscript, and 7 figures and 6 tables in the Supporting Material