Structural Stability, Tunable Electronic, and Optical Properties of XSi₂N₄/Cs₂SnI₆ (X = Cr, Mo, W) Heterostructures: First-Principles Studies

Novel optoelectronic and photovoltaic devices are promising, exploiting MoSi2N4-based van der Waals (vdW) heterostructures. Herein, six vertical XSi2N4/Cs2SnI6 (X = Cr, Mo, W) heterostructures are constructed and the atomic structure, stability, and optoelectronic properties via first-principles calculations are investigated. The results of binding energies indicate that XSi2N4/SnI4 is energetically favorable to be established compared to the XSi2N4/CsI. Computed charge density differences show that at the XSi2N4/SnI4 interface, there is no significant charge migration or rearrangement, making it unsuitable for use in charge transport devices. It is worth noticing that the built-in electric field induced by electron transfer from CsI to the XSi2N4 layer prevents light-induced electron and hole recombination, thereby improving carrier lifetime. Furthermore, the CrSi2N4/CsI heterostructure exhibits a wider range of visible light absorption, demonstrating its potential for applications in photoelectronic devices. The electronic and optical properties of XSi2N4/Cs2SnI6 can be tuned through element substitution. The findings could provide useful guidance for designing XSi2N4/Cs2SnI6 photoelectronic and photovoltaic devices.