Integration of promising piezoelectric and photocatalytic properties in Janus In$XY$ ($X$ = S, Se, Te; $Y$ = Cl, Br, I) monolayers and their heterojunctions

Abstract: Two-dimensional (2D) Janus materials show great promise as piezoelectric materials and photocatalysts for water splitting. In this work, we systematically investigated the piezoelectric and photocatalytic properties of the hexagonal Janus InXY (X = S, Se, Te; Y = Cl, Br, I) monolayers (MLs) using first-principles calculations. Except for InSeCl ML, the remaining eight InXY MLs are stable and exhibit exceptionally high in-plane piezoelectric coefficients ($|d_{22}| = $6.07--155.27 pm/V), which exceed those of most known 2D materials. InXY MLs possess band edges straddling the water redox potentials at pH = 0. Their intrinsic vertical polarization induces an intralayer polarization field $E_{\rm intra}$, leading to low exciton binding energies (0.44--0.78 eV). Moreover, their strong vertical piezoelectric responses ($|d_{32}|$ = 0.34--0.65 pm/V) suggest that in-plane stress can further enhance $E_{\rm intra}$ to facilitate the separation of photogenerated carriers. Additionally, these InXY MLs exhibit high electron mobility (101--899 cm$^2$/V/s) and a pronounced anisotropy ratio in carrier mobility, which effectively suppresses charge recombination. To optimize performance, we constructed a van der Waals heterojunction (InSI/InSeBr), which demonstrates remarkable photocatalytic properties, including enhanced redox ability, a direct Z-scheme charge transfer pathway, strong visible-light absorption, high carrier mobility, and excellent photocorrosion resistance. Our results indicate that hexagonal Janus InXY MLs and their heterojunctions are multifunctional materials integrating piezoelectricity and photocatalysis, paving the way for energy conversion applications.