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 In$XY$ ($X$ = S, Se, Te; $Y$ = Cl, Br, I) monolayers (MLs) using first-principles calculations. Except for InSeCl ML, the remaining eight In$XY$ 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. In$XY$ 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 In$XY$ MLs exhibit high electron mobility (101--899 cm$^2$/V/s) and a pronounced anisotropy ratio in carrier mobility, which effectively suppresses charge recombination. Among them, several stand out: InSI and InSeBr MLs show high electron mobility and a large carrier mobility anisotropy ratio; InSeBr ML exhibits excellent in-plane and out-of-plane piezoelectricity; and InSeBr, InSeI, and InTe$Y$ ($Y$ = Cl, Br, I) MLs show strong visible-light absorption. 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.