A multi-factor adjustable PtSe2/GaN van der Waals heterostructure with enhanced photocatalytic performance

Two-dimensional van der Waals heterostructures with multiple tunable approaches in electronic and optical properties are highly superior for photocatalysis and novel devices. By applying first-principles calculations, we systematically studied the electronic structure, optical absorption, carrier mobility and solar-to-hydrogen efficiency of PtSe2/GaN heterostructures, which are affected by different thicknesses, varying directions of polarization of the GaN nanosheets and applied mechanical strain of the whole system. The results indicate that these heterostructures exhibit thermodynamic stability at room-temperature (300 K), and most configurations have type-II band alignment, among which the heterostructure consisting of GaN trilayers and PtSe2 shows high visible-light absorption (1.71 × 105 cm-1) and ultra-wide range of pH values (pH = 0-14) for the photocatalytic water splitting reaction and exceedingly high overpotential for the hydrogen evolution reaction (3.375 eV). Simultaneously, being two of the most significant parameters of photocatalysis and devices, the carrier mobility and solar-to-hydrogen efficiency have also been calculated, respectively, reaching up to 1601 cm2 V-1 s-1 and 17.2%. Moreover, the photoelectrical properties can be highly tuned through further biaxial strain engineering; especially, the visible-light absorption can be enhanced to 2.85 × 105 cm-1 by applying 6% compression strain. Thus, the PtSe2/GaN heterostructure we proposed shows a broad prospect for photocatalytic water splitting.