Solvent-Directed Femtosecond Laser Ablation: Tuning Phase and Defect Engineering in Hybrid CdPS3/CdS Nanostructures

Abstract: The limited visible-light absorption of wide-bandgap van der Waals crystals fundamentally restricts their utility in solar energy conversion. Here, we report a surfactant-free, solvent-directed laser synthesis strategy to engineer the phase and optoelectronic properties of Cadmium Phosphorus Trisulfide (CdPS3). By exploiting the non-equilibrium thermodynamics of femtosecond pulsed laser ablation in liquid (fs-PLAL), we demonstrate a tunable transition from the stoichiometric ternary phase to a highly active binary-rich heterostructure. While ablation in water preserves the monoclinic CdPS3 lattice, the reducing environment of isopropanol triggers the formation of CdS quantum dots and metallic cadmium defect sites. This solvent-induced phase engineering transforms the ultraviolet-active host into a robust visible-light photocatalyst. The resulting hybrid CdPS3/CdS nanocolloids exhibit superior charge separation efficiency, driven by Schottky-like metal-semiconductor junctions, achieving ~ 90% degradation of Methylene Blue under 532 nm irradiation within 30 minutes. This work establishes fs-PLAL as a scalable defect-engineering tool for complex ternary layered materials, offering a new design of high-performance metal-thiophosphate-based photocatalysts.