Abstract

Pulsed laser deposition (PLD), as an advanced synthesis technology with unparalleled control over thin films, has evolved into a universal platform for optoelectronic materials engineering. Its unique advantages including precise stoichiometric transfer, heterogeneous structure preparation and in-situ monitoring enable the design of opto-electrocatalysts with controllable active sites.

Traditional methods struggle to pinpoint active sites in hydrogen technologies such as fuel cells and water electrolysis, impeding catalyst customization and mechanistic understanding. Nevertheless, PLD remains underused here despite its outstanding performances in targeted photo-assisted electrocatalysts design. This review systematically explores the breakthrough achievements and provides detailed insights into photo-enhanced water electrolysis and fuel cells based on PLD. Beginning with the fundamentals of epitaxial film growth and film classification, particularly emphasis the related in situ optical analysis techniques.

It subsequently highlights recent advances in electro-oxidation and reduction reactions of H2 and O2, demonstrating the control capabilities of PLD in precisely correlating the structure and activity at the atomic level. Finally, the review concludes by proposing scalable fabrication strategies and performance optimization frameworks to bridge fundamental insights with industrial-scale optoelectronic integration systems.