Planarizing Spalled GaAs(100) Surfaces by MOVPE Growth

III–V photovoltaic devices have demonstrated exceptional performance across various applications, with controlled crystal fracturing, known as controlled spalling, emerging as a promising method to reduce costs by enabling substrate reuse. Spalling GaAs(100) substrates, a commonly used substrate in III–V photovoltaics, results in faceted ridges that must be planarized to grow high-quality photovoltaic devices. Here we demonstrate that a GaAs(100) wafer offcut toward [01̅1] and spalled toward [011] can be efficiently planarized by growing C:GaAs by metal–organic vapor phase epitaxy (MOVPE) on the surface, with up to 95% of the nominally deposited material used to fill the valleys between ridges. We find that reducing the offcut to 2° enhances the planarizing capability of C:GaAs. A surface morphology model indicates that the density of surface dangling bonds significantly influences the growth evolution of undoped GaAs surfaces. In contrast, the model suggests that the effectiveness of C:GaAs as a smoothing layer stems from modifying the atomic surface structure and, consequently, the associated sticking coefficients of the facets, which can alter the evolution of surface morphology. Our findings provide guidelines for the epitaxial planarization of semiconductor surfaces and improve the understanding of MOVPE growth on nonplanar surfaces.