Overcoming Material Incompatibility via 2D Free‐Surface Engineering

Heteroepitaxy has been pivotal in advancing both optoelectronics and microelectronics, driving the development of faster, more efficient devices across diverse applications. However, achieving high material quality remains challenging due to lattice mismatches. Strain induced by variations in lattice parameters and thermal properties provides additional degrees of freedom for material tailoring but often leads to dislocation generation, wafer bowing, and cracking. These issues are addressed through a scalable post-epitaxial approach that strategically targets the misfit dislocation network, leading to the creation of a sub-nanometric 2D free surface (2DFS). This interface effectively decouples the epilayer from the substrate, significantly reducing strain-related defects. Scalable heterostructures exhibited pronounced defect annihilation, as demonstrated by electron microscopy, defect etching, and photoluminescence analysis-an effect attributed to the surrounding free surfaces. This method strikes an optimal balance between bulk-quality characteristics and high surface integrity, offering a new paradigm for achieving heteroepitaxial bulk-class materials.