We study through reflection high‐energy electron diffraction (RHEED) and low‐temperature photoluminescence (PL) spectroscopy the molecular‐beam epitaxy of ZnSe homoepitaxial layers on solid‐phase recrystallized substrates. We show that with a proper exsitu substrate polishing a two‐dimensional (2D) RHEED pattern is readily observed when introducing the substrate into the growth chamber at low temperature. We demonstrate that the insitu pre‐growth treatment has a dramatic influence on ZnSe nucleation and that a suitable preparation leads to direct 2D growth of ZnSe layers which exhibit superior optical properties. The PL spectra are dominated by the near‐band edge emission, with no deep‐level and defect‐related lines.

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