Abstract

Epitaxial heterostructures of narrow-gap IV-VI and III-V semiconductors offer a platform for new electronics and mid-infrared photonics. Stark dissimilarities in the bonding and the crystal structure between the rocksalt IV–VIs and the zincblende III–Vs, however, mandate the development of nucleation and growth protocols to reliably prepare high-quality heterostructures. In this work, we demonstrate a route to single crystal (111)-oriented PbSe epitaxial films on nearly lattice-matched InAs (111)A templates. Without this technique, the high-energy heterovalent interface readily produces two populations of PbSe grains that are rotated 180° in-plane with respect to each other, separated by rotational twin boundaries. We find that a high-temperature surface treatment with the PbSe flux extinguishes one of these interfacial stackings, resulting in single-crystalline films with interfaces that are mediated by a monolayer of distorted PbSe. While very thin PbSe-on-InAs films do not emit light, hinting toward a type-III band alignment, we see strong room temperature photoluminescence from a 1.5 μm thick film with a minority carrier lifetime of 20 ns at low-excitation conditions and bimolecular recombination at high excitation conditions, respectively, even with threading dislocation densities exceeding 108 cm−2. We also note near-complete strain relaxation in these films despite large thermal expansion mismatch to the substrate, with dislocations gliding to relieve strain even at cryogenic temperatures. These results bring to light the exceptional properties of IV-VI semiconductors and the new IV-VI/III-V interfaces for a range of applications in optoelectronics.

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