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We prepare quasi-1D films of Sb2Se3 on GaAs by molecular beam epitaxy. The aligned grains and anisotropic bonding hierarchy of the Sb2Se3 unit cell together produce giant birefringence in the near-infrared. 

PbSe is a narrow bandgap IV–VI compound semiconductor with application in mid-wave infrared optoelectronics, thermoelectrics, and quantum devices. Alkaline-earth or rare-earth elements such as Sr and Eu can substitute Pb to widen the bandgap of PbSe in heterostructure devices, but they come with challenges such as deteriorating optical and electronic properties, even in dilute concentrations due to their dissimilar atomic nature. We substitute Pb instead with column IV Ge and assess the potential of rocksalt phase PbGeSe as a wider bandgap semiconductor in thin films grown by molecular beam epitaxy on GaAs substrates. Low sticking of GeSe adatoms requires synthesis temperatures below 260 °C to incorporate Ge, but this yields poor structural and compositional uniformity as determined by x-ray diffraction. Consequently, as-grown films in the range Pb0.94Ge0.06Se–Pb0.83Ge0.17Se (6%–17% Ge) show much less bandgap widening in photoluminescence than prior work on bulk crystals using absorption. We observe that post-growth rapid thermal annealing at temperatures of 375–450 °C improves the crystal quality and recovers bandgap widening. Rapid interdiffusion of Ge during annealing, however, remains a challenge in harnessing such PbGeSe materials for compositionally sharp heterostructures. Annealed 17% Ge films emit light at 3–3.1 μm with a minimal shift in wavelength vs temperature. These samples are wider in bandgap than PbSe films by 55 meV at room temperature, and the widening increases to 160 meV at 80 K, thanks to sharply different dependence of bandgap on temperature in PbSe vs PbGeSe. 

We investigate the beneficial effects of rapid thermal annealing on structure and photoluminescence of PbSe thin films on GaAs (001) grown below 150 °C, with a goal of low temperature integration for infrared optoelectronics. Thin films of PbSe deposited on GaAs by molecular beam epitaxy are epitaxial at these reduced growth temperatures, yet the films are highly defective with a mosaic grain structure with low angle and dendritic boundaries following coalescence. Remarkably, we find that rapid thermal annealing for as short as 180 s at temperatures between 300 and 425 °C in nitrogen ambient leads to extensive re-crystallization and transformation of these grain boundaries. The annealing at the same time dramatically improves the band edge luminescence at 3.7 μm from previously undetectable levels to nearly half as intense as our best conventionally grown PbSe films at 300 °C. We show using an analysis of laser pump-power dependent photoluminescence measurements that this dramatic improvement in the photoluminescence intensity is due to a reduction in the trap-assisted recombination. However, we find it much less correlated with improved structural parameters determined by x-ray diffraction rocking curves, thereby pointing to the importance of eliminating point defects over extended defects. Overall, the success of rapid thermal annealing in improving the luminescent properties of low growth temperature PbSe is a step toward the integration of PbSe infrared optoelectronics in low thermal budget, back end of line compatible fabrication processes. 

We report on photoluminescence in the 3–7 µm mid-wave infrared (MWIR) range from sub-100 nm strained thin films of rocksalt PbSe(001) grown on GaAs(001) substrates by molecular beam epitaxy. These bare films, grown epitaxially at temperatures below 400 °C, luminesce brightly at room temperature and have minority carrier lifetimes as long as 172 ns. The relatively long lifetimes in PbSe thin films are achievable despite threading dislocation densities exceeding 109 cm−2 arising from island growth on the nearly 8% lattice- and crystal-structure-mismatched GaAs substrate. Using quasi-continuous-wave and time-resolved photoluminescence, we show that the Shockley–Read–Hall recombination is slow in our high dislocation density PbSe films at room temperature, a hallmark of defect tolerance. Power-dependent photoluminescence and high injection excess carrier lifetimes at room temperature suggest that degenerate Auger recombination limits the efficiency of our films, although the Auger recombination rates are significantly lower than equivalent III–V bulk materials and even a bit slower than expectations for bulk PbSe. Consequently, the combined effects of defect tolerance and low Auger recombination rates yield an estimated peak internal quantum efficiency of roughly 30% at room temperature, unparalleled in the MWIR for a severely lattice-mismatched thin film. We anticipate substantial opportunities for improving performance by optimizing crystal growth as well as understanding Auger processes in thin films. These results highlight the unique opportunity to harness the unusual chemical bonding in PbSe and related IV–VI semiconductors for heterogeneously integrated mid-infrared light sources constrained by tight thermal budgets in new device designs.