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Bulk PbSnSe has a two-phase region or miscibility gap as the crystal changes from a Van der Waals-bonded orthorhombic 2D layered structure in SnSe-rich compositions to the related 3D-bonded rocksalt structure in PbSe-rich compositions with large contrast in the electrical, optical, and thermal properties across this transition. With an aim to understand and harness this transition in thin films devices, we epitaxially integrate PbSnSe on GaAs by molecular beam epitaxy using an in-situ PbSe surface treatment and show a significantly reduced two-phase region by stabilizing the Pnma layered structure out to Pb$_{0.45}$Sn$_{0.55}$Se, beyond the bulk-limit of Pb$_{0.25}$Sn$_{0.75}$Se. Pushing further, we directly access metastable two-phase epitaxial films of layered and rocksalt grains that are nearly identical in composition around Pb$_{0.5}$Sn$_{0.5}$Se and entirely circumvent the miscibility gap. We present microstructural evidence for an incomplete displacive transformation from rocksalt to layered structure in these films that we speculate occurs during the sample cool down to room temperature after synthesis. In situ temperature-cycling experiments on a Pb$_{0.58}$Sn$_{0.42}$Se rocksalt film reproduce characteristic attributes of a displacive transition and show a modulation in electronic properties. We find well-defined orientation relationships between the phases formed and reveal unconventional strain relief mechanisms involved in the crystal structure transformation, using transmission electron microscopy. Overall, our work adds a scalable thin film integration route to harnessing the dramatic contrast in material properties in PbSnSe across a potentially ultrafast structural transition., Comment: 29 pages, 11 figures

We report on photoluminescence in the 3-7 $\mu$m 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 {\deg}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 $10^9$ $cm^{-2}$ 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 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, though 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., Comment: 24 pages, 6 figures

We present an infrared photodetector leveraging an all-epitaxial device architecture consisting of a 'designer' plasmonic metal integrated with a quantum-engineered detector structure, all in a mature III-V semiconductor material system. Incident light is coupled into surface plasmon-polariton modes at the detector/'designer' metal interface, and the strong confinement of these modes allows for a sub-diffractive ($\sim \lambda_0 / 33$) detector absorber layer thickness, effectively decoupling the detector's absorption efficiency and dark current. We demonstrate high-performance detectors operating at non-cryogenic temperatures (T = 195 K), without sacrificing external quantum efficiency, and superior to well established and commercially-available detectors. This work provides a practical and scalable plasmonic optoelectronic device architecture with real world mid-infrared applications.

Remarkable systems have been reported recently using the polylithic integration of semiconductor optoelectronic devices and plasmonic materials exhibiting epsilon-near-zero (ENZ) and negative permittivity. In traditional noble metals, the ENZ and plasmonic response is achieved near their plasma frequencies, limiting plasmonic optoelectronic device design flexibility. Here, we leverage an all-epitaxial approach to monolithically and seamlessly integrate designer plasmonic materials into a quantum dot light emitting diode (LED), leading to a ~5.6 x enhancement over an otherwise identical non-plasmonic control sample. Devices exhibited optical powers comparable, and temperature performance far superior, to commercially-available devices., Comment: Journal letter, four pages, five figures