Remote epitaxy is a promising approach for synthesizing exfoliatable crystalline membranes and enabling epitaxy of materials with large lattice mismatch. However, the atomic scale mechanisms for remote epitaxy remain unclear. Here we experimentally demonstrate that GaSb films grow on graphene-terminated GaSb (001) via a seeded lateral epitaxy mechanism, in which pinhole defects in the graphene serve as selective nucleation sites, followed by lateral epitaxy and coalescence into a continuous film. Remote interactions are not necessary in order to explain the growth. Importantly, the small size of the pinholes permits exfoliation of continuous, free-standing GaSb membranes. Due to the chemical similarity between GaSb and other III-V materials, we anticipate this mechanism to apply more generally to other materials. By combining molecular beam epitaxy with in-situ electron diffraction and photoemission, plus ex-situ atomic force microscopy and Raman spectroscopy, we track the graphene defect generation and GaSb growth evolution a few monolayers at a time. Our results show that the controlled introduction of nanoscale openings in graphene provides an alternative route towards tuning the growth and properties of 3D epitaxial films and membranes on 2D material masks.

This study presents the growth and characterization of an 8.1 μm-emitting, InGaAs/AlInAs/InP-based quantum cascade laser (QCL) formed on an InP-on-Si composite template by metalorganic chemical vapor deposition (MOCVD). First, for the composite-template formation, a GaAs buffer layer was grown by solid-source molecular-beam epitaxy on a commercial (001) GaP/Si substrate, thus forming a GaAs/GaP/Si template. Next, an InP metamorphic buffer layer (MBL) structure was grown atop the GaAs/GaP/Si template by MOCVD, followed by the MOCVD growth of the full QCL structure. The top-surface morphology of the GaAs/GaP/Si template before and after the InP MBL growth was assessed via atomic force microscopy, over a 100 μm2 area, and no antiphase domains were found. The average threading dislocation density (TDD) for the GaAs/GaP/Si template was found to be ∼1 × 109 cm−2, with a slightly lower defect density of ∼7.9 × 108 cm−2 after the InP MBL growth. The lasing performance of the QCL structure grown on Si was compared to that of its counterpart grown on InP native substrate and found to be quite similar. That is, the threshold-current density of the QCL on Si, for deep-etched ridge-guide devices with uncoated facets, is somewhat lower than that for its counterpart on native InP substrate, 1.50 vs 1.92 kA/cm2, while the maximum output power per facet is 1.64 vs 1.47 W. These results further demonstrate the resilience of QCLs to relatively high residual TDD values.

Room-temperature, pulsed-operation lasing of 8.5  μm-emitting InP-based quantum cascade lasers (QCLs), with low threshold-current density and watt-level output power, is demonstrated from structures grown on (001) GaAs substrates by metal-organic chemical vapor deposition. Prior to growing the laser structure, which contains a 35-stage In0.53Ga0.47As/In0.52Al0.48As lattice-matched active-core region, a ∼2  μm-thick nearly fully relaxed InP buffer with strained 1.6 nm-thick InAs quantum-dot-like dislocation-filter layers was grown. A smooth terminal buffer-layer surface, with roughness as low as 0.4 nm on a 10 × 10  μm2 scale, was obtained, while the estimated threading-dislocation density was in the mid-range × 108 cm−2. A series of measurements, on lasers grown on InP metamorphic buffer layers (MBLs) and on native InP substrates, were performed for understanding the impact of the buffer-layer's surface roughness, residual strain, and threading-dislocation density on unipolar devices such as QCLs. As-cleaved devices, grown on InP MBLs, were fabricated as 25  μm × 3 mm deep-etched ridge guides with lateral current injection. The results are pulsed maximum output power of 1.95 W/facet and a low threshold-current density of 1.86 kA/cm2 at 293 K. These values are comparable to those obtained from devices grown on InP: 2.09 W/facet and 2.42 kA/cm2. This demonstrates the relative insensitivity of the device-performance metrics on high residual threading-dislocation density, and high-performance InP-based QCLs emitting near 8  μm can be achieved on lattice-mismatched substrates.

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