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Functional thin film superlattices with stability in extreme environments can lead to transformative performance in optical and thermal applications such as thermophotovoltaics. In this work, key issues associated with defects that prevent layer-by-layer growth in epitaxial, low-miscibility oxide superlattices are investigated. Layer protrusions, approximately 8 nm wide and 3 nm thick, arise from a strain relaxation mechanism in 8 nm bilayer superlattices of Ba(Zr0.5Hf0.5)O3/MgO and propagate through the subsequent superlattice layers forming an inverted pyramid structure that is spatially phase offset from the matrix. The density and size of these defects scales with the number of interfaces in the sample, indicating that surface roughness during growth is a significant factor in the formation of these defects. In situ high temperature transmission electron microscopy (1000 °C, in vacuo) measurement reveals that phase decomposition of Ba(Zr0.5Hf0.5)O3 and decoherence of the superlattice is nucleated by these defects. This work highlights that achieving optimum growth conditions is imperative to the synthesis of single-crystalline superlattices with sharp interfaces for optimized performance in extreme environments. [ABSTRACT FROM AUTHOR]

One of the key materials of interest for p-type oxide semiconductor thin film electronics is cuprous oxide (Cu2O), due to its relatively high hole mobility. In this work, we use experiments, analytical models, and density functional theory calculations to study the scattering mechanisms that determine Hall mobility in two Cu2O samples. First, we examine a polycrystalline Cu2O thin film deposited by RF magnetron sputtering, and second, a single-crystalline Cu2O bulk substrate. Temperature-dependent Hall measurements indicate that neutral impurity and grain boundary scattering are dominant for the polycrystalline Cu2O thin film, while phonon scattering is dominant for single-crystalline Cu2O. Our first-principles calculations show that the room-temperature intrinsic hole mobility of Cu2O is 106 cm2 V−1 s−1, indicating the great promise of the material for p-type electronic devices. This intrinsic mobility is limited by phonon scattering, with the most dominant scattering modes having phonon energies of 88.4 and 17.1 meV. These results indicate that the key pathways to increase the hole mobility in Cu2O thin films are by reducing the impurity concentration and by increasing grain size. Our work thus sets the stage for the future development of high performance Cu2O-based p-type thin film transistors. [ABSTRACT FROM AUTHOR]

The II-IV-N2 class of heterovalent ternary nitrides has gained significant interest as alternatives to the III-nitrides for electronic and optoelectronic applications. In this study, we apply first-principles calculations based on density functional theory to systematically investigate the effects of structural distortions due to cation size mismatch on the configurational disorder of the cation sublattice and the valence band structure in this class of materials. We find that larger size mismatch between the group-II and the group-IV cations results in stronger lattice distortions from the ideal hexagonal ratio, which in turn inhibits the propensity of these materials toward octet-rule violating cation disorder. We also demonstrate that the formation energy of a single cation antisite pair, which is fast and simple to calculate, is a strong indicator of a material's propensity toward disorder. Furthermore, the breaking of in-plane symmetry leads to a splitting of the top three valence bands at Γ , which is also directly related to the magnitude of structural distortions. Our work demonstrates that the structural and functional properties of the II-IV-N2 materials can be finely tuned through controllable structural distortions that stem from the choice of cations. [ABSTRACT FROM AUTHOR]

Ultrawide-band-gap (UWBG) semiconductors are promising for fast, compact, and energy-efficient power-electronics devices. Their wider band gaps result in higher breakdown electric fields that enable high-power switching with a lower energy loss. Yet, the leading UWBG semiconductors suffer from intrinsic materials' limitations with regard to their doping asymmetry that impedes their adoption in CMOS technology. Improvements in the ambipolar doping of UWBG materials will enable a wider range of applications in power electronics as well as deep-UV optoelectronics. These advances can be accomplished through theoretical insights on the limitations of current UWBG materials coupled with the computational prediction and experimental demonstration of alternative UWBG semiconductor materials with improved doping and transport properties. As an example, we discuss the case of rutile GeO2 (r-GeO2), a water-insoluble GeO2 polytype, which is theoretically predicted to combine an ultra-wide gap with ambipolar dopability, high carrier mobilities, and a higher thermal conductivity than β-Ga2O3. The subsequent realization of single-crystalline r-GeO2 thin films by molecular beam epitaxy provides the opportunity to realize r-GeO2 for electronic applications. Future efforts toward the predictive discovery and design of new UWBG semiconductors include advances in first-principles theory and high-performance computing software, as well as the demonstration of controlled doping in high-quality thin films with lower dislocation densities and optimized film properties. [ABSTRACT FROM AUTHOR]

Lanthanum nitride (LaN) has attracted research interest in catalysis due to its ability to activate the triple bonds of N2 molecules, enabling efficient and cost-effective synthesis of ammonia from N2 gas. While exciting progress has been made to use LaN in functional applications, the electronic character of LaN (metallic, semi-metallic, or semiconducting) and magnitude of its bandgap have so far not been conclusively determined. Here, we investigate the electronic properties of LaN with hybrid density functional theory calculations. In contrast to previous claims that LaN is semi-metallic, our calculations show that LaN is a direct-bandgap semiconductor with a bandgap value of 0.62 eV at the X point of the Brillouin zone. The dispersive character of the bands near the band edges leads to light electron and hole effective masses, making LaN promising for electronic and optoelectronic applications. Our calculations also reveal that nitrogen vacancies and substitutional oxygen atoms are two unintentional shallow donors with low formation energies that can explain the origin of the previously reported electrical conductivity. Our calculations clarify the semiconducting nature of LaN and reveal candidate unintentional point defects that are likely responsible for its measured electrical conductivity. [ABSTRACT FROM AUTHOR]

A fundamental understanding and control of impurity incorporation and charge carrier recombination are critical for emerging ScxAl1−xN electronics, optoelectronics, and photonics. We report on the photoluminescence properties of ScxAl1−xN grown by plasma-assisted molecular beam epitaxy with varying growth temperatures and Sc contents. Bright and broad emission comprising a dominant peak at ∼3.52 eV and a weak peak at ∼2.90 eV was observed in Sc0.05Al0.95N. The origin of the ∼3.52 eV emission line is attributed to charge carrier recombination from the localized excited state of (Vcation-ON)2−/− to its ground state, whereas the second peak at ∼2.90 eV results from charge carrier recombination of isolated V cation 3 − / 2 − to the valence band. We further show that oxygen defect-related emission can be significantly suppressed by increasing growth temperature. This work sheds light on the recombination dynamics of photoexcited carriers in ScxAl1−xN and further offers insight into how to improve the optical and electrical properties of ScxAl1−xN that are relevant for a broad range of applications. [ABSTRACT FROM AUTHOR]

We calculate the alloy-disorder-limited electron mobility of AlxGa1−xN from first principles. AlxGa1−xN is a technologically important ultra-wide-bandgap alloy with promise in light emitting diodes and high-power transistors. Alloying introduces statistical disorder, which causes electrons to scatter between different crystal-momentum states, leading to a reduction in mobility for intermediate alloy compositions. The corresponding lifetime, which appears as an energy broadening in the band structure, can be evaluated by unfolding the band structure from the supercell basis to the primitive-cell basis. We fit the first-principles band broadening with a model scattering potential and evaluate the low-field electron mobility using the semiclassical Boltzmann transport equation in the relaxation-time approximation. Our calculated mobility is in agreement with experimental values. We also find the lowest alloy-scattering electron mobility (total electron mobility) across the entire composition range to be 186 c m 2 / V s (136 c m 2 / V s), which is comparable to the highest electron mobility predicted in the competitor system, β- (Al x Ga 1 − x) 2 O 3 . Our results elucidate the intrinsic limits imposed by alloy disorder on electron transport in AlxGa1−xN. [ABSTRACT FROM AUTHOR]