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  1. U Doped GaN Publication

    Gallium nitride (GaN) is near ubiquitous in modern day technologies forming the backbone of solid-state lighting and high-power electronics. Engineering the physical properties of GaN has been investigated to some degree by the incorporation or doping of most of the elements of the periodic table, but the actinides remain unexplored. Molecular beam epitaxy is used to demonstrate uranium doping of GaN single crystals. High structural quality of the host matrix is maintained despite partial elemental segregation of the uranium dopant into 1D structures at the levels presented here. Electronic transport measurements reveal relatively high conductivity, which persists down to cryogenicmore » temperature and characterized by the formation of narrow gaps in the electronic band structures very close to the Fermi level. Photoluminescence measurements reveal the U-doped GaN exhibits optical behavior similar to that of the GaN substrate. The addition of actinide materials to a non-centrosymmetric, optically active, radiation hard, and electronically tunable host matrix opens a world of possibilities for investigating and leveraging elements with high electron correlations in the pursuit of novel devices.« less
  2. Strain and Defect-Tailored Magnetotransport in NiCo2O4 Thin Films and Freestanding Membranes

    Magnetic spinel NiCo2O4 is promising for developing spintronic applications due to its high magnetic Curie temperature, high spin polarization, fast spin dynamics, and strain-tunable magnetic anisotropy, while its electronic and magnetic properties depend sensitively on epitaxial strain and disorder. Here, we use epitaxial NiCo2O4 thin films and freestanding NiCo2O4 membranes as model systems to reveal the complex interplay of strain and defects in determining the metallicity and magnetotransport properties of the ferrimagnetic spinel. NiCo2O4 on perovskite substrates and NiCo2O4 membranes exhibit insulating behaviors and spin canting, in sharp contrast to the metallic NiCo2O4 films on spinel substrates that possess strongmore » perpendicular magnetic anisotropy. Anisotropic magnetoresistance studies provide critical information about disorder-induced spin scattering and strain-induced tetragonal magnetocrystalline anisotropy, which is corroborated by comprehensive electron microscopy characterizations. Here, our study presents a promising venue for designing flexible magnetic memory, sensor, and spintronic applications.« less
  3. Programmable Phase Selection between Altermagnetic and Noncentrosymmetric Polymorphs of MnTe on InP via Molecular Beam Epitaxy

    Phase selecting nearly degenerate crystalline polymorphs during epitaxial growth can be challenging yet critical to targeting physical properties for specific applications. Here, we establish how phase selectivity of altermagnetic and noncentrosymmetric polymorphs of MnTe can be programmed by subtle changes to the surface of lattice-matched InP substrates in molecular beam epitaxy growth. Bulk altermagnetic MnTe is thermodynamically stable in the hexagonal NiAs-structure and is synthesized here on the polar (111)A surface (In-terminated) of InP, while the noncentrosymmetric, cubic ZnS-structure with wide band gap (>3 eV), which epitaxially matches III–V materials, is stabilized on the (111)B surface (P-terminated). Electron microscopy, X-raymore » photoemission spectroscopy, and reflection high-energy electron diffraction indicate that phase selection is triggered at the interface and proceeds along the growing surface. First-principles calculations suggest that interfacial termination and strain have a significant effect on the interfacial energy; stabilizing the NiAs polymorph on the In-terminated surface and the ZnS structure on the P-terminated surface. Here, selectively grown, high-quality, phase pure films of both MnTe polymorphs will enable our understanding of the novel properties of these materials, thereby facilitating their use in new applications ranging from spintronics to microelectronic devices.« less
  4. Origins of anisotropic linear magnetoresistance with isotropic mobility in Cd3As2 films on GaAs$[110]$

    Thin film synthesis allows for the potential to orient crystals in different orientations, permitting measurement of orientation-dependent material aspects such as band structures and transport anisotropy. Here, Dirac semimetal Cd3As2 films are epitaxially grown on GaAs$[110]$ substrates, which has a $[001]$ orientation in-plane. Films contain domains of two different c-axis orientations resulting from an aligned a-axis in-plane. Magnetoresistance measurements performed along both $$[1\bar{1}0]$$ and $[001]$ substrate directions reveal similar mobility and carrier concentration, but much larger magnetoresistance along the $[001]$ direction, which can be explained by the guiding center diffusion model as arising from anisotropic disorder and different atomic spacings.
  5. Epitaxial Electrodeposition of Fe with Controlled In-Plane Variants for a Reversible Metal Anode in an Aqueous Electrolyte

    The development of reversible metal anodes is a key challenge for advancing aqueous battery technologies, particularly for scalable and safe stationary energy storage applications. Here, in this study, we demonstrate a strategy to realize epitaxial electrodeposition of iron (Fe) on single-crystal copper (Cu) substrates in aqueous electrolytes. We compare the electrodeposition behavior of Fe on polycrystalline and single-crystalline Cu substrates, revealing that the latter enables highly uniform, dense, and crystallographically aligned Fe growth. Comprehensive electron backscatter diffraction (EBSD) and X-ray diffraction (XRD) analysis confirms the formation of Fe with specific out-of-plane and in-plane orientations, including well-defined rotational variants. Our findingsmore » highlight that epitaxial electrodeposition of Fe can suppress dendritic growth and significantly enhance Coulombic efficiency during plating/stripping cycles. This approach bridges fundamental crystallography with practical electrochemical performance, providing a pathway toward high-efficiency aqueous batteries utilizing Earth-abundant materials.« less
  6. Hybrid MBE Route to Adsorption-Controlled Growth of BaTiO3 Membranes with Robust Polarization Switching

    Freestanding ferroelectric membranes are promising for flexible electronics, nonvolatile memory, photonics, and spintronics, but their synthesis is challenged by the need for reproducibility with precise stoichiometric control. Here, we demonstrate the adsorption-controlled growth of single-crystalline, epitaxial BaTiO3 films by hybrid molecular beam epitaxy (MBE) on a binary oxide sacrificial layer. Using a simple water-droplet lift-off method, we obtained submillimeter- to millimeter-sized membranes that retained crystallinity, as confirmed by high-resolution X-ray diffraction, and exhibited robust tetragonal symmetry, as verified by Raman spectroscopy. Impedance spectroscopy confirmed a high dielectric constant of ∼1340, reflecting the robust dielectric response of the membranes. Ferroelectric functionalitymore » was revealed by piezoresponse force microscopy (PFM) and further verified by polarization-electric field (P-E) loop measurements with Positive-Up-Negative-Down (PUND). The P-E loops exhibited a remnant polarization of ∼5 μC cm–2 and a coercive field of ∼63 kV cm–1. Furthermore, these results were interpreted in relation to c- and a-domain configurations.« less
  7. How transparent is graphene? A surface science perspective on remote epitaxy

    Remote epitaxy is the synthesis of a single crystalline film on a graphene-covered substrate, where the film adopts epitaxial registry to the substrate as if the graphene is transparent. Despite many exciting applications for flexible electronics, strain engineering, and heterogeneous integration, an understanding of the fundamental synthesis mechanisms remains elusive. Here we offer a perspective on the synthesis mechanisms, focusing on the foundational assumption of graphene transparency. We identify challenges for quantifying the strength of the remote substrate potential that permeates through graphene, and propose Fourier and beating analysis as a bias-free method for decomposing the lattice potential contributions frommore » the substrate, from graphene, and from surface reconstructions, each at different frequencies. We highlight the importance of graphene-induced reconstructions on epitaxial templating, drawing comparison to moiré epitaxy. We highlight the role of the remote potential in tuning surface diffusion and adatom kinetics on graphene, which are crucial for navigating the competition between remote epitaxy and defect-seeded mechanisms like pinhole epitaxy. In light of this weak remote potential, we re-evaluate the current state-of-the-art experimental evidence, highlighting why it remains challenging to experimentally validate a ‘remote’ epitaxy mechanism that cannot be explained by alternatives, such as pinhole-seeded epitaxy or serial van der Waals epitaxy. We end with one experimental example that, to out knowledge, cannot be explained by competing mechanisms: a different long-range epitaxial relationship for GdPtSb films grown on graphene/sapphire, compared to direct epitaxy on sapphire. We suggest for future experiments that directly measure the remote potential and impact of tuneable growth kinetics.« less
  8. Ferroelectric Switching in Hybrid Molecular-Beam-Epitaxy-Grown BaTiO3 Films

    Molecular beam epitaxy (MBE) is a promising synthesis technique for both heterostructure growth and epitaxial integration of ferroelectric BaTiO3. However, direct measurement of the remnant polarization (Pr) has not been previously reported in MBE-grown BaTiO3 films. We report the in situ growth of an all-epitaxial SrRuO3/BaTiO3/SrRuO3 heterostructure on Nb-doped SrTiO3 (001) substrates by hybrid MBE using metal–organic precursors. This capacitor structure consisting of 16 nm SrRuO3/40 nm BaTiO3/16 nm SrRuO3 shows hysteretic polarization–electric field (P–E) curves with Pr ∼ 15 μC cm–2 at frequencies ranging from 500 Hz to 20 kHz, after isolating the intrinsic ferroelectric response from non-ferroelectric contributionsmore » using the Positive-Up-Negative-Down (PUND) method. We hypothesize that the asymmetry in switching behavior and current leakage has origins in structural defects. Furthermore, this work opens the door to defect-engineered ferroelectric BaTiO3-based heterostructures grown by hybrid MBE for future electronic, photonic and spintronic applications.« less
  9. Growth and Characterization of Epitaxial FeWO4 Thin Films with Controlled Oxygen Stoichiometry

    Here, we report the growth of single-phase epitaxial FeWO4 thin films, using plasma-assisted molecular beam epitaxy, and investigate structural, optical, and electronic properties. The FeWO4 films grow in (100) orientation on c-plane sapphire (0001) substrates and exhibit 3 rotational twin variants where FeWO4 [001] is aligned to sapphire [100] equivalent in-plane directions. X-ray diffraction measurements indicate that the epitaxial FeWO4 (100) structure is optimized when 80-100 W of rf power is applied to an atomic oxygen source during growth, yielding films with minimal strain and impurity phases or other orientations. In films grown with 120 W of rf power, FeWO4more » crystallites develop inhomogeneous and homogeneous strains and are potentially contaminated with Fe3+ oxide phase impurities. In films grown with 60 W of rf power, FeWO4 crystallites do not form fully epitaxial layers. X-ray photoelectron spectroscopy indicates that the structural changes are correlated with the Fe3+/Fe2+ oxidation state ratio increasing from 0.6-1.4 with rf power from 60-120 W. X-ray fluorescence spectroscopy indicates that the Fe/W composition ratio is also increasing from 1.1-1.8 with rf power from 60-120 W. Ultraviolet and visible optical absorption spectra indicate a 1.8 ± 0.1 eV band gap with an additional interband absorption feature at 3.1 ± 0.1 eV in the 80-100 W films, with similar onsets observed in the 60 W films. In the 120 W films, the higher lying transition is shifted to 2.7 ± 0.1 eV due to the Fe3+ enrichment. Electrical resistivity decreases over 2 orders of magnitude with oxidation from 104-105 Ω cm in 60 W films to 120 ± 10 Ω cm in 120 W films. Thermopower measurements show p-type to n-type conductivity conversion when oxidation states shift from Fe2+ majority in the 100 W films to Fe3+ majority in the 120 W films. We conclude that electron polaron hopping driven by Fe3+ is a dominant transport mechanism and a source of n-type conductivity in overoxidized FeWO4 films.« less
  10. Epitaxial stabilization and oxygen vacancy control of EuNiO3 thin films

    Rare-earth nickelates exhibit valuable behavior for neuromorphic computing at low temperature: Building blocks for biologically inspired microelectronic neurons like electrically driven insulator–metal transitions (IMTs), negative differential resistance, and self-oscillations have been shown up to 230 K for SmNiO3 and NdNiO3. EuNiO3 raises the IMT far above room temperature (460 K) but high-quality thin films are challenging to synthesize. Here, we explore the epitaxial stabilization of EuNiO3 using pulsed laser deposition. X-ray diffraction reciprocal space maps, x-ray absorption spectroscopy, and transmission electron microscopy show that higher growth temperature (800 °C) reduces oxygen vacancy concentrations in EuNiO3. Pseudomorphic EuNiO3 is demonstrated onmore » both SrLaAlO4 and NdGaO3 substrates, and LaNiO3 buffer layers are incorporated to facilitate future vertical device fabrication. In contrast to bulk thermodynamic predictions, the greater oxidation and crystallinity at higher temperature we observe indicates that epitaxial substrates can stabilize EuNiO3 at O2 pressures less than 1 atm.« less
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