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Chalcogenide perovskites such as BaZrS3 are promising candidates for next generation optoelectronics such as photodetectors and solar cells. Compared to widely studied polycrystalline thin films, single crystals of BaZrS3 with minimal extended and point defects, are ideal platform to study the material's intrinsic transport properties and to make first-generation optoelectronic devices. However, the surface dielectrics formed on BaZrS3 single crystals due to sulfating or oxidation have led to significant challenges to achieving high quality electrical contacts, and hence, realizing the high-performance optoelectronic devices. Here, we report the development of electrical contact fabrication processes on BaZrS3 single crystals, where various processes were employed to address the surface dielectric issue. Moreover, with optimized electrical contacts fabricated through dry etching, high-performance BaZrS3 photoconductive devices with a low dark current of 0.1 nA at 10 V bias and a fast transient photoresponse with rise and decay time of <0.2 s were demonstrated.

We present a general fabrication strategy for freestanding single-crystalline complex oxide device arrays via wet chemical etching-based microfabrication processes and epitaxial lift-off. Here, we used 0.5Ba(Zr$_{0.2}$Ti$_{0.8}$)O$_3$-0.5Ba(Zr$_{0.7}$Ti$_{0.3}$)O$_3$ (BCZT) as a model relaxor ferroelectric oxide system and La$_{0.7}$Sr$_{0.3}$MnO$_3$ as the sacrificial layer for demonstration. Arrays of SrRuO$_3$ (SRO) / BCZT / SRO ferroelectric capacitor mesas were first defined and isolated on the growth wafer, and then they were released using epitaxial lift-off with lithography-defined surrounding etching holes, after which the freestanding device arrays were integrated onto a glass substrate. Our proposed strategy sheds light on preparing various freestanding single-crystalline oxide devices and paves the way for their heterogeneous integration onto arbitrary substates.

Atomistic origin of stacking faults in non-close packed systems is a fundamentally distinct mechanism from the well-known close packed structures with ABC stacking, and represents an uncharted territory in material research. According to experimental data, stacking faults in simple hexagonal WC happen in {1-100} planes that are packed rectangularly and have ABAB stacking. This work identified the type of the defect and crystallographic behaviour by creating energetically relaxed potential atomistic models of stacking faults in WC. Experimental evidence supporting the rotation axis along stacking fault caused by variation in carbon ordering at the interstitial site has been established, in accordance with the theoretical model.

Ferroelectricity is characterized by the presence of spontaneous and switchable macroscopic polarization. Scaling limits of ferroelectricity have been of both fundamental and technological importance, but the probes of ferroelectricity have often been indirect due to confounding factors such as leakage in the direct electrical measurements. Recent interest in low-voltage switching electronic devices squarely puts the focus on ultrathin limits of ferroelectricity in an electronic device form, specifically on the robustness of ferroelectric characteristics such as retention and endurance for practical applications. Here, we illustrate how manipulating the kinetic energy of the plasma plume during pulsed laser deposition can yield ultrathin ferroelectric capacitor heterostructures with high bulk and interface quality, significantly low leakage currents and a broad "growth window". These heterostructures venture into previously unexplored aspects of ferroelectric properties, showcasing ultralow switching voltages ($<$0.3 V), long retention times ($>$10$^{4}$s), and high endurance ($>$10$^{11}$cycles) in 20 nm films of the prototypical perovskite ferroelectric, BaTiO$_{3}$. Our work demonstrates that materials engineering can push the envelope of performance for ferroelectric materials and devices at the ultrathin limit and opens a direct, reliable and scalable pathway to practical applications of ferroelectrics in ultralow voltage switches for logic and memory technologies.

Low-weight, passive, thermal-adaptive radiation technologies are needed to maintain an operable temperature for spacecraft while they experience various energy fluxes. In this study, we used a thin-film coating with the Fabry-Perot (FP) effect to enhance emissivity contrast ({\Delta}{\epsilon}) between VO2 phase-change states. This coating utilizes a novel hybrid material architecture that combines VO2 with a mid- and long-wave infrared transparent chalcogenide, zinc sulfide (ZnS), as a cavity spacer layer. We simulated the design parameter space to obtain a theoretical maximum {\Delta}{\epsilon} of 0.63 and grew prototype devices. Using X-ray diffraction, Raman spectroscopy, and Fourier Transform Infrared (FTIR) Spectroscopy, we determined that an intermediate buffer layer of TiO2 is necessary to execute the crystalline growth of monoclinic VO2 on ZnS. Through temperature-dependent FTIR spectroscopy measurements, our fabricated devices demonstrated FP-cavity enhanced adaptive thermal emittance., Comment: 16 pages, 5 figures, full article

A key open question in the study of layered superconducting nickelate films is the role that hydrogen incorporation into the lattice plays in the appearance of the superconducting state. Due to the challenges of stabilizing highly crystalline square planar nickelate films, films are prepared by the deposition of a more stable parent compound which is then transformed into the target phase via a topotactic reaction with a strongly reducing agent such as CaH$_2$. Recent studies, both experimental and theoretical, have introduced the possibility that the incorporation of hydrogen from the reducing agent into the nickelate lattice may be critical for the superconductivity. In this work, we use secondary ion mass spectrometry to examine superconducting La$_{1-x}$X$_x$NiO$_2$ / SrTiO$_3$ (X = Ca and Sr) and Nd$_6$Ni$_5$O$_{12}$ / NdGaO$_3$ films, along with non-superconducting NdNiO$_2$ / SrTiO$_3$ and (Nd,Sr)NiO$_2$ / SrTiO$_3$. We find no evidence for extensive hydrogen incorporation across a broad range of samples, including both superconducting and non-superconducting films. Theoretical calculations indicate that hydrogen incorporation is broadly energetically unfavorable in these systems, supporting our conclusion that hydrogen incorporation is not generally required to achieve a superconducting state in layered square-planar nickelates., Comment: 23 pages, 21 figures (including supplemental information)

Rare earth dopants are one of the most extensively studied optical emission centers for a broad range of applications such as laser optoelectronics, sensing, lighting, and quantum information technologies due to their narrow optical linewidth and exceptional coherence properties. Epitaxial doped oxide thin films can serve as a promising and controlled host to investigate rare-earth dopants suitable for scalable quantum memories, on-chip lasers and amplifiers. Here, we report high-quality epitaxial thin films of Tm-doped CaZrO$_3$ grown by pulsed laser deposition for infrared optoelectronic and quantum memory applications. We perform extensive structural and chemical characterization to probe the crystallinity of the films and the doping behavior. Low temperature photoluminescence measurements show sharp radiative transitions in the short-wave infrared range of 1.75 - 2 \mu m., Comment: 17 pages, 4 figures

Insulating materials featuring ultralow thermal conductivity for diverse applications also require robust mechanical properties. Conventional thinking, however, which correlates strong bonding with high atomic-vibration-mediated heat conduction, led to diverse weakly bonded materials that feature ultralow thermal conductivity and low elastic moduli. One must, therefore, search for strongly-bonded single crystals in which heat transport is impeded by other means. Here, we report intrinsic, glass-like, ultralow thermal conductivity and ultrahigh elastic-modulus/thermal-conductivity ratio in single-crystalline Ruddlesden-Popper Ban+1ZrnS3n+1, n = 2,3, which are derivatives of BaZrS3. Their key features are strong anharmonicity and intra-unit-cell rock-salt blocks. The latter produce strongly bonded intrinsic superlattices, impeding heat conduction by broadband reduction of phonon velocities and mean free paths and concomitant strong phonon localization. The present study initiates a paradigm of mechanically stiff phonon glasses.

Vapor-pressure mismatched materials such as transition metal chalcogenides have emerged as electronic, photonic, and quantum materials with scientific and technological importance. However, epitaxial growth of vapor-pressure mismatched materials are challenging due to differences in the reactivity, sticking coefficient, and surface adatom mobility of the mismatched species constituting the material, especially sulfur containing compounds. Here, we report a novel approach to grow chalcogenides - hybrid pulsed laser deposition - wherein an organosulfur precursor is used as a sulfur source in conjunction with pulsed laser deposition to regulate the stoichiometry of the deposited films. Epitaxial or textured thin films of sulfides with variety of structure and chemistry such as alkaline metal chalcogenides, main group chalcogenides, transition metal chalcogenides and chalcogenide perovskites are demonstrated, and structural characterization reveal improvement in thin film crystallinity, and surface and interface roughness compared to the state-of-the-art. The growth method can be broadened to other vapor-pressure mismatched chalcogenides such as selenides and tellurides. Our work opens up opportunities for broader epitaxial growth of chalcogenides, especially sulfide-based thin film technological applications., Comment: 27 pages

It is well known that a magnetic monopole-electric charge system carries an angular momentum in its electromagnetic fields. Here we show that in the Dirac string formulation of magnetic charge the monopole-electric charge system also carries a momentum in its electromagnetic fields. This overlooked field momentum arises from the Coulomb electric field of the electric charge and the solenoidal magnetic field of the Dirac string. This implies that the monopole-charge system must either: (i) carry a ``hidden momentum" in the string, indicating that the string is real, or (ii) that the monopole-charge system violates the center-of-energy theorem. The overall conclusion is that the Dirac monopole with a {\it regulated} Dirac string is not a true monopole, and is not even a good effective description for topological monopoles ({\it e.g.} the 't Hooft-Polyakov monopole outside the core)., Comment: 8 pages, no figures, revtex-4, published Phys. Rev. D

The Wu-Yang fiber bundle approach to magnetic charge is extended with a disk-like sheet current density and associated magnetic field in the overlap region between the Northern hemisphere and Southern hemisphere, where the different vector potentials connect. This disk magnetic field plays a role similar to the Dirac string in the Dirac approach to magnetic charge - it brings an inward magnetic flux of $4 \pi g$ which then gives rise to an outward Coulomb magnetic flux of $4 \pi g$. As with the Dirac string approach we show that placing an electric charge near this disk magnetic field gives rise to a non-zero electromagnetic field momentum. We discuss some of the possible physical consequences of this electromagnetic field momentum. We conclude by showing that the non-singular, but non-single valued Banderet monopole potential also has a disk-like magnetic flux and non-zero electromagnetic field momentum in the presence of an electric charge., Comment: 16 pages, 3 figures EPS figures, revtex-4. Changes in text to take into account referee comments/suggestions. To be published in Annals of Physics