Here we investigate stripes of alternating structural phases spontaneously forming in epitaxially strained Ca_2RuO_4 thin films below the metal-insulator transition. Using large-volume X-ray reciprocal-space mapping, we show that satellite-pattern intensities across 24 symmetry-inequivalent Bragg reflections collapse onto a single parameter-free curve. The collapse identifies a coherent martensitic laminate of few-nm-wide domains separated by 012 interfaces, with displacements along ⟨012̅⟩. Satellite-extinction analysis demonstrates that both coexisting phases retain the bulk orthorhombic space group despite the pseudocubic LaAlO_3 substrate, biaxial epitaxial strain, and intrinsic strain at the interfaces. Classical invariant-plane-strain crystallography thus governs the nanoscale domain geometry of a Mott insulator with intertwined magnetic, electronic, and lattice order.

Tantalum dioxide (TaO2) is a metastable tantalum compound. Here, we report the epitaxial stabilization of TaO2 on Al2O3 (1102) (r-plane sapphire) substrates using suboxide molecular-beam epitaxy and thermal laser epitaxy, demonstrating single-oriented, monodomain growth of anisotropically strained thin films. Microstructural investigation is performed using synchrotron x-ray diffraction and scanning transmission electron microscopy. The tetravalent oxidation state of tantalum is confirmed using x-ray absorption and photoemission spectroscopy as well as electron energy-loss spectroscopy. Optical properties are investigated via spectroscopic ellipsometry and reveal a 0.3 eV Mott gap of the tantalum 5d electrons. Density-functional theory and group theoretical arguments are used to evaluate the limited stability of the rutile phase and reveal the potential to unlock a hidden metal-insulator transition concomitant with a structural phase transition to a distorted rutile phase, akin to NbO2. Our study expands the understanding of tantalum oxides and paves the way for their integration into next-generation electronic and photonic devices.

Excitement about the magnetic and electronic properties of RuO_2 is growing, fueled by reports of antiferromagnetism, strain-induced superconductivity, and its recent classification as a member of a newly proposed magnetic class, altermagnets, with RuO_2 widely regarded as the paradigmatic example. Nevertheless, the magnetic ground state of RuO_2 remains contentious, as several recent experiments report no evidence of magnetic order. To address this discrepancy, we performed resonant elastic scattering measurements on a series of epitaxial RuO_2 thin films grown on the (100)-plane of TiO_2 substrates across a range of strain states. Leveraging full polarization control and azimuthal scans of the structurally forbidden 100 Bragg reflection, we systematically tested for signatures of colinear antiferromagnetic order. We found that the resonant elastic scattering signal in RuO_2 thin films likely originates from anisotropic charge scattering, not long-range antiferromagnetic order. Using angle-resolved photoemission spectroscopy we uncover a band structure without altermagnetic band splitting that is consistent with a nonmagnetic phase. Similarly, anisotropic magnetoresistance results show no evidence of magnetism. The combination of three independent measurements suggests the absence of altermagnetism in RuO_2.

Recently, superconductivity was discovered with a superconducting transition temperature (Tc) of 2 K in strained (110)-oriented RuO2 films grown on TiO2(110) single-crystal substrates. In this work, we predict and realize superconductivity in strained (100)-oriented RuO2 thin films grown on TiO2(100) single-crystal substrates. We show that while density functional theory predicts the Tc of strained RuO2(100) films to be even higher than the RuO2(110) films, our transport and angle-resolved photoemission spectroscopy measurements find the Tc to be about 1 K in strained RuO2(100) films grown on TiO2(100) substrates. Nonetheless, the thickness dependence of the Tc follows a similar trend in both cases. Our scanning SQUID measurements reveal a local superfluid response, indicating a 100 mK inhomogeneity in Tc over a 100 μm scale. Ruthenium oxide has attracted recent interest as a non-superconducting material where superconductivity can be induced by epitaxial strain. Here, the authors explore strained (100)-oriented RuO2 films on TiO2(100) substrate and reveal strain-induced superconductivity similarly to strained RuO2(110) films, providing insights into the thickness-dependence and electronic structure mechanisms of superconductivity.

Strong coupling between polarization (P) and strain (ɛ) in ferroelectric complex oxides offers unique opportunities to dramatically tune their properties. Here colossal strain tuning of ferroelectricity in epitaxial KNbO3 thin films grown by sub-oxide molecular beam epitaxy is demonstrated. While bulk KNbO3 exhibits three ferroelectric transitions and a Curie temperature (Tc) of ≈676 K, phase-field modeling predicts that a biaxial strain of as little as -0.6% pushes its Tc > 975 K, its decomposition temperature in air, and for -1.4% strain, to Tc > 1325 K, its melting point. Furthermore, a strain of -1.5% can stabilize a single phase throughout the entire temperature range of its stability. A combination of temperature-dependent second harmonic generation measurements, synchrotron-based X-ray reciprocal space mapping, ferroelectric measurements, and transmission electron microscopy reveal a single tetragonal phase from 10 K to 975 K, an enhancement of ≈46% in the tetragonal phase remanent polarization (Pr), and a ≈200% enhancement in its optical second harmonic generation coefficients over bulk values. These properties in a lead-free system, but with properties comparable or superior to lead-based systems, make it an attractive candidate for applications ranging from high-temperature ferroelectric memory to cryogenic temperature quantum computing.

Quasi van der Waals Epitaxy (qvdWE) has been realized for decades at the interfaces between 3D and 2D materials or van der Waals materials. The growth of magnetic topological insulators (MTI) Cr: (BixSb1-x)2Te3 (CBST) on GaAs (111) substrates for Quantum Anomalous Hall Effect (QAH) is actually one of the examples of qvdWE, which is not well noticed despite the fact that its advantages have been used in growth of various MTI materials. This is distinguished from the growth of MTIs on other substrates. Although the qvdWE mode has been used in many 2D growth on III-V substrates, the specific features and mechanisms are not well demonstrated and summarized yet. Here in this work, we have for the first time shown the features of both coherent interfaces and the existence of strain originating from qvdWE at the same time.

Unlike naturally occurring oxide crystals such as ruby and gemstones, there are no naturally occurring nitride crystals because the triple bond of the nitrogen molecule is one of the strongest bonds in nature. Here, we report that when the transition metal scandium is subjected to molecular nitrogen, it self-catalyzes to break the nitrogen triple bond to form highly crystalline layers of ScN, a semiconductor. This reaction proceeds even at room temperature. Self-activated ScN films have a twin cubic crystal structure, atomic layering, and electronic and optical properties comparable to plasma-based methods. We extend our research to showcase Sc’s scavenging effect and demonstrate self-activated ScN growth under various growth conditions and on technologically significant substrates, such as 6H–SiC, AlN, and GaN. Ab initio calculations elucidate an energetically efficient pathway for the self-activated growth of crystalline ScN films from molecular N2. The findings open a new pathway to ultralow-energy synthesis of crystalline nitride semiconductor layers and beyond.

In its ground state, RuO2 was long thought to be an ordinary metallic paramagnet. Recent neutron and x-ray diffraction revealed that bulk RuO2 is an antiferromagnet (AFM) with TN above 300 K. Furthermore, epitaxial strain induces novel superconductivity in thin films of RuO2 below 2 K. Here, we present a resonant elastic x-ray scattering (REXS) study at the Ru L2 edge of the strained RuO2 films exhibiting the strain-induced superconductivity. We observe an azimuthal modulation of the 100 Bragg peak consistent with canted AFM found in bulk. Most notably, in the strained films displaying novel superconductivity, we observe a 1 eV shift of the Ru eg orbitals to a higher energy. The energy shift is smaller in thicker, relaxed films and films with a different strain direction. Our results provide further evidence of the utility of epitaxial strain as a tuning parameter in complex oxides.

Electronic instabilities drive ordering transitions in condensed matter. Despite many advances in the microscopic understanding of the ordered states, a more nuanced and profound question often remains unanswered: how do the collective excitations influence the electronic order formation? Here, we experimentally show that a phonon affects the spin density wave (SDW) formation after an SDW-quench by femtosecond laser pulses. In a thin film, the temperature-dependent SDW period is quantized, allowing us to track the out-of-equilibrium formation path of the SDW precisely. By exploiting its persistent coupling to the lattice, we probe the SDW through the transient lattice distortion, measured by femtosecond X-ray diffraction. We find that within 500 femtoseconds after a complete quench, the SDW forms with the low-temperature period, directly bypassing a thermal state with the high-temperature period. We argue that a wavevector-matched phonon launched by the quench changes the formation path of the SDW through the dynamic pinning of the order parameter.

The lamellar cuprate superconductors exhibit the highest ambient-pressure superconducting transition temperatures (T-c), and after more than three decades of extraordinary research activity, continue to pose formidable scientific challenges. A major experimental obstacle has been to distinguish universal phenomena from materialsor technique-dependent ones. Angle-resolved photoemission spectroscopy (ARPES) measures momentum-dependent single-particle electronic excitations and has been invaluable in the endeavor to determine the anisotropic momentum-space properties of the cuprates. HgBa2CuO4+delta (Hg1201) is a single-CuO2 -layer cuprate with a particularly high optimal T-c and a simple crystal structure, yet there exists little information from ARPES about the electronic properties of this model system. Here we present an ARPES study of doping-, temperature-, and momentum-dependent systematics of near-nodal dispersion anomalies in Hg1201. The data reveal a hierarchy of three distinct energy scales: a subgap low-energy kink, an intermediate-energy kink near 55 meV, and a peak-dip-hump structure. The first two features are attributed to the coupling of electrons to Ba-derived optical phonons and in-plane bond-stretching phonons, respectively. The nodal peak-dip-hump structure appears to have a common doping dependence in several single-layer cuprates and is interpreted as a manifestation of pseudogap physics at the node. These results establish several universal phenomena, both in terms of connecting multiple experimental techniques for a single material and in terms of connecting comparable spectral features in multiple structurally similar cuprates.

High-performance hydrogen evolution reaction (HER) catalysts are compelling for the conversion of renewable electricity to fuels and feedstocks. The best HER catalysts rely on the use of platinum and show the highest performance in acidic media. Efficient HER catalysts based on inexpensive and Earth-abundant elements that operate in neutral (hence biocompatible) media could enable low-cost direct seawater splitting and the realization of bio-upgraded chemical fuels. In the challenging neutral-pH environment, water splitting is a multistep reaction. Here we present a HER catalyst comprising Ni and CrO x sites doped onto a Cu surface that operates efficiently in neutral media. The Ni and CrO x sites have strong binding energies for hydrogen and hydroxyl groups, respectively, which accelerates water dissociation, whereas the Cu has a weak hydrogen binding energy, promoting hydride coupling. The resulting catalyst exhibits a 48 mV overpotential at a current density of 10 mA cm −2 in a pH 7 buffer electrolyte. These findings suggest design principles for inexpensive, efficient and biocompatible catalytic systems.