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Creators/Authors contains: "Fitzsimmons, Michael R."

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  1. Free, publicly-accessible full text available September 10, 2024
  2. Abstract

    Cobalt oxides have long been understood to display intriguing phenomena known as spin-state crossovers, where the cobalt ion spin changes vs. temperature, pressure, etc. A very different situation was recently uncovered in praseodymium-containing cobalt oxides, where a first-order coupled spin-state/structural/metal-insulator transition occurs, driven by a remarkable praseodymium valence transition. Such valence transitions, particularly when triggering spin-state and metal-insulator transitions, offer highly appealing functionality, but have thus far been confined to cryogenic temperatures in bulk materials (e.g., 90 K in Pr1-xCaxCoO3). Here, we show that in thin films of the complex perovskite (Pr1-yYy)1-xCaxCoO3-δ, heteroepitaxial strain tuning enables stabilization of valence-driven spin-state/structural/metal-insulator transitions to at least 291 K, i.e., around room temperature. The technological implications of this result are accompanied by fundamental prospects, as complete strain control of the electronic ground state is demonstrated, from ferromagnetic metal under tension to nonmagnetic insulator under compression, thereby exposing a potential novel quantum critical point.

  3. Abstract

    Magnetic skyrmions exhibit unique, technologically relevant pseudo‐particle behaviors which arise from their topological protection, including well‐defined, 3D dynamic modes that occur at microwave frequencies. During dynamic excitation, spin waves are ejected into the interstitial regions between skyrmions, creating the magnetic equivalent of a turbulent sea. However, since the spin waves in these systems have a well‐defined length scale, and the skyrmions are on an ordered lattice, ordered structures from spin‐wave interference can precipitate from the chaos. This work uses small‐angle neutron scattering (SANS) to capture the dynamics in hybrid skyrmions and investigate the spin‐wave structure. Performing simultaneous ferromagnetic resonance and SANS, the diffraction pattern shows a large increase in low‐angle scattering intensity, which is present only in the resonance condition. This scattering pattern is best fit using a mass fractal model, which suggests the spin waves form a long‐range fractal network. The fractal structure is constructed of fundamental units with a size that encodes the spin‐wave emissions and are constrained by the skyrmion lattice. These results offer critical insights into the nanoscale dynamics of skyrmions, identify a new dynamic spin‐wave fractal structure, and demonstrate SANS as a unique tool to probe high‐speed dynamics.

    Free, publicly-accessible full text available May 4, 2024
  4. Abstract

    Actinide materials have various applications that range from nuclear energy to quantum computing. Most current efforts have focused on bulk actinide materials. Tuning functional properties by using strain engineering in epitaxial thin films is largely lacking. Using uranium dioxide (UO2) as a model system, in this work, the authors explore strain engineering in actinide epitaxial thin films and investigate the origin of induced ferromagnetism in an antiferromagnet UO2. It is found that UO2+xthin films are hypostoichiometric (x<0) with in‐plane tensile strain, while they are hyperstoichiometric (x>0) with in‐plane compressive strain. Different from strain engineering in non‐actinide oxide thin films, the epitaxial strain in UO2is accommodated by point defects such as vacancies and interstitials due to the low formation energy. Both epitaxial strain and strain relaxation induced point defects such as oxygen/uranium vacancies and oxygen/uranium interstitials can distort magnetic structure and result in magnetic moments. This work reveals the correlation among strain, point defects and ferromagnetism in strain engineered UO2+xthin films and the results offer new opportunities to understand the influence of coupled order parameters on the emergent properties of many other actinide thin films.