Three-dimensional antisphere arrays (3DAAs) of Ni have been fabricated using electrochemical deposition into self-assembled polystyrene sphere templates, which offers the advantage of straightforward scalability. Using the first-order reversal curve (FORC) method, the magnetic reversal mechanism is identified from the characteristic features in the FORC distribution. A left-bending boomerang-like feature is observed in the thinnest sample, which transforms to a ridge oriented along the local coercivity Hc axis with increasing sample thickness. This transformation identifies a change in the reversal process from an exchange dominated domain-growth reversal to a localized weakly interacting particle-like reversal. Micromagnetic simulations confirm the decrease in domain growth and increase of pinning behaviors as the thickness of the Ni 3DAAs structure increases, providing strong support to the FORC analysis and interpretation.

The spin crossover (SCO) transitions at both the surface and over the entire volume of the [Fe{H₂B(pz)₂}₂(bipy)] polycrystalline films on Al₂O₃ substrates have been studied, where pz  =  pyrazol-1-yl and bipy  =  2,2'-bipyridine. For [Fe{H₂B(pz)₂}₂(bipy)] films of hundreds of nm thick, magnetometry and x-ray absorption spectroscopy measurements show thermal hysteresis in the SCO transition with temperature, although the transition in bulk [Fe{H₂B(pz)₂}₂(bipy)] occurs in a non-hysteretic fashion at 157 K. While the size of the crystallites in those films are similar, the hysteresis becomes more prominent in thinner films, indicating a significant effect of the [Fe{H₂B(pz)₂}₂(bipy)]/Al₂O₃ interface. Bistability of spin states, which can be inferred from the thermal hysteresis, was directly observed using temperature-dependent x-ray diffraction; the crystallites behave as spin-state domains that coexist during the transition. The difference between the spin state of molecules at the surface of the [Fe{H₂B(pz)₂}₂(bipy)] films and that of the molecules within the films, during the thermal cycle, indicates that both cooperative (intermolecular) effects and coordination are implicated in perturbations to the SCO transition.

The magnetic interactions between rare-earth and Fe ions in hexagonal rare-earth ferrites (h-RFeO3), may amplify the weak ferromagnetic moment on Fe, making these materials more appealing as multiferroics. To elucidate the interaction strength between the rare-earth and Fe ions as well as the magnetic moment of the rare-earth ions, element-specific magnetic characterization is needed. Using x-ray magnetic circular dichroism, we have studied the ferrimagnetism in h-YbFeO3 by measuring the magnetization of Fe and Yb separately. The results directly show antialignment of magnetization of Yb and Fe ions in h-YbFeO3 at low temperature, with an exchange field on Yb of about 17 kOe. The magnetic moment of Yb is about 1.6μB at low temperature, significantly reduced compared with the 4.5μB moment of a free Yb3+. In addition, the saturation magnetization of Fe in h-YbFeO3 has a sizable enhancement compared with that in h-LuFeO3. These findings directly demonstrate that ferrimagnetic order exists in h-YbFeO3; they also account for the enhancement of magnetization and the reduction of coercivity in h-YbFeO3 compared with those in h-LuFeO3 at low temperature, suggesting an important role for the rare-earth ions in tuning the multiferroic properties of h-RFeO3.

Realizing van der Waals (vdW) epitaxy in the 1980s represents a breakthrough that circumvents the stringent lattice matching and processing compatibility requirements in conventional covalent heteroepitaxy. However, due to the weak vdW interactions, there is little control over film qualities by the substrate. Typically, discrete domains with a spread of misorientation angles are formed, limiting the applicability of vdW epitaxy. Here, the epitaxial growth of monocrystalline, covalent Cr₅ Te₈ 2D crystals on monolayer vdW WSe₂ by chemical vapor deposition is reported, driven by interfacial dative bond formation. The lattice of Cr₅ Te₈ , with a lateral dimension of a few tens of micrometers, is fully commensurate with that of WSe₂ via 3 × 3 (Cr₅ Te₈ )/7 × 7 (WSe₂ ) supercell matching, forming a single-crystalline moiré superlattice. This work establishes a conceptually distinct paradigm of thin-film epitaxy, termed "dative epitaxy", which takes full advantage of covalent epitaxy with chemical bonding for fixing the atomic registry and crystal orientation, while circumventing its stringent lattice matching and processing compatibility requirements; conversely, it ensures the full flexibility of vdW epitaxy, while avoiding its poor orientation control. Cr₅ Te₈ 2D crystals grown by dative epitaxy exhibit square magnetic hysteresis, suggesting minimized interfacial defects that can serve as pinning sites.