Open Access

Show Abstract ▼

Abstract: We explore whether insertion of an ultrathin Mn 'spy layer' within a magnetic hard/soft bilayer can enable depth-sensitive element-specific measurements of the static and dynamic magnetization, while avoiding significant disruption of the original magnetic state. MgO(110)/FePt(100 Å)/NiFe(200 Å)/Mn(tMn Å)/NiFe(200 Å) samples with Mn thicknesses of tMn=0, 5, and 10Å were fabricated by magnetron sputtering and studied by element-selective x-ray magnetic circular dichroism (XMCD), vector network analyzer ferromagnetic resonance (VNA-FMR), and x-ray detected ferromagnetic resonance (XFMR). For tMn= 5 Å, the magnetic reversal properties remain broadly similar to tMn= 0 Å. For tMn=10 Å, the two NiFe layers decouple with XMCD hysteresis loops at the Mn edge showing two switching events that suggest the presence of two distinct Mn-containing regions. While the Mn moments within each region have ferromagnetic order, their relative alignment is antiparallel at high field. Analysis of the magnetic data and additional scanning transmission electron microscopy (STEM) measurements point to the presence of a Mn layer at the lower NiFe/Mn interface, and the formation of a NiFeMn alloy at the upper Mn/NiFe interface. The Mn moments of the former region lie antiparallel to those of the underlying NiFe layer. The VNA-FMR data suggests that for tMn= 5 and 10 Å, the interfacial exchange coupling at the FePt/NiFe is suppressed and the in-plane uniaxial magnetic anisotropy of the NiFe is increased, perhaps due to migration of Mn towards the buried interface. The above findings show that Mn is a problematic magnetic spy, and that a Mn thickness of less than 5Å would be required.

Show Abstract ▼

Abstract: We performed a pump-probe experiment on the chiral magnet Cu2⁢OSeO3 to study the relaxation dynamics of its noncollinear magnetic orders, employing a millisecond magnetic field pulse as the pump and resonant elastic x-ray scattering as the probe. Our findings reveal that the system requires ∼0.2  s to stabilize after the perturbation applied to both the conical and skyrmion lattice phase, which is significantly slower than the typical nanosecond timescale observed in micromagnetics. This prolonged relaxation is attributed to the formation and slow dissipation of local topological defects, such as emergent monopoles. By unveiling the experimental lifetime of these emergent singularities in a noncollinear magnetic system, our study highlights a universal relaxation mechanism in solitonic textures within the slow dynamics regime, offering new insights into topological physics and advanced information storage solutions.

Open Access

Show Abstract ▼

Abstract: Magnetic skyrmions are topologically protected spin textures with emergent particle-like behaviors. Their dynamics under external stimuli is of great interest and importance for topological physics and spintronics applications alike. So far, skyrmions are only found to move linearly in response to a linear drive, following the conventional model treating them as isolated quasiparticles. Here, by performing time and spatially resolved resonant elastic X-ray scattering of the insulating chiral magnet Cu2OSeO3, we show that for finite-sized skyrmion crystallites, a purely linear temperature gradient not only propels the skyrmions but also induces continuous rotational motion through a chiral lattice torque. Consequently, a skyrmion crystallite undergoes a rolling motion under a small gradient, while both the rolling speed and the rotational sense can be controlled. Our findings offer a new degree of freedom for manipulating these quasiparticles toward device applications and underscore the fundamental phase difference between the condensed skyrmion lattice and isolated skyrmions.

Open Access

Show Abstract ▼

Abstract: The increased capacity offered by oxygen-redox active cathode materials for rechargeable lithium- and sodium-ion batteries (LIBs and NIBs, respectively) offers a pathway to the next generation of high-gravimetric-capacity cathodes for use in devices, transportation and on the grid. Many of these materials, however, are plagued with voltage fade, voltage hysteresis and O2 loss, the origins of which can be traced back to changes in their electronic and chemical structures on cycling. Developing a detailed understanding of these changes is critical to mitigating these cathodes’ poor performance. In this work, we present an analysis of the redox mechanism of P2–Na0.67[Mg0.28Mn0.72]O2, a layered NIB cathode whose high capacity has previously been attributed to trapped O2 molecules. We examine a variety of charge compensation scenarios, calculate their corresponding densities of states and spectroscopic properties, and systematically compare the results to experimental data: 25Mg and 17O nuclear magnetic resonance (NMR) spectroscopy, operando X-band and ex situ high-frequency electron paramagnetic resonance (EPR), ex situ magnetometry, and O and Mn K-edge X-ray Absorption Spectroscopy (XAS) and X-ray Absorption Near Edge Spectroscopy (XANES). Via a process of elimination, we suggest that the mechanism for O redox in this material is dominated by a process that involves the formation of strongly antiferromagnetic, delocalized Mn–O states which form after Mg2+ migration at high voltages. Our results primarily rely on noninvasive techniques that are vital to understanding the electronic structure of metastable cycled cathode samples.

Open Access

Show Abstract ▼

Abstract: Spinel ferrites exhibit significant promise in photocatalysis and other applications due to their compositional diversity and favourable electronic structure, magnetism, and partially tuneable cation distribution. However, their complex properties, for example, the different behaviour of bulk and nanostructured materials, are not well understood. Here, we combine advanced computational and experimental methods with reactivity measurements to explore the inversion degrees, electronic structures, and photocatalytic activities of MFe2O4 spinels (M = Co, Cu, Zn). X-ray diffraction and anomalous X-ray scattering measurements determined bulk inversion degrees of 0.81, 0.91, and 0.26 for CoFe2O4, CuFe2O4, and ZnFe2O4, respectively. Photocatalytic tests showed that only ZnFe2O4 is active in the oxygen evolution reaction (OER), which correlates with its favourable band alignment, as determined through electronic structure simulations. Surface-sensitive X-ray Absorption Spectroscopy (XAS) measurements provided insights into the cation distributions at the surfaces, showing significant deviations from bulk properties, particularly in ZnFe2O4 in which 52% of the near-surface tetrahedral sites are occupied by Fe cations, compared to 26% in the bulk. DFT simulations of ZnFe2O4 illustrated how the surface terminations can alter the thermodynamic preference for cation distribution in comparison with the bulk. Our findings illustrate the complex interplay between surface and bulk properties in spinel ferrites.