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During the past decade, CoFe2O4 (hard)/Co-Fe alloy (soft) magnetic nanocomposites have been routinely prepared by partial reduction of CoFe2O4 nanoparticles. Monoxide (i.e., FeO or CoO) has often been detected as a byproduct of the reduction, although it remains unclear whether the formation of this phase occurs during the reduction itself or at a later stage. Here, a novel reaction cell was designed to monitor the reduction in situ using synchrotron powder X-ray diffraction (PXRD). Sequential Rietveld refinements of the in situ data yielded time-resolved information on the sample composition and confirmed that the monoxide is generated as an intermediate phase. The macroscopic magnetic properties of samples at different reduction stages were measured by means of vibrating sample magnetometry (VSM), revealing a magnetic softening with increasing soft phase content, which was too pronounced to be exclusively explained by the introduction of soft material in the system. The elemental compositions of the constituent phases were obtained from joint Rietveld refinements of ex situ high-resolution PXRD and neutron powder diffraction (NPD) data. It was found that the alloy has a tendency to emerge in a Co-rich form, inducing a Co deficiency on the remaining spinel phase, which can explain the early softening of the magnetic material.

In insulating materials with ordered magnetic spiral phases, ferroelectricity can emerge due to the breaking of inversion symmetry. This property is of both fundamental and practical interest, in particular with a view to exploiting it in low-power electronic devices. Advances towards technological applications have been hindered, however, by the relatively low ordering temperatures $T_\mathrm{spiral}$ of most magnetic spiral phases, which rarely exceed 100 K. We have recently established that the ordering temperature of a magnetic spiral can be increased up to 310 K by the introduction of chemical disorder. Here we explore the design space opened up by this novel mechanism by combining it with a targeted lattice control of some magnetic interactions. In Cu-Fe layered perovskites we obtain $T_\mathrm{spiral}$ values close to 400 K, comfortably far from room temperature and almost 100 K higher than using chemical disorder alone. Moreover, we reveal a linear, universal relationship between the spiral's wave vector and the onset temperature of the spiral phase. This linear law ends at a paramagnetic-collinear-spiral triple point, which defines the highest spiral ordering temperature that can be achieved in this class of materials. Based on these findings, we propose a general set of rules for designing magnetic spirals in layered perovskites using external pressure, chemical substitutions and/or epitaxial strain, which should guide future efforts to engineer magnetic spiral phases with ordering temperatures suitable for technological applications., Comment: 5 figures, 35 pages, to be appeared on Science Advance

Excitations in a spin ice behave as magnetic monopoles, and their population and mobility control the dynamics of a spin ice at low temperature. CdEr$_2$Se$_4$ is reported to have the Pauling entropy characteristic of a spin ice, but its dynamics are three-orders of magnitude faster than the canonical spin ice Dy$_2$Ti$_2$O$_7$. In this letter we use diffuse neutron scattering to show that both CdEr$_2$Se$_4$ and CdEr$_2$S$_4$ support a dipolar spin ice state -- the host phase for a Coulomb gas of emergent magnetic monopoles. These Coulomb gases have similar parameters to that in Dy$_2$Ti$_2$O$_7$, i.e. dilute and uncorrelated, so cannot provide three-orders faster dynamics through a larger monopole population alone. We investigate the monopole dynamics using ac susceptometry and neutron spin echo spectroscopy, and verify the crystal electric field Hamiltonian of the Er$^{3+}$ ions using inelastic neutron scattering. A quantitative calculation of the monopole hopping rate using our Coulomb gas and crystal electric field parameters shows that the fast dynamics in CdEr$_2$X$_4$ (X = Se, S) are primarily due to much faster monopole hopping. Our work suggests that CdEr$_2$X$_4$ offer the possibility to study alternative spin ice ground states and dynamics, with equilibration possible at much lower temperatures than the rare earth pyrochlore examples., Comment: 11 pages, 9 figures, accepted for publication in Physical Review Letters

In the past years, magnetism-driven ferroelectricity and gigantic magnetoelectric effects have been reported for a number of frustrated magnets with spiral magnetic orders. Such materials are of high current interest due to their potential for spintronics and low-power magnetoelectric devices. However, their low magnetic order temperatures (typically <100K) greatly restrict their fields of application. Here we demonstrate that the stability domain of the spiral phase in the perovskite YBaCuFeO5 can be enlarged by more than 150K through a controlled manipulation of the Fe/Cu chemical disorder. Moreover we show that this novel mechanism can stabilize the magnetic spiral state of YBaCuFeO5 above the symbolic value of 25{\deg}C at zero magnetic field. Our findings demonstrate that the properties of a magnetic spiral, including its wavelength and stability range, can be engineered through the control of chemical disorder, offering a great potential for the design of materials with magnetoelectric properties beyond room temperature., Comment: 4 Figures