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Register a new userUnderstanding Magnetic Phase Coexistence in Ru$_2$Mn$_{1-x}$Fe$_x$Sn Heusler Alloys: A Neutron Scattering, Thermodynamic, and Phenomenological Analysis
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The random substitutional solid solution between the antiferromagnetic (AFM) full-Heusler alloy Ru$_2$MnSn and the ferromagnetic (FM) full-Heusler alloy Ru$_2$FeSn provides a rare opportunity to study FM-AFM phase competition in a near-lattice-matched, cubic system, with full solubility. At intermediate $x$ in Ru$_2$Mn$_{1-x}$Fe$_x$Sn this system displays suppressed magnetic ordering temperatures, spatially coexisting FM and AFM order, and strong coercivity enhancement, despite rigorous chemical homogeneity. Here, we construct the most detailed temperature- and $x$-dependent understanding of the magnetic phase competition and coexistence in this system to date, combining wide-temperature-range neutron diffraction and small-angle neutron scattering with magnetometry and specific heat measurements on thoroughly characterized polycrystals. A complete magnetic phase diagram is generated, showing FM-AFM coexistence between $x approx 0.30$ and $x approx 0.70$. Important new insight is gained from the extracted length scales for magnetic phase coexistence (25-100 nm), the relative magnetic volume fractions and ordering temperatures, in addition to remarkable $x$-dependent trends in magnetic and electronic contributions to specific heat. An unusual feature in the magnetic phase diagram (an intermediate FM phase) is also shown to arise from an extrinsic effect related to a minor Ru-rich secondary phase. The established magnetic phase diagram is then discussed with the aid of phenomenological modeling, clarifying the nature of the mesoscale phase coexistence with respect to the understanding of disordered Heisenberg models.
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We demonstrate how exchange hardening can arise in a chemically-disordered solid solution from a first-principles statistical mechanics approach. A general mixed-basis chemical and magnetic cluster expansion has been developed, and applied to the Mn$_{1-x}$Fe$_x$Ru$_2$Sn Heusler alloy system; single-phase solid solutions between antiferromagnetic ch{MnRu2Sn} and ferromagnetic ch{FeRu2Sn} with disorder on the Mn/Fe sublattice that exhibit unexpected exchange hardening. Monte Carlo simulations applied to the cluster expansion are able to reproduce the experimentally measured magnetic transition temperatures and the bulk magnetization as a function of composition. The magnetic ordering around a site is shown to be dependent not only on bulk composition, but also on the identity of the site and the local composition around that site. The simulations predict that local antiferromagnetic orderings form inside a bulk ferromagnetic region at intermediate compositions that drives the exchange hardening. Furthermore, the antiferromagnetic regions disorder at a lower temperature than the ferromagnetic regions, providing an atomistic explanation for the experimentally-observed decrease in exchange hardening with increasing temperature. These effects occur on a length scale too small to be resolved with previously-used characterization techniques.
This study presents the effect of local electronic correlations on the Heusler compounds Co$_2$Mn$_{1-x}$Fe$_x$Si as a function of the concentration $x$. The analysis has been performed by means of first-principles band-structure calculations based on the local approximation to spin-density functional theory (LSDA). Correlation effects are treated in terms of the Dynamical Mean-Field Theory (DMFT) and the LSDA+U approach. The formalism is implemented within the Korringa-Kohn-Rostoker (KKR) Greens function method. In good agreement with the available experimental data the magnetic and spectroscopic properties of the compound are explained in terms of strong electronic correlations. In addition the correlation effects have been analysed separately with respect to their static or dynamical origin. To achieve a quantitative description of the electronic structure of Co$_2$Mn$_{1-x}$Fe$_x$Si both static and dynamic correlations must be treated on equal footing.
We report a comprehensive small-angle neutron scattering~(SANS) study of Mn$_{1-x}$Fe$_{x}$Si at zero magnetic field. To delineate changes of magneto-crystalline anisotropies (MCAs) from effects due to defects and disorder, we recorded complementary susceptibility and specific heat data, and investigated selected compositions of Mn$_{1-x}$Co$_{x}$Si. For all systems studied the transition temperature and magnetic phase diagrams evolve monotonically with composition consistent with literature. The SANS patterns of the magnetic order recorded under zero-field cooling display strong changes of the directions of the intensity maxima and smeared out intensity distributions as a function of composition. We show that cubic MCAs account for the complex evolution of the SANS patterns, where for increasing $x$ the character of the MCAs shifts from terms that are fourth-order to terms that are sixth order in spin--orbit coupling. The magnetic field dependence of the susceptibility and SANS establishes that the helix reorientation as a function of magnetic field for Fe- or Co-doped MnSi is dominated by pinning due to defects and disorder. The presence of thermodynamic anomalies of the specific heat at the phase boundaries of the skyrmion lattice phase in the doped samples and properties observed in Mn$_{1-x}$Co$_{x}$Si establishes that the pinning due to defects and disorder remains, however, weak and comparable to the field scale of the helix reorientation. The observation that MCAs, that are sixth order in spin-orbit coupling, play an important role for the spontaneous order in Mn$_{1-x}$Fe$_{x}$Si and Mn$_{1-x}$Co$_{x}$Si, offering a fresh perspective for a wide range of topics in cubic chiral magnets such as the generic magnetic phase diagram, the morphology of topological spin textures, the paramagnetic-to-helical transition, and quantum phase transitions.
We report the structural, magnetic, and magnetocaloric properties of Co$_2$Cr$_{1-x}$Ti$_x$Al ($x=$ 0--0.5) Heusler alloys for spintronic and magnetic refrigerator applications. Room temperature X-ray diffraction and neutron diffraction patterns along with Rietveld refinements confirm that the samples are of single phase and possess a cubic structure. Interestingly, magnetic susceptibly measurements indicate a second order phase transition from paramagnetic to ferromagnetic where the Curie temperature (T$_{rm C}$) of Co$_2$CrAl increases from 330~K to 445~K with Ti substitution. Neutron powder diffraction data of the $x=$ 0 sample across the magnetic phase transition taken in a large temperature range confirm the structural stability and exclude the possibility of antiferromagnetic ordering. The saturation magnetization of the $x=$ 0 sample is found to be 8000~emu/mol (1.45~$mu_{rm B}$/{it f.u.}) at 5~K, which is in good agreement with the value (1.35$pm$0.05~$mu_{rm B}$/{it f.u.}) obtained from the Rietveld analysis of the neutron powder diffraction pattern measured at temperature of 4~K. By analysing the temperature dependence of the neutron data of the $x=$ 0 sample, we find that the change in the intensity of the most intense Bragg peak (220) is consistent with the magnetization behavior with temperature. Furthermore, an enhancement of change in the magnetic entropy and relative cooling power values has been observed for the $x=$ 0.25 sample. Interestingly, the critical behavior analysis across the second order magnetic phase transition and extracted exponents ($betaapprox$ 0.496, $gammaapprox$ 1.348, and $deltaapprox$ 3.71 for the $x=$ 0.25 sample) suggest the presence of long-range ordering, which deviates towards 3D Heisenberg type interactions above T$_{rm C}$, consistent with the interaction range value $sigma$.
Mn$_{3}$Sn is a non-collinear antiferromagnet which displays a large anomalous Hall effect at room temperature. It is believed that the principal contribution to its anomalous Hall conductivity comes from Berry curvature. Moreover, dc transport and photoemission experiments have confirmed that Mn$_{3}$Sn may be an example of a time-reversal symmetry breaking Weyl semimetal. Due to a small, but finite moment in the room temperature inverse triangular spin structure, which allows control of the Hall current with external field, this material has garnered much interest for next generation memory devices and THz spintronics applications. In this work, we report a THz range study of oriented Mn$_{3}$Sn thin films as a function of temperature. At low frequencies we found the optical conductivity can be well described by a single Drude oscillator. The plasma frequency is strongly suppressed in a temperature dependent fashion as one enters the 260 K helical phase. This may be associated with partial gapping of the Fermi surfaces that comes from breaking translational symmetry along the c-axis. The scattering rate shows quadratic temperature dependence below 200 K, highlighting the possible important role of interactions in this compound.
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