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We report on a study on a representative set of Fe$_{2}$P-based MnFePSi samples by means of $^{55}$Mn NMR in both zero and applied magnetic field. The first-order nature of the magnetic transition is demonstrated by truncated order parameter curves with a large value of the local ordered moment at the Curie point, even at compositions where the transition appears second order from magnetic measurements. No weak ferromagnetic order could be detected at Si-poor compositions showing the kinetic arrest phenomenon, but rather the phase separation of fully ferromagnetic domains from volume fractions where Mn spins are fluctuating. The more pronounced decrease of the ordered moment at the $3f$ sites on approaching $T_C$, characteristic of the mixed magnetism of these materials, is demonstrated to be driven by a vanishing spin density rather than enhanced spin fluctuations at the $3f$ site. An upper limit of 0.03~$\mu_B$ is set for the fluctuating Mn moment at the $3f$ site by the direct detection of a $^{55}$Mn NMR resonance peak in the Mn-rich samples above $T_C$, showing nearly temperature-independent frequency shifts. A sharper secondary peak observed at the same compositions reveals however the disproportionation of a significant $3f$-Mn fraction with negligible hyperfine couplings, which retains its diamagnetic character across the transition, down to the lowest available temperatures. Such a diamagnetic fraction qualitatively accounts for the reduced average $3f$ moment previously reported at large Mn concentrations., Comment: 12 pages, 13 figures. Submitted to Phys. Rev. B

The lack of inversion symmetry in the crystal lattice of magnetic materials gives rise to complex non-collinear spin orders through interactions of relativistic nature, resulting in interesting physical phenomena, such as emergent electromagnetism. Studies of cubic chiral magnets revealed a universal magnetic phase diagram, composed of helical spiral, conical spiral and skyrmion crystal phases. Here, we report a remarkable deviation from this universal behavior. By combining neutron diffraction with magnetization measurements we observe a new multi-domain state in Cu2OSeO3. Just below the upper critical field at which the conical spiral state disappears, the spiral wave vector rotates away from the magnetic field direction. This transition gives rise to large magnetic fluctuations. We clarify physical origin of the new state and discuss its multiferroic properties.

The magnetic phase diagram of the chiral magnet Cu$_2$OSeO$_3$ has been investigated by dc magnetisation and ac susceptibility over a very large frequency range from 0.1 Hz up to 1 kHz and temperatures below 50 K. Qualitatively different phase diagrams have been obtained by applying the magnetic field along the easy $\langle100\rangle$ or the hard $\langle110\rangle$ crystallographic directions. Strong $\chi"$ appears close to $B_{c2}$, but only below 30 K and is more pronounced when $B$ is applied along $\langle100\rangle$. In addition, the transition from the helical to the conical phase leads to two adjacent $B_{c1}$ lines below 50 K. The frequency dependence of $\chi"$ indicates the existence of very broad distributions of relaxation times both at $B_{c1}$ and $B_{c2}$. The associated very long characteristic times eventually prevent the system from reaching thermal equilibrium at low temperatures and lead to thermal hysteresis., Comment: 8 pages, 7 figures

We present an investigation of the magnetic field-temperature phase diagram of Cu$_2$OSeO$_3$ based on DC magnetisation and AC susceptibility measurements covering a broad frequency range of four orders of magnitude, from very low frequencies reaching 0.1 Hz up to 1 kHz. The experiments were performed in the vicinity of $T_C=58.2$ K and around the skyrmion lattice A-phase. At the borders between the different phases the characteristic relaxation times reach several milliseconds and the relaxation is non-exponential. Consequently the borders between the different phases depend on the specific criteria and frequency used and an unambiguous determination is not possible., Comment: 10 pages, 12 figures, accepted for publication in Physical Review B (2016)

(Mn,Fe)2(P,Si) single crystals have been successfully grown by flux method. Single crystal diffraction demonstrates that Mn0.83Fe1.17P0.72Si0.28 crystallizes in a hexagonal crystal structure (space group P-62m) at both 100 and 280 K, in the ferromagnetic and paramagnetic states, respectively. The magnetization measurements show that the crystals display a first-order ferromagnetic phase transition at their Curie temperature (TC). The preferred magnetization direction in is along the c axis. A weak magnetic anisotropy of K1 = 0.25x106 J/m3 and K2 = 0.19x106 J/m3 is found at 5 K. These values indicate a soft magnetic behaviour favourable for magnetic refrigeration. A series of discontinuous magnetization jumps is observed far below TC by increasing the field at a constant temperature. These magnetization jumps are irreversible, occur spontaneously at constant temperature and magnetic field, but can be restored by cycling across the first-order phase transition.

A strong electronic reconstruction resulting in a quenching of the Fe magnetic moments has recently been predicted to be at the origin of the giant magnetocaloric effect displayed by Fe2Pbased materials. To verify this scenario, X-ray Magnetic Circular Dichroism experiments have been carried out at the L edges of Mn and Fe for two typical compositions of the (Mn,Fe)2(P,Si,B) system. The dichroic absorption spectra of Mn and Fe have been measured element specific in the vicinity of the first-order ferromagnetic transition. The experimental spectra are compared with first-principle calculations and charge-transfer multiplet simulations in order to derive the magnetic moments. Even though signatures of a metamagnetic behaviour are observed either as a function of the temperature or the magnetic field, the similarity of the Mn and Fe moment evolution suggests that the quenching of the Fe moment is weaker than previously predicted.

The inverse magnetocaloric effect taking place at the antiferro-to-ferromagnetic transition of (Co,Fe)MnP phosphides has been characterized by magnetic and direct {\Delta}Tad measurements. In Co0.53Fe0.47MnP, entropy change of 1.5 Jkg-1K-1 and adiabatic temperature change of 0.6 K are found at room temperature for an intermediate field change ({\Delta}B= 1 T). Several methods were used to control the metamagnetic transition properties, in each case a peculiar splitting of the antiferro-to-ferromagnetic transition is observed., Comment: 12 pages, 7 figures accepted J. Appl. Phys. (2013)

Structural, magnetic and magnetocaloric properties of Mn2-xCrxSb compounds have been studied. In these compounds a first order magnetic phase transition from the ferrimagnetic to the antiferromagnetic state occurs with decreasing temperature, giving rise to giant inverse magnetocaloric effects that can be tuned over a wide temperature interval through changes in substitution concentration. Entropy changes as high as 7.5 J/kgK have been observed, and a composition independent entropy change is obtained for several different concentrations/working temperatures, making these compounds suitable candidates for a composite working material., Comment: 4 pages, 5 figures

Magnetic and magnetocaloric properties of high-purity, giant magnetocaloric polycrystalline and single-crystalline Fe2P are investigated. Fe2P displays a moderate magnetic entropy change which spans over 70 K and the presence of strong magnetization anisotropy proves this system is not fully itinerant but displays a mix of itinerant and localized magnetism. The properties of pure Fe2P are compared to those of giant magnetocaloric (Fe,Mn)2(P,A) compounds helping understand the exceptional characteristics shown by the latter which are so promising for heat pump and energy conversion applications., Comment: 10 pages, 17 figures

A specific heat measuring instrument, with the capacity for the application of magnetic fields up to 9 Tesla, resorting to microcalorimetry chips from the company Xensor Integration, has been successfully assembled and its functioning specifications are reported in the current paper. With this instrument is it possible to perform specific heat measurements with applied magnetic fields up to 9 Tesla in milligram samples. This offers our group the possibility to calculate the actual adiabatic temperature change of a material, as well as providing reliable and precise information on any phase transition that may be influenced by the application of a magnetic field., Comment: Previously published in the proceedings of Thermag V and currently submitted for a Special Issue of the International Journal of Refrigeration

We report on structural, magnetic and magnetocaloric properties of MnxFe1.95-xP0.50Si0.50 (x > 1.10) compounds. With increasing the Mn:Fe ratio, a first-order magneto-elastic transition gradually changes into a first-order magneto-structural transition via a second-order magnetic transition. The study also shows that thermal hysteresis can be tuned by varying the Mn:Fe ratio. Small thermal hysteresis (less than 1 K) can be obtained while maintaining a giant magnetocaloric effect. This achievement paves the way for real refrigeration applications using magnetic refrigerants., Comment: 4 pages, 3 figures, Supplemental Material

The efficient coupling between lattice degrees of freedom and spin degrees of freedom in magnetic materials can be used for refrigeration and energy conversion. This coupling is enhanced in materials exhibiting the giant magnetocaloric effect. First principle electronic structure calculations on hexagonal MnFe(P, Si) reveal a new form of magnetism: the coexistence of strong and weak magnetism in alternate atomic layers. The weak magnetism of Fe layers (disappearance of local magnetic moments at the Curie temperature) is responsible for a strong coupling with the crystal lattice while the strong magnetism in adjacent Mn-layers ensures Curie temperatures high enough to enable operation at and above room temperature. Varying the composition on these magnetic sublattices gives a handle to tune the working temperature and to achieve a strong reduction of the undesired thermal hysteresis. In this way we design novel materials based on abundantly available elements with properties matched to the requirements of an efficient refrigeration or energy-conversion cycle., Comment: 6 pages, 6 figures

Using X-ray diffraction, DSC and magnetization measurements, a magnoestructural map of the (Mn,Fe)3(Si,P) system was assembled and reported in the current paper. Besides the already known cubic phase for Mn3-xFexSi system and the tetragonal and orthorhombic phases for the Mn3-xFexP system, a novel hexagonal phase has been observed for Mn3 xFexSi1-yPy, within the approximate range of 0.2

We report the observation of a field-induced transformation from the easy-plane antiferromagnetic structure to the easy-axis ferrimagnetic structure in a single crystal of TbFe_4.4Al_7.6 (tetragonal ThMn_12 structure) at 5 K. Such a field-induced, irreversible transition has been identified for the first time. This transition is accompanied by a giant orthorhombic distortion: epsilon_aa = - epsilon_bb ~ 3.5x10^-4 that is associated with a magnetic hardness (mu_0H_C ~ 3 T) that is unprecedented in this category of materials., Comment: pdf file, 14 pages, 3 figures; PRB in print

We have calculated the low-field magnetic susceptibility $\chi$ of a system consisting of non-interacting mono-dispersed nanoparticles using a classical statistical approach. The model makes use of the assumption that the axes of symmetry of all nanoparticles are aligned and oriented at a certain angle $\psi$ with respect to the external magnetic field. An analytical expression for the temperature dependence of the susceptibility $\chi(T)$ above the blocking temperature is obtained. The derived expression is a generalization of the Curie law for the case of anisotropic magnetic particles. We show that the normalized susceptibility is a universal function of the ratio of the temperature over the anisotropy constant for each angle $\psi$. In the case that the easy-axis is perpendicular to the magnetic field the susceptibility has a maximum. The temperature of the maximum allows one to determine the anisotropy energy., Comment: 6 pages (incl. 5 figures), submitted for publication