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Recently, a Verwey type transition in the mixed valence alkali sesquioxide Cs4O6 was deduced from the charge ordering of molecular peroxide O2 amp; 8722;2 and superoxide O amp; 8722;2 anions accompanied by the structural transformation and a dramatic change in electronic conductivity [Adler et al., Sci. Adv. 4, eaap7581 2018 ]. Here, we report that in the sister compound Rb4O6, a similar Verwey type charge ordering transition is strongly linked to O amp; 8722;2 orbital and spin dynamics. On cooling, a powder neutron diffraction experiment reveals a charge ordering anda cubic to tetragonal transition at TCO 290 K, which is followed by a further structural instability at Ts 92 K that involves an additional reorientation of magnetic O amp; 8722;2 anions. Magnetic resonance techniques supported by density functional theory computations suggest the emergence of a peculiar type of amp; 960; amp; 8727; orbital ordering of the magnetically active O amp; 8722;2 units, which promotes the formation of a quantum spin state composed of weakly coupled spin dimers. These results reveal that as in 3d transition metal compounds, also in the amp; 960; amp; 8727; open shell alkali sesquioxides the interplay between Jahn Teller like electron lattice coupling and Kugel Khomskii type superexchange determines the nature of orbital ordering and the magnetic ground state

International audience; The cubic chiral helimagnets with the P2 1 3 space group represent a group of compounds in which the stable skyrmion-lattice state is experimentally observed. The key parameter that controls the energy landscape of such systems and determines the emergence of a topologically nontrivial magnetic structure is the Dzyaloshinskii-Moriya interaction (DMI). Chemical substitution is recognized as a convenient instrument to tune the DMI in real materials and has been successfully utilized in studies of a number of chiral magnets, such as MnSi, FeGe, MnGe, and others. In our study, we applied small-angle neutron scattering to investigate how chemical substitution influences the skyrmionic properties of an insulating helimagnet Cu 2 OSeO 3 when Cu ions are replaced by either Zn or Ni. Our results demonstrate that the DMI is enhanced in the Ni-substituted compounds (Cu,Ni) 2 OSeO 3 , but weakened in (Cu,Zn) 2 OSeO 3. The observed changes in the DMI strength are reflected in the magnitude of the spin-spiral propagation vector and the temperature stability of the skyrmion phase.

Ni-Co-Mn-Sb-based Heusler shape-memory alloys that undergo a martensitic-structural transition around room temperature are well known for exhibiting large magnetic entropy change and elastocaloric effect. Here, we report the observation of a large adiabatic temperature change of −11 K in a Ni-Co-Mn-Sb system by using direct adiabatic temperature-change measurements in pulsed magnetic fields. We show that a large magnetic cooling can be achieved in a wide temperature range spanning from 120 to 270 K by purposefully varying the chemical composition. The temperature- and field-dependent irreversibility of the effect is analyzed through a detailed experimental study of the protocol-dependent magnetocaloric effect. The present study is an important contribution towards the understanding of irreversible magnetocaloric effects in materials with magnetostructural transition.

Non-collinear antiferromagnets are revealing many unexpected phenomena and they became crucial for the field of antiferromagnetic spintronics. To visualize and prepare a well-defined domain structure is of key importance. The spatial magnetic contrast, however, remains extraordinary difficult to be observed experimentally. Here, we demonstrate a magnetic imaging technique based on a laser induced local thermal gradient combined with detection of the anomalous Nernst effect. We employ this method in one the most actively studied representative of this class of materials - Mn₃Sn. We undoubtedly proof that the observed contrast is of magnetic origin. We further show an algorithm to prepare a well defined domain pattern at room temperature based on heat assisted recording principle. Our study opens a prospect to study spintronics phenomena in non-collinear antiferromagnets with spatial resolution.

Antiferromagnetic materials are of great interest for spintronics. Here we present a comprehensive study of the growth, structural characterization, and resulting magnetic properties of thin films of the non-collinear antiferromagnet Mn$_{3}$Ir. Using epitaxial engineering on MgO (001) and Al$_{2}$O$_{3}$ (0001) single crystal substrates, we control the growth of cubic ${\gamma}$-Mn$_{3}$Ir in both (001) and (111) crystal orientations, and discuss the optimization of growth conditions to achieve high-quality crystal structures with low surface roughness. Exchange bias is studied in bilayers, with exchange bias fields as large as -29 mT (equivalent to a unidirectional anisotropy constant of 11.5 nJ cm$^{-2}$) measured in Mn$_{3}$Ir (111) / permalloy heterostructures at room temperature. In addition, a distinct dependence of blocking temperature on in-plane crystallographic direction in Mn$_{3}$Ir (001) / Py bilayers is observed. These findings are discussed in the context of chiral antiferromagnetic domain structures, and will inform progress towards topological antiferromagnetic spintronic devices., Comment: 15 pages, 10 figures

We report synthesis and crystal structure refinement of Ag2RuO4, followed by combined analysis of its physical properties through bulk experimental tools (magnetic susceptibility, electron transport, and heat capacity measurements), a microscopic experimental tool (temperature dependent neutron diffraction), and ab initio first-principles calculations. We observe a rather unique (RuO3/1O2/2)n polyoxoanion, where Ru is in a distorted trigonal bipyramidal coordination by oxygen. The RuO5 polyhedra are linked via the apical oxygen atoms to form chains extending along the crystallographic a axis. Crystal structure, magnetization, and ab initio calculations indicate that Ru is in the +6 oxidation state with a nominal valence electron configuration of 4d2. Bulk magnetization, specific-heat, and neutron-diffraction measurements provide clear indication of an antiferromagnetic transition around 75 K with moderate spin canting in the order of 30∘ with respect to the c axis. The neutron-diffraction results as well as the density functional theory based first-principles calculations of exchange interactions revealed that the strong intrachain interaction is predominantly of ferromagnetic (FM) type, and that this spin order along the chains couples with the neighboring chains through comparatively weak FM and antiferromagnetic interactions. Notably, the Landé g factor is found to be 1.8 (with an infinite chain model and even a simple Curie-Weiss approach), away from the ideal value of 2, due to the low dimensionality of the Ru/O substructure.

The thermal excitation of electrons to higher, unoccupied states leads in certain cases to the paradox situation that the chemical potential needs to be shifted to lower energies. Here, a manipulation of Dirac fermions through the temperature dependence of the chemical potential is analyzed while maintaining sufficient insulating character in the bulk. The appearance of a bulk conduction band and consequently, a remarkable energy shift of the Dirac point is observed in Bi2Te2Se at low temperatures (20 K), compared to the high temperatures (200–300 K), as revealed by hard x-ray photoelectron spectroscopy as well as momentum-resolved photoelectron microscopy. The temperature-induced shift of the Dirac cone and the appearance of bulk bands are related to the paradoxical shift of the chemical potential. The experiments are completely reversible, i.e., repeated cooling and heating of the sample up to room temperature recovers the original spectra. Such bulk related energy shifts must be considered not only in photoelectron spectroscopy but also in analysis of other measurable physical quantities and while designing devices for applications.

Epitaxial films of the B20-structure compound Fe1−yCoyGe were grown by molecular beam epitaxy on Si (111) substrates. The magnetization varied smoothly from the bulklike values of one Bohr magneton per Fe atom for FeGe to zero for nonmagnetic CoGe. The chiral lattice structure leads to a Dzyaloshinskii-Moriya interaction (DMI), and the films' helical magnetic ground state was confirmed using polarized neutron reflectometry measurements. The pitch of the spin helix, measured by this method, varies with Co content y and diverges at y∼0.45. This indicates a zero crossing of the DMI, which we reproduced in calculations using first-principles methods. We also measured the longitudinal and Hall resistivity of our films as a function of magnetic field, temperature, and Co content y. The Hall resistivity is expected to contain contributions from the ordinary, anomalous, and topological Hall effects. Both the anomalous and topological Hall resistivities show peaks around y∼0.5. Our first-principles calculations show a peak in the topological Hall constant at this value of y, related to the strong spin polarization predicted for intermediate values of y. Our calculations predict half-metallicity for y=0.6, consistent with the experimentally observed linear magnetoresistance at this composition, and potentially related to the other unusual transport properties for intermediate value of y. While it is possible to reconcile theory with experiment for the various Hall effects for FeGe, the large topological Hall resistivities for y∼0.5 are much larger than expected when the very small emergent fields associated with the divergence in the DMI are taken into account.

The origin of incommensurate structural modulation in Ni-Mn based Heusler-type magnetic shape-memory alloys (MSMAs) is still an unresolved issue in spite of intense focus on it due to its role in the magnetic field induced ultrahigh strains. In the archetypal MSMA Ni2MnGa, the observation of “nonuniform displacement” of atoms from their mean positions in the modulated martensite phase, premartensite phase, and charge density wave as well as the presence of phason broadening of satellite peaks has been taken in support of the electronic instability model linked with a soft acoustic phonon. We present here results of a combined high-resolution synchrotron x-ray powder diffraction (SXRPD) and neutron powder diffraction (NPD) study on Ni2Mn1.4In0.6 using a (3+1)D superspace group approach, which reveals not only uniform atomic displacements in the modulated structure of the martensite phase with physically acceptable ordered magnetic moments in the antiferromagnetic phase at low temperatures, but also the absence of any premartensite phase and phason broadening of the satellite peaks. Our HRTEM studies and first-principles calculations of the ground state also support uniform atomic displacements predicted by powder diffraction studies. All these observations suggest that the structural modulation in the martensite phase of Ni2Mn1.4In0.6 MSMA can be explained in terms of the adaptive phase model. The present study underlines the importance of superspace group analysis using complementary SXRPD and NPD in understanding the physics of the origin of modulation as well as the magnetic and the modulated ground states of the Heusler-type MSMAs. Our work also highlights the fact that the mechanism responsible for the origin of modulated structure in different Ni-Mn based MSMAs may not be universal and it must be investigated thoroughly in different alloy compositions.

The large magnetocaloric effect (MCE) observed in Ni-Mn based shape memory Heusler alloys put them forward to use in magnetic refrigeration technology. It is associated with a first-order magnetostructural (martensitic) phase transition.We conducted a comprehensive study of the MCE for the off-stoichiometric Heusler alloy Ni2.2Mn0.8Ga in the vicinity of its first-order magnetostructural phase transition. We found a reversible MCE under repeated magnetic field cycles. The reversible behavior can be attributed to the small thermal hysteresis of the martensitic phase transition. Based on the analysis of our detailed temperature dependent x-ray diffraction data, we demonstrate the geometric compatibility of the cubic austenite and tetragonal martensite phases. This finding directly relates the reversible MCE behavior to an improved geometric compatibility condition between cubic austenite and tetragonal martensite phases. The approach will help to design shape memory Heusler alloys with a large reversible MCE taking advantage of the first-order martensitic phase transition.

Physical review / B 97(22), 224102 (2018). doi:10.1103/PhysRevB.97.224102, The origin of incommensurate structural modulation in Ni-Mn based Heusler-type magnetic shape-memory alloys (MSMAs) is still an unresolved issue in spite of intense focus on it due to its role in the magnetic field induced ultrahigh strains. In the archetypal MSMA Ni$_2$MnGa, the observation of “nonuniform displacement” of atoms from their mean positions in the modulated martensite phase, premartensite phase, and charge density wave as well as the presence of phason broadening of satellite peaks has been taken in support of the electronic instability model linked with a soft acoustic phonon. We present here results of a combined high-resolution synchrotron x-ray powder diffraction (SXRPD) and neutron powder diffraction (NPD) study on Ni$_2$Mn$_{1.4}$In$_{0.6}$ using a (3+1)D superspace group approach, which reveals not only uniform atomic displacements in the modulated structure of the martensite phase with physically acceptable ordered magnetic moments in the antiferromagnetic phase at low temperatures, but also the absence of any premartensite phase and phason broadening of the satellite peaks. Our HRTEM studies and first-principles calculations of the ground state also support uniform atomic displacements predicted by powder diffraction studies. All these observations suggest that the structural modulation in the martensite phase of Ni$_2$Mn$_{1.4}$In$_{0.6}$ MSMA can be explained in terms of the adaptive phase model. The present study underlines the importance of superspace group analysis using complementary SXRPD and NPD in understanding the physics of the origin of modulation as well as the magnetic and the modulated ground states of the Heusler-type MSMAs. Our work also highlights the fact that the mechanism responsible for the origin of modulated structure in different Ni-Mn based MSMAs may not be universal and it must be investigated thoroughly in different alloy compositions., Published by APS, Woodbury, NY

The large magnetocaloric effect (MCE) observed in Ni-Mn based shape-memory Heusler alloys put them forward to use in magnetic refrigeration technology. It is associated with a first-order magnetostructural (martensitic) phase transition. We conducted a comprehensive study of the MCE for the off-stoichiometric Heusler alloy Ni$_{2.2}$Mn$_{0.8}$Ga in the vicinity of its first-order magnetostructural phase transition. We found a reversible MCE under repeated magnetic field cycles. The reversible behavior can be attributed to the small thermal hysteresis of the martensitic phase transition. Based on the analysis of our detailed temperature dependent X-ray diffraction data, we demonstrate the geometric compatibility of the cubic austenite and tetragonal martensite phases. This finding directly relates the reversible MCE behavior to an improved geometric compatibility condition between cubic austenite and tetragonal martensite phases. The approach will help to design shape-memory Heusler alloys with a large reversible MCE taking advantage of the first-order martensitic phase transition., 6 pages, 4 figures

Non-centrosymmetric transition-metal mono-pnictides such as NbAs, NbP and TaAs attracted a lot of attention because their bandstructures show linear non-degenerate band crossings, dubbed Weyl nodes [1,2]. Additionally, for certain magnetic-field orientations, the highest de Haas-van Alphen frequencies observed are smaller than 50 T. For that reason, all bands are expected to be in the quantum limit at fields easily reachable by pulsed magnetic fields. Thus, these semimetals constitute an ideal playground to study the quantum limit by electric transport and magnetic-torque measurements. Our first results for NbP show an unexpected linear increase in magnetic-torque measurements. In our contribution we show the results of our magnetic-torque measurements on NbP, NbAs, TaP and TaAs in pulsed fields up to 70 T.