Evidence of the Anomalous Fluctuating Magnetic State by Pressure-Driven 4f Valence Change in EuNiGe3.

In rare-earth compounds with valence fluctuation, the proximity of the 4f level to the Fermi energy leads to instabilities of the charge configuration and the magnetic moment. Here, we provide direct experimental evidence for an induced magnetic polarization of the Eu3+ atomic shell with J = 0, due to intra-atomic exchange and spin-orbital coupling interactions with the Eu2+ atomic shell. By applying external pressure, a transition from antiferromagnetic to a fluctuating behavior in EuNiGe3 single crystals is probed. Magnetic polarization is observed for both valence states of Eu2+ and Eu3+ across the entire pressure range. The anomalous magnetism is discussed in terms of a homogeneous intermediate valence state where frustrated Dzyaloshinskii-Moriya couplings are enhanced by the onset of spin-orbital interaction and engender a chiral spin-liquid-like precursor.

Magnetic properties and signatures of ordering in triangular lattice antiferromagnet KCeO2.

The magnetic ground state and the crystalline electric field level scheme of the triangular lattice antiferromagnet KCeO2 are investigated. Below TN=300 mK, KCeO2 develops signatures of magnetic order in specific heat measurements and low energy inelastic neutron scattering data. Trivalent Ce3+ ions in the D3d local environment of this compound exhibit large splittings among the lowest three 4f1 Kramers doublets defining for the free ion the J=5/2 sextet and a ground state doublet with dipole character, consistent with recent theoretical predictions in M. S. Eldeeb et al. Phys. Rev. Materials 4, 124001 (2020). An unexplained, additional local mode appears, and potential origins of this anomalous mode are discussed.

Modulations in martensitic Heusler alloys originate from nanotwin ordering.

Heusler alloys exhibiting magnetic and martensitic transitions enable applications like magnetocaloric refrigeration and actuation based on the magnetic shape memory effect. Their outstanding functional properties depend on low hysteresis losses and low actuation fields. These are only achieved if the atomic positions deviate from a tetragonal lattice by periodic displacements. The origin of the so-called modulated structures is the subject of much controversy: They are either explained by phonon softening or adaptive nanotwinning. Here we used large-scale density functional theory calculations on the Ni2MnGa prototype system to demonstrate interaction energy between twin boundaries. Minimizing the interaction energy resulted in the experimentally observed ordered modulations at the atomic scale, it explained that a/b twin boundaries are stacking faults at the mesoscale, and contributed to the macroscopic hysteresis losses. Furthermore, we found that phonon softening paves the transformation path towards the nanotwinned martensite state. This unified both opposing concepts to explain modulated martensite.

Pressure-Induced Ferromagnetism due to an Anisotropic Electronic Topological Transition in Fe_{1.08}Te.

A rapid and anisotropic modification of the Fermi-surface shape can be associated with abrupt changes in crystalline lattice geometry or in the magnetic state of a material. We show that such an electronic topological transition is at the basis of the formation of an unusual pressure-induced tetragonal ferromagnetic phase in Fe_{1.08}Te. Around 2 GPa, the orthorhombic and incommensurate antiferromagnetic ground state of Fe_{1.08}Te is transformed upon increasing pressure into a tetragonal ferromagnetic state via a conventional first-order transition. On the other hand, an isostructural transition takes place from the paramagnetic high-temperature state into the ferromagnetic phase as a rare case of a "type-0" transformation with anisotropic properties. Electronic-structure calculations in combination with electrical resistivity, magnetization, and x-ray diffraction experiments show that the electronic system of Fe_{1.08}Te is instable with respect to profound topological transitions that can drive fundamental changes of the lattice anisotropy and the associated magnetic order.

Signatures of a magnetic field-induced unconventional nematic liquid in the frustrated and anisotropic spin-chain cuprate LiCuSbO4.

Modern theories of quantum magnetism predict exotic multipolar states in weakly interacting strongly frustrated spin-1/2 Heisenberg chains with ferromagnetic nearest neighbor (NN) inchain exchange in high magnetic fields. Experimentally these states remained elusive so far. Here we report strong indications of a magnetic field-induced nematic liquid arising above a field of ~13 T in the edge-sharing chain cuprate LiSbCuO4 ≡ LiCuSbO4. This interpretation is based on the observation of a field induced spin-gap in the measurements of the 7Li NMR spin relaxation rate T 1-1 as well as a contrasting field-dependent power-law behavior of T 1-1 vs. T and is further supported by static magnetization and ESR data. An underlying theoretical microscopic approach favoring a nematic scenario is based essentially on the NN XYZ exchange anisotropy within a model for frustrated spin-1/2 chains and is investigated by the DMRG technique. The employed exchange parameters are justified qualitatively by electronic structure calculations for LiCuSbO4.

Solitonic Spin-Liquid State Due to the Violation of the Lifshitz Condition in Fe(1+y)Te.

A combination of phenomenological analysis and Mössbauer spectroscopy experiments on the tetragonal Fe(1+y)Te system indicates that the magnetic ordering transition in compounds with higher Fe excess, y≥0.11, is unconventional. Experimentally, a liquidlike magnetic precursor with quasistatic spin order is found from significantly broadened Mössbauer spectra at temperatures above the antiferromagnetic transition. The incommensurate spin-density wave order in Fe(1+y)Te is described by a magnetic free energy that violates the weak Lifshitz condition in the Landau theory of second-order transitions. The presence of multiple Lifshitz invariants provides the mechanism to create multidimensional, twisted, and modulated solitonic phases.

Pressure-induced inhomogeneous chiral-spin ground state in FeGe.

(57)Fe nuclear forward scattering on the chiral magnet FeGe reveals an extremely large precursor phase region above the helimagnetic ordering temperature T(C)(p) and beyond the pressure-induced quantum phase transition at 19 GPa. The decrease of the magnetic hyperfine field ⟨B(hf)⟩ with pressure is accompanied by a large increase of the width of the distribution of ⟨B(hf)⟩, indicating a strong quasistatic inhomogeneity of the magnetic states in the precursor region. Hyperfine fields of the order of 4 T (equivalent to a magnetic moment µ(Fe)≈0.4µ(B)) persist up to 28.5 GPa. No signatures of magnetic order have been found at about 31 GPa. The results, supported by ab initio calculations, suggest that chiral magnetic precursor phenomena, such as an inhomogeneous chiral-spin state, are vastly enlarged due to increasing spin fluctuations as FeGe is tuned to its quantum phase transition.

Theory of skyrmion states in liquid crystals.

Within the Oseen-Frank theory we derive numerically exact solutions for axisymmetric localized states in chiral liquid crystal layers with homeotropic anchoring. These solutions describe recently observed two-dimensional skyrmions in confinement-frustrated chiral nematics [P. J. Ackerman et al., Phys. Rev. E 90, 012505 (2014)]. We stress that these solitonic states arise due to a fundamental stabilization mechanism responsible for the formation of skyrmions in cubic helimagnets and other noncentrosymmetric condensed-matter systems.

Large noncollinearity and spin reorientation in the novel Mn2RhSn Heusler magnet.

Noncollinear magnets provide essential ingredients for the next generation memory technology. It is a new prospect for the Heusler materials, already well known due to the diverse range of other fundamental characteristics. Here, we present a combined experimental and theoretical study of novel noncollinear tetragonal Mn(2)RhSn Heusler material exhibiting unusually strong canting of its magnetic sublattices. It undergoes a spin-reorientation transition, induced by a temperature change and suppressed by an external magnetic field. Because of the presence of Dzyaloshinskii-Moriya exchange and magnetic anisotropy, Mn(2)RhSn is suggested to be a promising candidate for realizing the Skyrmion state in the Heusler family.

Confinement of chiral magnetic modulations in the precursor region of FeGe.

We report on magnetic susceptibility and specific heat measurements of the cubic helimagnet FeGe in external magnetic fields and temperatures near the onset of long-range magnetic order at TC = 278.2(3) K. Pronounced anomalies in the field-dependent χac(H) data as well as in the corresponding imaginary part χ''ac(H) reveal a precursor region around TC in the magnetic phase diagram. The occurrence of a maximum at T0 = 279.6 K in the zero-field specific heat data indicates a second-order transition into a magnetically ordered state. A shoulder evolves above this maximum as a magnetic field is applied. The field dependence of both features coincides with crossover lines from the field-polarized to the paramagnetic state deduced from χac(T) at constant magnetic fields. The experimental findings are analyzed within the standard Dzyaloshinskii theory for cubic helimagnets. The remarkable multiplicity of modulated precursor states and the complexity of the magnetic phase diagram near the magnetic ordering are explained by the change of the character of solitonic inter-core interactions and the onset of specific confined chiral modulations in this area.

Precursor phenomena at the magnetic ordering of the cubic helimagnet FeGe.

We report on detailed magnetic measurements on the cubic helimagnet FeGe in external magnetic fields and temperatures near the onset of long-range magnetic order at T(C)=278.2(3) K. Precursor phenomena display a complex succession of temperature-driven crossovers and phase transitions in the vicinity of T(C). The A-phase region, present below T(C) and fields H<0.5 kOe, is split in several pockets. The complexity of the magnetic phase diagram is theoretically explained by the confinement of solitonic kinklike or Skyrmionic units that develop an attractive and oscillatory intersoliton coupling owing to the longitudinal inhomogeneity of the magnetization.

Adaptive modulations of martensites.

Modulated phases occur in numerous functional materials like giant ferroelectrics and magnetic shape-memory alloys. To understand the origin of these phases, we employ and generalize the concept of adaptive martensite. As a starting point, we investigate the coexistence of austenite, adaptive 14M phase, and tetragonal martensite in Ni-Mn-Ga magnetic shape-memory alloy epitaxial films. We show that the modulated martensite can be constructed from nanotwinned variants of the tetragonal martensite phase. By combining the concept of adaptive martensite with branching of twin variants, we can explain key features of modulated phases from a microscopic view. This includes metastability, the sequence of 6M-10M-14M-NM intermartensitic transitions, and the magnetocrystalline anisotropy.

Memory effect in Dy0.5Sr0.5MnO3 single crystals.

We have performed a series of magnetic aging experiments on single crystals of Dy(0.5)Sr(0.5)MnO(3). The results demonstrate striking memory and chaos-like effects in this insulating half-doped perovskite manganite and suggest the existence of strong magnetic relaxation mechanisms of a clustered magnetic state. The spin-glass-like state established below a temperature T(sg)≈ 34 K originates from quenched disorder arising due to the ionic-radii mismatch at the rare earth site. However, deviations from the typical behavior seen in canonical spin glass materials are observed which indicate that the glassy magnetic properties are due to cooperative and frustrated dynamics in a heterogeneous or clustered magnetic state. In particular, the microscopic spin flip time obtained from dynamical scaling near the spin glass freezing temperature is four orders of magnitude larger than microscopic times found in atomic spin glasses. The magnetic viscosity deduced from the time dependence of the zero-field-cooled magnetization exhibits a peak at a temperature T < T(sg) and displays a marked dependence on waiting time in zero field.

Phase transitions and rare-earth magnetism in hexagonal and orthorhombic DyMnO(3) single crystals.

The floating-zone method with different growth ambiences has been used to selectively obtain hexagonal or orthorhombic DyMnO(3) single crystals. The crystals were characterized by x-ray powder diffraction of ground specimens and a structure refinement as well as electron diffraction. We report magnetic susceptibility, magnetization and specific heat studies of this multiferroic compound in both the hexagonal and the orthorhombic structure. The hexagonal DyMnO(3) shows magnetic ordering of Mn(3+) (S = 2) spins on a triangular Mn lattice at T(N)(Mn) = 57 K characterized by a cusp in the specific heat. This transition is not apparent in the magnetic susceptibility due to the frustration on the Mn triangular lattice and the dominating paramagnetic susceptibility of the Dy(3+) (S = 9/2) spins. At T(N)(Dy) = 3 K, a partial antiferromagnetic order of Dy moments has been observed. In comparison, the magnetic data for orthorhombic DyMnO(3) display three transitions. The data broadly agree with results from earlier neutron diffraction experiments, which allows for the following assignment: a transition from an incommensurate antiferromagnetic ordering of Mn(3+) spins at T(N)(Mn) = 39 K, a lock-in transition at T(lock-in) = 16 K and a second antiferromagnetic transition at T(N)(Dy) = 5 K due to the ordering of Dy moments. Both the hexagonal and the orthorhombic crystals show magnetic anisotropy and complex magnetic properties due to 4f-4f and 4f-3d couplings.

Quantum order in the chiral magnet MnSi.

Systems lacking inversion symmetry, such as selected three-dimensional compounds, multilayers and surfaces support Dzyaloshinsky-Moriya (DM) spin-orbit interactions. In recent years DM interactions have attracted great interest, because they may stabilize magnetic structures with a unique chirality and non-trivial topology. The inherent coupling between the various properties provided by DM interactions is potentially relevant for a variety of applications including, for instance, multiferroic and spintronic devices. The, perhaps, most extensively studied material in which DM interactions are important is the cubic B20 compound MnSi. We review the magnetic field and pressure dependence of the magnetic properties of MnSi. At ambient pressure this material displays helical order. Under hydrostatic pressure a non-Fermi liquid state emerges, where a partial magnetic order, reminiscent of liquid crystals, is observed in a small pocket. Recent experiments strongly suggest that the non-Fermi liquid state is not due to quantum criticality. Instead it may be the signature of spin textures and spin excitations with a non-trivial topology.

Full tunability of strain along the fcc-bcc bain path in epitaxial films and consequences for magnetic properties.

Strained coherent film growth is commonly either limited to ultrathin films or low strains. Here, we present an approach to achieve high strains in thicker films, by using materials with inherent structural instabilities. As an example, 50 nm thick epitaxial films of the Fe70Pd30 magnetic shape memory alloy are examined. Strained coherent growth on various substrates allows us to adjust the tetragonal distortion from c/a{bct}=1.09 to 1.39, covering most of the Bain transformation path from fcc to bcc crystal structure. Magnetometry and x-ray circular dichroism measurements show that the Curie temperature, orbital magnetic moment, and magnetocrystalline anisotropy change over broad ranges.

Investigations on the spin-glass state in Dy(0.5)Sr(0.5)MnO(3) single crystals through structural, magnetic and thermal properties.

Single crystals of Dy(0.5)Sr(0.5)MnO(3) are grown using the optical floating zone technique, and their structural, magnetic, transport and thermal properties have been investigated. Magnetization measurements under field-cooled and zero-field-cooled conditions display irreversibility below 35 K. The magnetization does not saturate up to fields of 5 T in the temperature range 5-350 K. AC susceptibility shows a cusp around 32 K that shifts to higher temperature with increasing frequency. This frequency dependence of the peak temperature follows a critical slowing down with exponent zν = 3.6. Electrical resistivity shows insulating behavior, and the application of magnetic fields up to 10 T does not change this qualitative behavior. However, a marked negative magnetoresistance is observed in the paramagnetic phase reaching 80% at 70 K and 10 T. The observed resistivity behavior does not obey an activated type of conduction. These features are characteristic of spin-glass behavior in this half-doped insulating manganite. It is argued that the spin-glass-like state originates from the A-site disorder, which in turn results from the random distribution of cations with different ionic radii. Specific-heat measurements reveal a sizable linear contribution at low temperature that may be associated with the glassy magnetic ordering and a Schottky-like anomaly in a wide temperature range between 8 and 40 K. The distribution of Schottky levels is explained by the inhomogeneity of the molecular field in the spin-glass state that leads to variable splitting of the Kramers ground-state doublets in Dy(3+).

Non-Fermi liquid metal without quantum criticality.

A key question in condensed matter physics concerns whether pure three-dimensional metals can always be described as Fermi liquids. Using neutron Larmor diffraction to overcome the traditional resolution limit of diffraction experiments, we studied the lattice constants of the cubic itinerant-electron magnet manganese silicide (MnSi) at low temperatures and high pressures. We were able to resolve the nature of the phase diagram of MnSi and to establish that a stable, extended non-Fermi liquid state emerges under applied pressure without quantum criticality. This suggests that new forms of quantum order may be expected even far from quantum phase transitions.

Spontaneous skyrmion ground states in magnetic metals.

Since the 1950s, Heisenberg and others have addressed the problem of how to explain the appearance of countable particles in continuous fields. Stable localized field configurations were searched for an ingredient for a general field theory of elementary particles, but the majority of nonlinear field models were unable to predict them. As an exception, Skyrme succeeded in describing nuclear particles as localized states, so-called 'skyrmions'. Skyrmions are a characteristic of nonlinear continuum models ranging from microscopic to cosmological scales. Skyrmionic states have been found under non-equilibrium conditions, or when stabilized by external fields or the proliferation of topological defects. Examples are Turing patterns in classical liquids, spin textures in quantum Hall magnets, or the blue phases in liquid crystals. However, it has generally been assumed that skyrmions cannot form spontaneous ground states, such as ferromagnetic or antiferromagnetic order, in magnetic materials. Here, we show theoretically that this assumption is wrong and that skyrmion textures may form spontaneously in condensed-matter systems with chiral interactions without the assistance of external fields or the proliferation of defects. We show this within a phenomenological continuum model based on a few material-specific parameters that can be determined experimentally. Our model has a condition not considered before: we allow for softened amplitude variations of the magnetization, characteristic of, for instance, metallic magnets. Our model implies that spontaneous skyrmion lattice ground states may exist generally in a large number of materials, notably at surfaces and in thin films, as well as in bulk compounds, where a lack of space inversion symmetry leads to chiral interactions.