Observation of the Anomalous Hall Effect in a Layered Polar Semiconductor.

Progress in magnetoelectric materials is hindered by apparently contradictory requirements for time-reversal symmetry broken and polar ferroelectric electronic structure in common ferromagnets and antiferromagnets. Alternative routes can be provided by recent discoveries of a time-reversal symmetry breaking anomalous Hall effect (AHE) in noncollinear magnets and altermagnets, but hitherto reported bulk materials are not polar. Here, the authors report the observation of a spontaneous AHE in doped AgCrSe2 , a layered polar semiconductor with an antiferromagnetic coupling between Cr spins in adjacent layers. The anomalous Hall resistivity 3 µ Ω c m $\mu \Omega \, \textnormal {cm}$ is comparable to the largest observed in compensated magnetic systems to date, and is rapidly switched off when the angle of an applied magnetic field is rotated to ≈80° from the crystalline c-axis. The ionic gating experiments show that the anomalous Hall conductivity magnitude can be enhanced by modulating the p-type carrier density. They also present theoretical results that suggest the AHE is driven by Berry curvature due to noncollinear antiferromagnetic correlations among Cr spins, which are consistent with the previously suggested magnetic ordering in AgCrSe2 . The results open the possibility to study the interplay of magnetic and ferroelectric-like responses in this fascinating class of materials.

Electron spin resonance on the spin-1/2 triangular magnet NaYbS2.

The delafossite structure of NaYbS2 contains a planar spin-1/2 triangular lattice of Yb3+ ions and features a possible realisation of a quantum spin-liquid state. We investigated the Yb3+ spin dynamics by electron spin resonance (ESR) in single-crystalline samples of NaYbS2. Very clear spectra with a well-resolved and large anisotropy could be observed down to the lowest accessible temperature of 2.7 K. In contrast to the ESR properties of other known spin-liquid candidate systems, the resonance seen in NaYbS2 is accessible at low fields (<1 T) and is narrow enough for accurate characterisation of the relaxation rate as well as the g factor of the Yb3+ spins.

On Fe-Fe Dumbbells in the Ideal and Real Structures of FeGa3.

The intermetallic phase FeGa3 belongs to the rare examples of substances with transition metals where semiconducting behavior is found. The necessary electron count of 17 ve/fu can be formally derived from eight Fe-Ga and one Fe-Fe two-center-two-electron bond. The situation is reminiscent of the well-known Fe2(CO)9 scenario, where a direct Fe-Fe two-center-two-electron bond was shown to not be present. Fe-Fe interaction in FeGa3 and its substitution variants represents the crucial point for explanation of electronic, thermal transport, and optical properties of this material. Chemical bonding analysis in position space of FeGa3 and Fe2(CO)9 on the basis of the topology of the electron localizability indicator distribution, QTAIM atoms, two- and three-center delocalization indices, domain natural orbitals, IQA analysis, and an evaluation of the Fe-Fe dissociation energy yields a complete picture of the partially compensated Fe-Fe bond, which is nevertheless strong enough to be of decisive importance. Structural reinvestigation of differently synthesized single crystals leads to the composition Fe1+ xGa3 (0 ≤ x ≤ 0.018), where the additional Fe atoms are predicted from DFT/PBE calculations to yield a magnetic moment of about 2 µB/Fe2 atom and metallic in-gap states. Accompanying magnetization and ESR measurements are consistent with this picture.

Resonant torsion magnetometry in anisotropic quantum materials.

Unusual behavior in quantum materials commonly arises from their effective low-dimensional physics, reflecting the underlying anisotropy in the spin and charge degrees of freedom. Here we introduce the magnetotropic coefficient k = ∂2F/∂θ2, the second derivative of the free energy F with respect to the magnetic field orientation θ in the crystal. We show that the magnetotropic coefficient can be quantitatively determined from a shift in the resonant frequency of a commercially available atomic force microscopy cantilever under magnetic field. This detection method enables part per 100 million sensitivity and the ability to measure magnetic anisotropy in nanogram-scale samples, as demonstrated on the Weyl semimetal NbP. Measurement of the magnetotropic coefficient in the spin-liquid candidate RuCl3 highlights its sensitivity to anisotropic phase transitions and allows a quantitative comparison to other thermodynamic coefficients via the Ehrenfest relations.

Spin dynamics of FeGa3-x Ge x studied by electron spin resonance.

The intermetallic semiconductor FeGa3 acquires itinerant ferromagnetism upon electron doping by a partial replacement of Ga with Ge. We studied the electron spin resonance (ESR) of high-quality single crystals of FeGa3-x Ge x for x from 0 up to 0.162 where ferromagnetic order is observed. For x = 0 we observed a well-defined ESR signal, indicating the presence of pre-formed magnetic moments in the semiconducting phase. Upon Ge doping the occurrence of itinerant magnetism clearly affects the ESR properties below ≈40 K, whereas at higher temperatures an ESR signal as seen in FeGa3 prevails independent on the Ge content. The present results show that the ESR of FeGa3-x Ge x is an appropriate and direct tool to investigate the evolution of 3d-based itinerant magnetism.

Negative magnetoresistance without well-defined chirality in the Weyl semimetal TaP.

Weyl semimetals (WSMs) are topological quantum states wherein the electronic bands disperse linearly around pairs of nodes with fixed chirality, the Weyl points. In WSMs, nonorthogonal electric and magnetic fields induce an exotic phenomenon known as the chiral anomaly, resulting in an unconventional negative longitudinal magnetoresistance, the chiral-magnetic effect. However, it remains an open question to which extent this effect survives when chirality is not well-defined. Here, we establish the detailed Fermi-surface topology of the recently identified WSM TaP via combined angle-resolved quantum-oscillation spectra and band-structure calculations. The Fermi surface forms banana-shaped electron and hole pockets surrounding pairs of Weyl points. Although this means that chirality is ill-defined in TaP, we observe a large negative longitudinal magnetoresistance. We show that the magnetoresistance can be affected by a magnetic field-induced inhomogeneous current distribution inside the sample.

Design of compensated ferrimagnetic Heusler alloys for giant tunable exchange bias.

Rational material design can accelerate the discovery of materials with improved functionalities. This approach can be implemented in Heusler compounds with tunable magnetic sublattices to demonstrate unprecedented magnetic properties. Here, we have designed a family of Heusler alloys with a compensated ferrimagnetic state. In the vicinity of the compensation composition in Mn-Pt-Ga, a giant exchange bias (EB) of more than 3 T and a large coercivity are established. The large exchange anisotropy originates from the exchange interaction between the compensated host and ferrimagnetic clusters that arise from intrinsic anti-site disorder. Our design approach is also demonstrated on a second material with a magnetic transition above room temperature, Mn-Fe-Ga, exemplifying the universality of the concept and the feasibility of room-temperature applications. These findings may lead to the development of magneto-electronic devices and rare-earth-free exchange-biased hard magnets, where the second quadrant magnetization can be stabilized by the exchange bias.