X-Ray Magnetic Circular Dichroism in Altermagnetic α-MnTe.

Altermagnetism is a recently identified magnetic symmetry class combining characteristics of conventional collinear ferromagnets and antiferromagnets, that were regarded as mutually exclusive, and enabling phenomena and functionalities unparalleled in either of the two traditional elementary magnetic classes. In this work we use symmetry, ab initio theory, and experiments to explore x-ray magnetic circular dichroism (XMCD) in the altermagnetic class. As a representative material for our XMCD study we choose α-MnTe with compensated antiparallel magnetic order in which an anomalous Hall effect has been already demonstrated. We predict and experimentally confirm a characteristic XMCD line shape for compensated moments lying in a plane perpendicular to the light propagation vector. Our results highlight the distinct phenomenology in altermagnets of this time-reversal symmetry breaking response, and its potential utility for element-specific spectroscopy and microscopy.

Altermagnetic lifting of Kramers spin degeneracy.

Lifted Kramers spin degeneracy (LKSD) has been among the central topics of condensed-matter physics since the dawn of the band theory of solids1,2. It underpins established practical applications as well as current frontier research, ranging from magnetic-memory technology3-7 to topological quantum matter8-14. Traditionally, LKSD has been considered to originate from two possible internal symmetry-breaking mechanisms. The first refers to time-reversal symmetry breaking by magnetization of ferromagnets and tends to be strong because of the non-relativistic exchange origin15. The second applies to crystals with broken inversion symmetry and tends to be comparatively weaker, as it originates from the relativistic spin-orbit coupling (SOC)16-19. A recent theory work based on spin-symmetry classification has identified an unconventional magnetic phase, dubbed altermagnetic20,21, that allows for LKSD without net magnetization and inversion-symmetry breaking. Here we provide the confirmation using photoemission spectroscopy and ab initio calculations. We identify two distinct unconventional mechanisms of LKSD generated by the altermagnetic phase of centrosymmetric MnTe with vanishing net magnetization20-23. Our observation of the altermagnetic LKSD can have broad consequences in magnetism. It motivates exploration and exploitation of the unconventional nature of this magnetic phase in an extended family of materials, ranging from insulators and semiconductors to metals and superconductors20,21, that have been either identified recently or perceived for many decades as conventional antiferromagnets21,24,25.

Spontaneous Anomalous Hall Effect Arising from an Unconventional Compensated Magnetic Phase in a Semiconductor.

The anomalous Hall effect, commonly observed in metallic magnets, has been established to originate from the time-reversal symmetry breaking by an internal macroscopic magnetization in ferromagnets or by a noncollinear magnetic order. Here we observe a spontaneous anomalous Hall signal in the absence of an external magnetic field in an epitaxial film of MnTe, which is a semiconductor with a collinear antiparallel magnetic ordering of Mn moments and a vanishing net magnetization. The anomalous Hall effect arises from an unconventional phase with strong time-reversal symmetry breaking and alternating spin polarization in real-space crystal structure and momentum-space electronic structure. The anisotropic crystal environment of magnetic Mn atoms due to the nonmagnetic Te atoms is essential for establishing the unconventional phase and generating the anomalous Hall effect.

Electrically induced and detected Néel vector reversal in a collinear antiferromagnet.

Antiferromagnets are enriching spintronics research by many favorable properties that include insensitivity to magnetic fields, neuromorphic memory characteristics, and ultra-fast spin dynamics. Designing memory devices with electrical writing and reading is one of the central topics of antiferromagnetic spintronics. So far, such a combined functionality has been demonstrated via 90° reorientations of the Néel vector generated by the current-induced spin orbit torque and sensed by the linear-response anisotropic magnetoresistance. Here we show that in the same antiferromagnetic CuMnAs films as used in these earlier experiments we can also control 180° Néel vector reversals by switching the polarity of the writing current. Moreover, the two stable states with opposite Néel vector orientations in this collinear antiferromagnet can be electrically distinguished by measuring a second-order magnetoresistance effect. We discuss the general magnetic point group symmetries allowing for this electrical readout effect and its specific microscopic origin in CuMnAs.

Multiple-stable anisotropic magnetoresistance memory in antiferromagnetic MnTe.

Commercial magnetic memories rely on the bistability of ordered spins in ferromagnetic materials. Recently, experimental bistable memories have been realized using fully compensated antiferromagnetic metals. Here we demonstrate a multiple-stable memory device in epitaxial MnTe, an antiferromagnetic counterpart of common II-VI semiconductors. Favourable micromagnetic characteristics of MnTe allow us to demonstrate a smoothly varying zero-field antiferromagnetic anisotropic magnetoresistance (AMR) with a harmonic angular dependence on the writing magnetic field angle, analogous to ferromagnets. The continuously varying AMR provides means for the electrical read-out of multiple-stable antiferromagnetic memory states, which we set by heat-assisted magneto-recording and by changing the writing field direction. The multiple stability in our memory is ascribed to different distributions of domains with the Néel vector aligned along one of the three magnetic easy axes. The robustness against strong magnetic field perturbations combined with the multiple stability of the magnetic memory states are unique properties of antiferromagnets.

Magneto-elastic coupling across the first-order transition in the distorted kagome lattice antiferromagnet Dy3Ru4Al12.

Structural changes through the first-order paramagnetic-antiferromagnetic phase transition of Dy3Ru4Al12 at 7 K have been studied by means of X-ray diffraction and thermal expansion measurements. The compound crystallizes in a hexagonal crystal structure of Gd3Ru4Al12 type (P63/mmc space group), and no structural phase transition has been found in the temperature interval between 2.5 and 300 K. Nevertheless, due to the spin-lattice coupling the crystal volume undergoes a small orthorhombic distortion of the order of 2×10-5 as the compound enters the antiferromagnetic state. We propose that the first-order phase transition is not driven by the structural changes but rather by the exchange interactions present in the system.

UH3-based ferromagnets: new look at an old material.

UH3 is the first discovered material with ferromagnetism based purely on the 5f electronic states, known for more than half century. Although the U metal is Pauli paramagnet, the reduced 5f-5f overlap in compounds allows for moment formation and ordering, typically if the U-U spacing exceeds the Hill limit, i.e. about 340 pm. The stable form of UH3, known as ß-UH3, has rather high TC ≈ 170 K. Such high value is rather unusual, considering dU-U = 331 pm. Properties of metastable α-UH3 with dU-U = 360 pm could be never well established. Using the fact that α-UH3 is in fact bcc U with interstitials filled by H, we attempted to synthesize α-UH3 starting from the γ-U alloys, with the bcc structure retained to room temperature by doping combined with ultrafast cooling. While up to 15% Zr a contamination by ß-UH3 was obtained, 20% Zr yielded single phase α-UH3. The TC value remains high and very similar to ß-UH3. One can see an increase up to 187 K for 15% Zr, followed by a weak decrease. Magnetic moments remain close to 1 µB/U atom. An insight is provided by ab-initio calculations, revealing a a charge transfer towards H-1s states, depopulating the U-6d and 7s states, leaving almost pure 5f character around the Fermi level. The 5f magnetism exhibits a high coercivity (µ0Hc up to 5.5 T) and large spontaneous volume magnetostriction of 3.2*10-3. Even higher increase of TC, reaching up to 203 K, can be achieved in analogous Mo stabilized hydrides, which yield an amorphous structure. The compounds represent, together with known hydrides of U6Fe and U6Co, a new group of robust 5f ferromagnets with small dU-U but high TC. Although common hydrides are fine powders, some of the new hydrides described as (UH3)(1-x)T x (T = Zr or Mo) remain monolithic, which allows to study transport and thermodynamic properties.

Electronic properties of α-UH3 stabilized by Zr.

Pure hydride of the α-UH3 type without any ß-UH3 admixture was prepared by high-pressure hydrogenation of bcc U stabilized by Zr. Such material, characterized by a general formula (UH3)1-x Zr x , is stable in air at ambient and elevated temperatures. H release is observed between 400-450 °C similar to ß-UH3. Its stability allowed to measure magnetic properties, specific heat, and electrical resistivity in a wide temperature range. Despite rather different crystal structure and inter-U spacing, the electronic properties are almost identical to ß-UH3. Its ferromagnetic ground state with Curie temperature TC ≈ 180 K (weakly and non-monotonously dependent on Zr concentration) and U moments of 1.0 µB indicate why mixtures of α- and ß-UH3 exhibited only one transition. Magnetic ordering leads to a large spontaneous magnetostriction ωs = 3.2*10-3, which can be explained by the increase of the spin moment between the paramagnetic (Disordered Local Moment) and the ferromagnetic state. The role of orbital moments in magnetism is indicated by fully relativistic electronic structure calculations.

Growth kinetics of ω particles in ß-Ti matrix studied by in-situ small-angle x-ray scattering.

Nucleation and growth kinetics of nanoparticles of hexagonal ω phase in a body-centered cubic ß titanium matrix in single crystals of ß-Ti alloys were investigated by small-angle x-ray scattering measured in-situ during ageing at various temperatures up to 450 °C. The experimental data were compared with numerical simulations based on a three-dimensional short-range order model of nanoparticle self-ordering. The x-ray contrast of the particles is caused by an inhomogeneous distribution of impurity atoms (Mo, Fe and Al), whose density profile around growing nanoparticles was simulated by solving the corresponding diffusion equation with moving boundary conditions. From the analysis of the experimental data we determined the mean distance and size of the nanoparticles and confirmed the validity of the ∝ t1/3 growth law following from the Lifshitz-Slyozov-Wagner theory. From a detailed comparison of the experimental data with simulations we also assessed the diffusion coefficient of the impurity atoms and its activation energy.

Structural investigation of GaInP nanowires using X-ray diffraction.

In this work the structure of ternary Ga x In1 - x P nanowires is investigated with respect to the chemical composition and homogeneity. The nanowires were grown by metal-organic vapor-phase epitaxy. For the investigation of ensemble fluctuations on several lateral length scales, X-ray diffraction reciprocal space maps have been analyzed. The data reveal a complicated varying materials composition across the sample and in the nanowires on the order of 20%. The use of modern synchrotron sources, where beam-sizes in the order of several 10 µm are available, enables us to investigate compositional gradients along the sample by recording diffraction patterns at different positions. In addition, compositional variations were found also within single nanowires in X-ray energy dispersive spectroscopy measurements.

Tetragonal phase of epitaxial room-temperature antiferromagnet CuMnAs.

Recent studies have demonstrated the potential of antiferromagnets as the active component in spintronic devices. This is in contrast to their current passive role as pinning layers in hard disk read heads and magnetic memories. Here we report the epitaxial growth of a new high-temperature antiferromagnetic material, tetragonal CuMnAs, which exhibits excellent crystal quality, chemical order and compatibility with existing semiconductor technologies. We demonstrate its growth on the III-V semiconductors GaAs and GaP, and show that the structure is also lattice matched to Si. Neutron diffraction shows collinear antiferromagnetic order with a high Néel temperature. Combined with our demonstration of room-temperature-exchange coupling in a CuMnAs/Fe bilayer, we conclude that tetragonal CuMnAs films are suitable candidate materials for antiferromagnetic spintronics.

Direct band gap wurtzite gallium phosphide nanowires.

The main challenge for light-emitting diodes is to increase the efficiency in the green part of the spectrum. Gallium phosphide (GaP) with the normal cubic crystal structure has an indirect band gap, which severely limits the green emission efficiency. Band structure calculations have predicted a direct band gap for wurtzite GaP. Here, we report the fabrication of GaP nanowires with pure hexagonal crystal structure and demonstrate the direct nature of the band gap. We observe strong photoluminescence at a wavelength of 594 nm with short lifetime, typical for a direct band gap. Furthermore, by incorporation of aluminum or arsenic in the GaP nanowires, the emitted wavelength is tuned across an important range of the visible light spectrum (555-690 nm). This approach of crystal structure engineering enables new pathways to tailor materials properties enhancing the functionality.

Particle-assisted Ga(x)In(1-x)P nanowire growth for designed bandgap structures.

Non-tapered vertically straight Ga(x)In(1-x)P nanowires were grown in a compositional range from Ga(0.2)In(0.8)P to pure GaP in particle-assisted mode by controlling the trimethylindium, trimethylgallium and hydrogen chloride flows in metal-organic vapor phase epitaxy. X-ray energy dispersive spectroscopy in transmission electron microscopy revealed homogeneous radial material composition in single nanowires, whereas variations in the material composition were found along the nanowires. High-resolution x-ray diffraction indicates a variation of the material composition on the order of about 19% measuring an entire sample area, i.e., including edge effects during growth. The non-capped nanowires emit room temperature photoluminescence strongly in the energy range of 1.43-2.16 eV, correlated with the bandgap expected from the material composition.

Unit cell parameters of wurtzite InP nanowires determined by x-ray diffraction.

High resolution x-ray diffraction is used to study the structural properties of the wurtzite polytype of InP nanowires. Wurtzite InP nanowires are grown by metal-organic vapor phase epitaxy using S-doping. From the evaluation of the Bragg peak position we determine the lattice parameters of the wurtzite InP nanowires. The unit cell dimensions are found to differ from the ones expected from geometric conversion of the cubic bulk InP lattice constant. The atomic distances along the c direction are increased whereas the atomic spacing in the a direction is reduced in comparison to the corresponding distances in the zinc-blende phase. Using core/shell nanowires with a thin core and thick nominally intrinsic shells we are able to determine the lattice parameters of wurtzite InP with a negligible influence of the S-doping due to the much larger volume in the shell. The determined material properties will enable the ab initio calculation of electronic and optical properties of wurtzite InP nanowires.