A-type Antiferromagnetic State Research Articles

Magnetism and Superconductivity in the t–J Model of La3Ni2O7 Under Multiband Gutzwiller Approximation

The recent discovery of possible high temperature superconductivity in single crystals of La3Ni2O7 under pressure renews the interest in research on nickelates. The density functional theory calculations reveal that both d z 2 and d x 2–y 2 orbitals are active, which suggests a minimal two-orbital model to capture the low-energy physics of this system. In this work, we study a bilayer two-orbital t–J model within multiband Gutzwiller approximation, and discuss the magnetism as well as the superconductivity over a wide range of the hole doping. Owing to the inter-orbital super-exchange process between d z 2 and d x 2–y 2 orbitals, the induced ferromagnetic coupling within layers competes with the conventional antiferromagnetic coupling, and leads to complicated hole doping dependence for the magnetic properties in the system. With increasing hole doping, the system transfers to A-type antiferromagnetic state from the starting G-type antiferromagnetic (G-AFM) state. We also find the inter-layer superconducting pairing of d x 2–y 2 orbitals dominates due to the large hopping parameter of d z 2 along the vertical inter-layer bonds and significant Hund’s coupling between d z 2 and d x 2–y 2 orbitals. Meanwhile, the G-AFM state and superconductivity state can coexist in the low hole doping regime. To take account of the pressure, we also analyze the impacts of inter-layer hopping amplitude on the system properties.

Exchange Bias Modulated by Antiferromagnetic Spin-Flop Transition in 2D Van der Waals Heterostructures.

Exchange bias is extensively studied and widely utilized in spintronic devices, such as spin valves and magnetic tunnel junctions. 2D van der Waals (vdW) magnets, with high-quality interfaces in heterostructures, provide an excellent platform for investigating the exchange bias effect. To date, intrinsic modulation of exchange bias, for instance, via precise manipulation of the magnetic phases of the antiferromagnetic layer, is yet to be fully reached, owing partly to the large exchange fields of traditional bulk antiferromagnets. Herein, motivated by the low-field spin-flop transition of a 2D antiferromagnet, CrPS4, exchange bias is explored by modulatingthe antiferromagnetic spin-flop phase transition in all-vdW magnetic heterostructures. The results demonstrate that undergoing the spin-flop transition during the field cooling process, the A-type antiferromagnetic ground state of CrPS4 turns into a canted antiferromagnetic one, therefore, it reduces the interfacial magnetic coupling and suppresses the exchange bias. Via conducting different cooling fields, one can select the exchange bias effect switching among the "ON", "depressed", and "OFF" states determined by the spin flop of CrPS4. This work provides an approach to intrinsically modulate the exchange bias in all-vdW heterostructures and paves new avenues to design and manipulate 2D spintronic devices.

Fully Magnetically Polarized Ultrathin La0.8Sr0.2MnO3 Films.

We report the observation of fully magnetically polarized ultrathin La0.8Sr0.2MnO3 films by using LaMnO3 and La0.45Sr0.55MnO3 buffer layers grown epitaxially on SrTiO3(001) substrates by molecular beam epitaxy. Specifically, we show that La0.8Sr0.2MnO3 films grown on 12-unit-cell LaMnO3 have bulk-like magnetic moments starting from a single unit cell thickness, while for the 15-unit-cell La0.45Sr0.55MnO3 buffer layer, the La0.8Sr0.2MnO3 transitions from an antiferromagnetic state to a fully spin-polarized ferromagnetic state at 4 unit cells. The magnetic results are confirmed by X-ray magnetic circular dichroism, while linear dichroic measurements carried out for the La0.8Sr0.2MnO3/La0.45Sr0.55MnO3 series show the presence of an orbital reorganization at the transition from the antiferromagnetic to ferromagnetic state corresponding to a change from a preferred in-plane orbital hole occupancy, characteristic of the A-type antiferromagnetic state of La0.45Sr0.55MnO3, to preferentially out of plane. We interpret our findings in terms of the different electronic charge transfers between the adjacent layers, confined to the unit cell in the case of insulating LaMnO3 and extended to a few unit cells in the case of conducting La0.45Sr0.55MnO3. Our work demonstrates an approach to growing ultrathin mixed-valence manganite films that are fully magnetically polarized from the single unit cell, paving the way to fully exploring the unique electronic properties of this class of strongly correlated oxide materials.

Pressure-tunable magnetic topological phases in magnetic topological insulator MnSb4Te7

Magnetic topological insulators (TIs), possessing both magnetic order and topological electronic structure, provides an excellent platform to research unusual physical properties. Here, we report a high-pressure study on the anomalous Hall effect of magnetic TI MnSb4Te7 through transports measurements combined with first-principle theoretical calculations. We discover that the ground state of MnSb4Te7 experiences a magnetic phase transition from the A-type antiferromagnetic state to ferromagnetic dominating state at 3.78 GPa, although its crystal sustains a rhombohedral phase under high pressures. The anomalous Hall conductance σxyA is dominated by intrinsic mechanism even after the magnetic phase transition. The results shed light on the intriguing magnetism in MnSb4Te7 and pave the way for further studies of the relationship between topology and magnetism in topological materials.

Dynamic magnetic crossover at the origin of the hidden-order in van der Waals antiferromagnet CrSBr

The van-der-Waals material CrSBr stands out as a promising two-dimensional magnet. Here, we report on its detailed magnetic and structural characteristics. We evidence that it undergoes a transition to an A-type antiferromagnetic state below TN ≈ 140 K with a pronounced two-dimensional character, preceded by ferromagnetic correlations within the monolayers. Furthermore, we unravel the low-temperature hidden-order within the long-range magnetically-ordered state. We find that it is associated to a slowing down of the magnetic fluctuations, accompanied by a continuous reorientation of the internal field. These take place upon cooling below Ts ≈ 100 K, until a spin freezing process occurs at T* ≈ 40 K. We argue this complex behavior to reflect a crossover driven by the in-plane uniaxial anisotropy, which is ultimately caused by its mixed-anion character. Our findings reinforce CrSBr as an important candidate for devices in the emergent field of two-dimensional magnetic materials.

Magnetic resonances in EuSn[formula omitted]As[formula omitted] single crystal

In this work, we report the broad-band ferromagnetic resonance spectroscopy of EuSn2As2 single crystals at different temperatures in combination with magnetization measurements and structural characterization. We observe conventional collective acoustic resonance mode of the A-type antiferromagnetic canted state in the Eu sub-lattice, and its transition to the paramagnetic resonance above the ordering temperature. Furthermore, we observe reproducibly additional well-defined spectral line. The origin of the additional line remains unclear. However, its temperature dependence associates it with the magnetism in the Eu sub-lattice.

Pressure-densified new rhombohedral phase of EuSn2As2

The magnetic topological insulator ${\mathrm{EuSn}}_{2}{\mathrm{As}}_{2}$ is known to crystallize in a ${\mathrm{Bi}}_{2}{\mathrm{Te}}_{3}$-type layered structure in rhombohedral symmetry at ambient conditions and undergo a structural phase transition toward a monoclinic $\ensuremath{\beta}$ phase under increasing pressure. Here, we identify by ab initio calculations a new high-pressure rhombohedral structure (termed the $\ensuremath{\gamma}$ phase) in $R\overline{3}m$ symmetry comprising Sn-As-As-Sn linear chains along the $z$ axis via the formation of As-As bonds in the AsSn/SnAs bilayers with strong anisotropic lattice distortion along the [001] orientation. This pressure-densified new rhombohedral phase has a metallic A-type antiferromagnetic ground state and is energetically more favorable than the original rhombohedral structure and the monoclinic $\ensuremath{\beta}$ phase above 11 GPa. Simulated x-ray diffraction patterns provide an excellent match to the previously unexplained distinct diffraction peak around $14.{7}^{\ensuremath{\circ}}$ found in experiments for ${\mathrm{EuSn}}_{2}{\mathrm{As}}_{2}$ above 13 GPa. These findings offer key insights into a new type of high-pressure phase of layered magnetic topological insulators, laying a foundation for further exploration of this intriguing class of materials.

Experimental evidence for field-induced metamagnetic transition of EuCd2As2

Recent studies have shown that layered compound EuCd2As2 could exhibit diverse topological states depending on the different magnetic structures, such as Weyl semimetal, Dirac semimetal and topological insulator. In order to further study the interplay between magnetism and topology of EuCd2As2, it is necessary to figure out its magnetic structure. Here, by magnetization (M) measurements and negative magnetostriction (λ) along the [001] direction measured by scanning tunneling microscopy on EuCd2As2 single crystals, we observe field-induced metamagnetic phase transition from A-type antiferromagnetic (AFM) ground state to field-polarized state, with canted AFM (CAFM) state in between. Magnetization and magnetostriction are more sensitive to the in-plane field than the out-of-plane field, indicating the magnetic moments lying in the ab plane. The absence of abrupt jump on M-H and λ-H curves demonstrates that the phase transition is a second-order type. In CAFM state, M increases linearly with the field and λ is proportional to M2. Tunneling conductance spectra show the field-induced evolution of the electronic density of states. Our results provide experimental evidence for understanding the magnetic structure of EuCd2As2.

Multiple Magnetic Topological Phases in Bulk van der Waals Crystal MnSb_{4}Te_{7}.

The magnetic van der Waals crystals MnBi_{2}Te_{4}/(Bi_{2}Te_{3})_{n} have drawn significant attention due to their rich topological properties and the tunability by external magnetic field. Although the MnBi_{2}Te_{4}/(Bi_{2}Te_{3})_{n} family have been intensively studied in the past few years, their close relatives, the MnSb_{2}Te_{4}/(Sb_{2}Te_{3})_{n} family, remain much less explored. In this work, combining magnetotransport measurements, angle-resolved photoemission spectroscopy, and first principles calculations, we find that MnSb_{4}Te_{7}, the n=1 member of the MnSb_{2}Te_{4}/(Sb_{2}Te_{3})_{n} family, is a magnetic topological system with versatile topological phases that can be manipulated by both carrier doping and magnetic field. Our calculations unveil that its A-type antiferromagnetic (AFM) ground state stays in a Z_{2} AFM topological insulator phase, which can be converted to an inversion-symmetry-protected axion insulator phase when in the ferromagnetic (FM) state. Moreover, when this system in the FM phase is slightly carrier doped on either the electron or hole side, it becomes a Weyl semimetal with multiple Weyl nodes in the highest valence bands and lowest conduction bands, which are manifested by the measured notable anomalous Hall effect. Our work thus introduces a new magnetic topological material with different topological phases that are highly tunable by carrier doping or magnetic field.

Magnetism-induced ideal Weyl state in bulk van der Waals crystal MnSb2Te4

We have unveiled a magnetic exchange-induced topological phase transition in a bulk natural van der Waals crystal MnSb2Te4, based on magnetization and magnetotransport measurements and first principles calculations. At the A-type antiferromagnetic ground state, MnSb2Te4 is a topologically trivial insulator with a bandgap of ∼ 42 meV at the Γ point of the Brillouin zone. A small magnetic field less than 1.4 T along the c axis can drive the system into a spin fully polarized state, which hosts only a single pair of Weyl points setting near the Γ point at the Fermi level without other band mixing, supported by both the first principles calculations and the measured anomalous Hall effect. The results would setup an excellent paradigm for the study of interplay between magnetism and nontrivial topology of the electronic band structure.

On the electronic structure and magnetism of CaCrO3: A hybrid-exchange density-functional-theory study

Recently the perovskite oxide CaCrO3 has raised concerns for its ground-state electronic structure and magnetic properties. In this report, the hybrid-exchange density functional, PBE0, is used to calculate the electronic structure and magnetic properties of CaCrO3. The ferromagnetic, A-type anti-ferromagnetic, C-type anti-ferromagnetic, and G-type anti-ferromagnetic states (defined in the text) have been investigated carefully. The computed magnetic ground state has a G-type anti-ferromagnetic configuration (the Néel state). The calculation result is that the nearest-neighboring exchange interactions in the ab-plane and along the c-axis are antiferromagnetic. The next-nearest-neighboring exchange interaction in the ab-plane is much weak but ferromagnetic. We hope this work would shed some light on the controversial ground state of CaCrO3.

Emergent multiferroicity and strain-driven metal-semiconductor transitions in LaMnO3/RMnO3 superlattices (R = Pr, Pm, Sm and Gd).

It is known that rare-earth manganites LnMnO3 with Ln = La to Gd are typical Mott insulators favoring the A-type antiferromagnetic (A-AFM) state. Certainly no ferroelectricity can be possible although the alternatively stacked LnO layers are both polar. Nevertheless, under the inspiration that one plus one is more than two, it is appreciated that by combining two components of this manganite series into a superlattice functionality is added. In this work, we construct a (001)-oriented LaMnO3/RMnO3 (R = Pr, Pm, Sm and Gd) superlattice and investigate the possible emergent ferroelectricity by means of first-principles calculations. It is revealed that the lattice matching in these superlattices may generate lattice distortions to each component based on the scenario of hybrid improper ferroelectricity, resulting in spontaneous ferroelectric polarization, which is larger than the traditional type II Ln'MnO3 (Ln' radius is smaller than that of Gd) polarization. In the meantime, the A-AFM state remains the magnetic ground state of these superlattices. Furthermore, it is predicted that the externally imposed in-plane compressive strain can trigger the semiconductor to half-metal transitions accompanying the A-AFM to ferromagnetic (FM) transitions. The present work sheds light on the possibility to design multiferroic materials and functionality by tailoring artificial superlattices/heterostructures from those non-ferroelectric systems, and to design electronic devices by utilizing the electronic transport properties under epitaxial strain.

Feasibility of ground state spin switching in a molecular analogue of the mixed-metal oxides with the perovskite structure

The carboxylate substitution reaction between the reported all-benzoate complex [Ce3Mn8O8(PhCO2)18(PhCO2H)2] (1) and 2-Cl-benzoic acid has led to isolation of [Ce3Mn8O8(2-Cl-PhCO2)15.3(PhCO2)2.7(H2O)2] (2). The structures of 1 and 2 are very similar, both containing a tetragonally-elongated MnIII8 cuboid with a CeIV at its center and two CeIII attached to opposite faces, but 2 shows extensive disorder in the ligands and the Cl atom positions and occupancies. Variable-temperature (T) solid-state dc and ac magnetic susceptibility data for 2 are significantly different from those for 1 and are assigned as due to small ligand-induced structural perturbation of the core that has brought an A-type antiferromagnetic (AF) excited state much closer to the C-type AF ground state. Fits of the dc χMT vs T data support this interpretation but due to the ligand disorder in 2, a more definitive description of the lowest energy spin states of 2 is not possible. Nevertheless, these results provide important support for the feasibility of ground state spin switching by ligand-induced core perturbation (‘chemical pressure’) in this family, and they encourage further studies.

Magnetic properties of the itinerant A- type antiferromagnet CaCo2P2 studied by Co59 and P31 nuclear magnetic resonance

$^{59}$Co and $^{31}$P nuclear magnetic resonance (NMR) measurements in external magnetic and zero magnetic fields have been performed to investigate the magnetic properties of the A-type antiferromagnetic (AFM) CaCo$_2$P$_2$. NMR data, especially, the nuclear spin lattice relaxation rates 1/$T_1$ exhibiting a clear peak, provide clear evidence for the AFM transition at a N\'eel temperature of $T_{\rm N}\sim$110~K. The magnetic fluctuations in the paramagnetic state were found to be three-dimensional ferromagnetic, suggesting ferromagnetic interaction between Co spins in the ${\it ab}$ plane characterize the spin correlations in the paramagnetic state. In the AFM state below $T_{\rm N}$, we have observed $^{59}$Co and $^{31}$P NMR signals under zero magnetic field. From $^{59}$Co NMR data, the ordered magnetic moments of Co are found to be in $ab$ plane and are estimated to be 0.35 $\mu_{\rm B}$ at 4.2 K. Furthermore, the external field dependence of $^{59}$Co NMR spectrum in the AFM state suggests a very weak magnetic anisotropy of the Co ions and also provides microscopic evidence of canting the Co ordered moments along the external magnetic field directions. The magnetic state of the Co ions in CaCo$_2$P$_2$ is well explained by the local moment picture in the AFM state, although the system is metallic as seen by $1/T_1T$ = constant behavior.

Magnetic states in a three-dimensional topological Kondo insulator

We theoretically study the magnetic phase diagram of a three-dimensional topological Kondo insulator by means of real-space dynamical mean field theory. We find that ferromagnetically ordered states become stable upon hole doping. Besides a wide ferromagnetic phase, we observe surface magnetism close to half-filling, which corresponds to an A-type antiferromagnetic state. We further study the impact of the magnetism on the symmetry protected surface states and find that depending on the surface and the magnetization direction, surface states are still protected by reflection symmetry present in our model. The symmetry protected surface states are shifted away by the magnetization from their original high symmetry momenta in the Brillouin zone. Remarkably, due to the magnetization, the surface states are deformed, resulting in the appearance of arcs in the momentum resolved spectrum.

High-field magnetoconductance in La-Sr manganites of FM and AFM ground states

Large-grain La1–xSrxMnO3 ceramic samples of compositions x = 0.45 and 0.55, representing the ferromagnetic (FM) and A-type antiferromagnetic (AFM) ground states, were produced via classical sintering at 1500 °C of cold-pressed sol-gel prepared single-phase nanoparticles. Using the same precursors, nanogranular forms of both manganite ceramics were prepared by fast spark plasma sintering at low temperature of 900 °C, which limits the growth of crystal grains. The magnetotransport of both the bulk and nanogranular forms was investigated in a broad range of magnetic fields up to 130 kOe and analyzed on the basis of detailed magnetic measurements. Both the large-grain and nanogranular systems with x = 0.45, possessing a pure FM state with similar Curie tempereature TC ≈ 345 K), show nearly the same conductivity enhancement in external fields when expressed relatively to the zero-field values. This positive magnetoconductance (MC) can be separated into two terms: (i) the hysteretic low-field MC that reflects the field-induced orientation of magnetic moments of individual grains, and (ii) the high-field MC that depends linearly on external field. In the case of large-grain ceramics with x = 0.55, a partially ordered FM state formed below TC = 264 K is replaced by pure A-type AFM ground state below 204 K. This A-type AFM state is characterized by positive magnetoconductance that is essentially of quadratic dependence on external field in the investigated range up to 130 kOe. On contrary, the nanogranular product with x = 0.55 exhibits a mixed FM/AFM state at low temperatures, and, as a consequence, its magnetotransport combines the features of FM and A-type AFM systems, in which the quadratic term is much enhanced and clearly dominates at high fields. For interpretation of observed behaviors, the theory of grain-boundary tunneling is revisited.

The structural properties of LaRO3 (R=Cr, Mn, Fe): a first-principles calculation

We investigate the structural properties of three lanthanum transition-metal oxides (LaRO3, R=Cr, Mn, Fe) by the first-principles method based on density functional theory. The crystal parameters and electronic structures are calculated for three different oxides. The results show that the magnitude of lattice distortion is the strongest in LaMnO3, and the slightest in LaCrO3 among three compounds. The magnetic ground states of LaCrO3 and LaFeO3 are G-type antiferromagnet. However, for LaMnO3, GGA+U fails to predict the experimental ground state, and only the internal coordinates are relaxed and the experimental lattice constants are fixed, the LDA+U can reproduce the experimental A-type antiferromagnetic state. It is found that Fe-3d electrons in LaFeO3 occupy the localized orbital with the low energy, while Cr-3d and Mn-3d electrons in LaCrO3 and LaMnO3 occupy the relatively wide energy states due to the strong hybridization between d electrons and p electrons of oxygen atoms.

Spin-polarized current injection induced magnetic reconstruction at oxide interface

Electrical manipulation of magnetism presents a promising way towards using the spin degree of freedom in very fast, low-power electronic devices. Though there has been tremendous progress in electrical control of magnetic properties using ferromagnetic (FM) nanostructures, an opportunity of manipulating antiferromagnetic (AFM) states should offer another route for creating a broad range of new enabling technologies. Here we selectively probe the interface magnetization of SrTiO3/La0.5Ca0.5MnO3/La0.7Sr0.3MnO3 heterojunctions and discover a new spin-polarized current injection induced interface magnetoelectric (ME) effect. The accumulation of majority spins at the interface causes a sudden, reversible transition of the spin alignment of interfacial Mn ions from AFM to FM exchange-coupled, while the injection of minority electron spins alters the interface magnetization from C-type to A-type AFM state. In contrast, the bulk magnetization remains unchanged. We attribute the current-induced interface ME effect to modulations of the strong double-exchange interaction between conducting electron spins and local magnetic moments. The effect is robust and may serve as a viable route for electronic and spintronic applications.

Crystallographic Features of Electronic States in the Highly-Correlated Electronic System Sr<sub>1-</sub><i><sub>x</sub></i>Sm<i><sub>x</sub></i>MnO<sub>3</sub> around <i>x</i> = 0.50

The highly-correlated electron system Sr1-xSmxMnO3 (SSMO) with the simple-perovskite structure has been found to exhibit fascinating electronic states accompanying antiferromagnetic and ferromagnetic orderings. It was, in particular, reported that the electronic state for 0.46 ≤ x ≤ 0.54 was characterized by the coexistence state consisting of the A-type antiferromagnetic and ferromagnetic states. However, the features of the coexistence state in this Sm-content range have not been understood yet. We have thus investigated the crystallographic features of prepared SSMO samples with 0.46 ≤ x ≤ 0.55, mainly by transmission electron microscopy. As a result, all prepared SSMO samples were first confirmed to have the orthorhombic-Pnma structure at 300 K. When the temperature was lowered from 300 K, in the case of x=0.47, the disordered-Pnma state was found to be transformed into an orbital-modulated (OM) state accompanying an incommensurate modulation. The notable feature of the OM state is that the state becomes unstable with increasing Sm contents at 100 K. In other words, the OM state was never changed into the CE-type state with the orbital and charge modulations. In addition, no orbital-ordered state for the A-type antiferromagnetic ordering was also found for 0.46 ≤ x ≤ 0.55.

Highly anisotropic exchange interactions ofjeff=12iridium moments on the fcc lattice inLa2BIrO6 (B=Mg,Zn)

We have performed inelastic neutron scattering (INS) experiments to investigate the magnetic excitations in the weakly distorted face-centered-cubic (fcc) iridate double perovskites La$_2$ZnIrO$_6$ and La$_2$MgIrO$_6$, which are characterized by A-type antiferromagnetic ground states. The powder inelastic neutron scattering data on these geometrically frustrated $j_{\rm eff}=1/2$ Mott insulators provide clear evidence for gapped spin wave excitations with very weak dispersion. The INS results and thermodynamic data on these materials can be reproduced by conventional Heisenberg-Ising models with significant uniaxial Ising anisotropy and sizeable second-neighbor ferromagnetic interactions. Such a uniaxial Ising exchange interaction is symmetry-forbidden on the ideal fcc lattice, so that it can only arise from the weak crystal distortions away from the ideal fcc limit. This may suggest that even weak distortions in $j_{\rm eff}=1/2$ Mott insulators might lead to strong exchange anisotropies. More tantalizingly, however, we find an alternative viable explanation of the INS results in terms of spin models with a dominant Kitaev interaction. In contrast to the uniaxial Ising exchange, the highly-directional Kitaev interaction is a type of exchange anisotropy which is symmetry-allowed even on the ideal fcc lattice. The Kitaev model has a magnon gap induced by quantum order-by-disorder, while weak anisotropies of the Kitaev couplings generated by the symmetry-lowering due to lattice distortions, can pin the order and enhance the magnon gap. Our findings highlight how even conventional magnetic orders in heavy transition metal oxides may be driven by highly-directional exchange interactions rooted in strong spin-orbit coupling.