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At least 235 records · Page 13

Interface-induced superconductivity in magnetic topological insulators

The interface between two different materials can show unexpected quantum phenomena. Here, in this study, we used molecular beam epitaxy to synthesize heterostructures formed by stacking together two magnetic materials, a ferromagnetic topological insulator (TI) and an antiferromagnetic iron chalcogenide (FeTe). We observed emergent interface-induced superconductivity in these heterostructures and demonstrated the co-occurrence of superconductivity, ferromagnetism, and topological band structure in the magnetic TI layer—the three essential ingredients of chiral topological superconductivity (TSC). The unusual coexistence of ferromagnetism and superconductivity is accompanied by a high upper critical magnetic field that exceeds the Pauli paramagnetic limit for conventional superconductors at low temperatures. These magnetic TI/FeTe heterostructures with robust superconductivity and atomically sharp interfaces provide an ideal wafer-scale platform for the exploration of chiral TSC and Majorana physics.

36 MATERIALS SCIENCE↗

Magnetoelastic-coupling-assisted first-order antiferromagnetic transitions in the corrugated honeycomb-lattice compounds (Ca, Sr) ⁢Mn 2 ⁢ P 2

Understanding the origin of unconventional magnetic order is a central theme in the research field of functional quantum materials for spin-dependent applications. In general, a paramagnetic (PM) to antiferromagnetic (AFM) transition is of thermodynamically second order in nature in the absence of a magnetic field. In the magnetically frustrated corrugated-honeycomb lattice compounds (Ca, Sr) ⁢Mn 2 ⁢ P 2 , electrical resistivity 𝜌 measurements in the 𝑎⁢𝑏 plane are reported to exhibit sharp discontinuities at the respective PM to AFM ordering temperatures 𝑇 N = 69.5 and 53 K, respectively, signifying the unusual first-order nature of the AFM transition. To reveal the origin of such anomalous transitions, high-resolution linear thermal-expansion measurements are reported for both CaMn 2 ⁢P 2 and SrMn 2 ⁢ P 2 in the 𝑎⁢𝑏 plane and along the 𝑐 axis using capacitance dilatometry. The thermal expansion measurements show a sharp discontinuity in Δ⁢𝐿/𝐿 at 𝑇 N , yielding a diverging behavior in the thermal expansion coefficient 𝛼⁡(𝑇) associated with strong magnetoelastic coupling, driving the first-order AFM transition in CaMn 2 ⁢P 2 . However, this effect is weaker in SrMn 2 ⁢P 2 , consistent with the magnetic entropy changes 𝑆⁡(𝑇) obtained from the heat-capacity measurements. Temperature-dependent 𝑎⁢𝑏-plane x-ray diffraction measurements for CaMn 2 ⁢ P 2 near its 𝑇 N yield a volume thermal expansion coefficient consistent with literature data for other materials. The uniaxial pressure derivatives of 𝑇 N in the two compounds are found to be respectively opposite in sign, presumably due to the different magnetic structures.

Pakhira, Santanu [Maulana Azad National Institute ↗

Antiferromagnetic excitonic insulator state in Sr3Ir2O7

Abstract Excitonic insulators are usually considered to form via the condensation of a soft charge mode of bound electron-hole pairs. This, however, presumes that the soft exciton is of spin-singlet character. Early theoretical considerations have also predicted a very distinct scenario, in which the condensation of magnetic excitons results in an antiferromagnetic excitonic insulator state. Here we report resonant inelastic x-ray scattering (RIXS) measurements of Sr 3 Ir 2 O 7 . By isolating the longitudinal component of the spectra, we identify a magnetic mode that is well-defined at the magnetic and structural Brillouin zone centers, but which merges with the electronic continuum in between these high symmetry points and which decays upon heating concurrent with a decrease in the material’s resistivity. We show that a bilayer Hubbard model, in which electron-hole pairs are bound by exchange interactions, consistently explains all the electronic and magnetic properties of Sr 3 Ir 2 O 7 indicating that this material is a realization of the long-predicted antiferromagnetic excitonic insulator phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Magnetic order in the S eff =1/2 triangular-lattice compound NdCd 3 ⁢P 3

Here, we present and characterize a new member of the R⁢Cd 3 ⁢P 3 (R=rare earth) family of materials, NdCd 3 ⁢P 3 , which possesses Nd 3+ cations arranged on well-separated triangular lattice layers. Magnetic susceptibility and heat capacity measurements demonstrate a likely S eff =1/2 ground state, and also reveal the formation of long-range antiferromagnetic order at T N =0.34K. Via measurements of magnetization, heat capacity, and electrical resistivity, we characterize the electronic properties of NdCd 3 ⁢P 3 and compare results to density functional theory calculations.

36 MATERIALS SCIENCE↗

Record thermopower found in an IrMn-based spintronic stack

The Seebeck effect converts thermal gradients into electricity. As an approach to power technologies in the current Internet-of-Things era, on-chip energy harvesting is highly attractive, and to be effective, demands thin film materials with large Seebeck coefficients. In spintronics, the antiferromagnetic metal IrMn has been used as the pinning layer in magnetic tunnel junctions that form building blocks for magnetic random access memories and magnetic sensors. Spin pumping experiments revealed that IrMn Néel temperature is thickness-dependent and approaches room temperature when the layer is thin. Here, we report that the Seebeck coefficient is maximum at the Néel temperature of IrMn of 0.6 to 4.0 nm in thickness in IrMn-based half magnetic tunnel junctions. We obtain a record Seebeck coefficient 390 (±10) μV K -1 at room temperature. Our results demonstrate that IrMn-based magnetic devices could harvest the heat dissipation for magnetic sensors, thus contributing to the Power-of-Things paradigm.

42 ENGINEERING↗

In situ synchrotron x-ray studies of epitaxial SrCoO x films during ionic liquid gating

The manipulation of ions in complex oxide materials can be used to mimic brain-like plasticity through changes to the resistivity of a neuromorphic device. Advances in the design of more energy efficient devices require improved understanding of how ions migrate within a material and across its interface. We investigate the exchange of oxygen and hydrogen in a model SrCoO x epitaxial film—a material that transitions between a ferromagnetic metal and antiferromagnetic insulator depending on the oxygen concentration. Changes to the film during ionic liquid gating were measured by in situ synchrotron x-ray techniques as a function of time and gate voltage, examining the reversibility of the oxide over one complete gating cycle. We find that the out-of-plane lattice constant and oxygen vacancy concentration of SrCoO x are largely reversible although changes were observed in the ordered vacancy structure. Our results provide much needed insight into electrolyte-gated phase behavior in the transition metal oxides.

Li, Yan [Argonne National Laboratory (ANL), Argonn↗

Anisotropic magnetism and Kondo-lattice behavior in the frustrated antiferromagnet Ce 3 ⁢MgBi 5

Here, we report the synthesis and physical characterization of single-crystalline Ce 3 ⁢MgBi 5 , a previously unexplored member of the Ce 3 ⁢𝑀⁢𝑃⁢𝑛 5 family. This compound crystallizes in the hexagonal 𝑃⁢6 3 /𝑚⁢𝑐⁢𝑚 structure, featuring an anisotropic Ce sublattice composed of zigzag chains along the 𝑐 axis and a distorted kagome-like network in the basal plane. Magnetization measurements reveal antiferromagnetic order below 𝑇 𝑁 ≈ 4.2K with strong magnetic anisotropy and multiple field-induced metamagnetic transitions for fields applied perpendicular to [001], leading to a dome-shaped 𝐻–𝑇 phase diagram. Electrical transport exhibits characteristic signatures of a Ce-based Kondo lattice, including broad resistivity maxima and pronounced field-dependent anomalies in the magnetoresistance and Hall response that track the magnetic phase boundaries. Specific-heat measurements confirm the magnetic transition and show that the full R ⁢ln⁡ 2 entropy expected for a Ce 3+ Kramers doublet is recovered by 20 K, indicating an extended temperature range of magnetic fluctuations consistent with Kondo correlations. Our results establish Ce 3 ⁢MgBi 5 as a platform within the Ce 3 ⁢𝑀⁢𝑃⁢𝑛 5 family for exploring the interplay of geometric frustration, magnetic anisotropy, and Kondo-lattice physics under applied magnetic fields.

Kondo effect↗

Epitaxial 2D Magnet and Topological Insulator Heterostructures

I will discuss our latest advances on the epitaxial growth of 2D van der Waals (vdW) magnets and their integration with topological insulators (TI). This work is motivated by the realization of topological phases such as the quantum anomalous Hall effect and highly efficient spin-orbit torque produced by TIs. Our initial studies of MnSe2 growth on Bi2Se3 showed a tendency for the interdiffusion of Mn into the Bi2Se3. This ultimately led to the synthesis of MnBi2Se4 (MBS), a new magnetic TI. Interestingly, the vdW phase is not the thermodynamically stable phase and bulk crystals do not exist, so the epitaxial stabilization of MBS creates the opportunity to explore the magnetic and topological properties of this material. We find that MBS is a layered antiferromagnet, similar to MnBi2Te4, but a difference is that the magnetic moments lie in the plane of the film. Angle resolved photoemission experiments show the presence of a topological surface state with Dirac dispersion. For bilayers of 2D magnets and TIs, we have developed FGT films on Bi2Te3. We first optimized FGT by studying its growth on Ge(111) substrates, where we find that kinetic considerations play a major role. Using cross-sectional scanning transmission electron microscopy and scanning tunneling microscopy, we optimize the FGT films to have atomically smooth surfaces and abrupt interfaces with the Ge(111). Subsequently, we have developed the growth of FGT on Bi2Te3 for the integration of 2D magnets with Tis. Interestingly, we observe room temperature ferromagnetism in FGT/Bi2Te3 heterostructures by varying the growth conditions.

Kawakami, Roland↗

Theory of optical axion electrodynamics and application to the Kerr effect in topological antiferromagnets

Abstract Emergent axion electrodynamics in magneto-electric media is expected to provide novel ways to detect and control material properties with electromagnetic fields. However, despite being studied intensively for over a decade, its theoretical understanding remains mostly confined to the static limit. Here, we introduce a theory of axion electrodynamics at general frequencies. We define a proper optical axion magneto-electric coupling through its relation to optical surface Hall conductivity and provide ways to calculate it in lattice systems. By employing our formulas, we show that axion electrodynamics can lead to a significant Kerr effect in thin-film antiferromagnets at wavelengths that are seemingly too long to resolve the spatial modulation of magnetism. We identify the wavelength scale above which the Kerr effect is suppressed. Our theory is particularly relevant to materials like MnBi 2 Te 4 , a topological antiferromagnet whose magneto-electric response is shown here to be dominated by the axion contribution even at optical frequencies.

36 MATERIALS SCIENCE↗

Field-tunable BKT and quantum phase transitions in spin-$\frac{1}{2}$ triangular lattice antiferromagnet

Quantum magnetism is one of the most active fields for exploring exotic phases and phase transitions. The recently synthesized Na 2 BaCo(PO 4 ) 2 (NBCP) is an ideal material incarnation of the spin-$\frac{1}{2}$ easy-axis triangular lattice antiferromagnet (TLAF). Experimental evidence shows that NBCP hosts the spin supersolid state with a giant magnetocaloric effect. Theory further predicts that magnetic fields can drive NBCP through Berezinskii-Kosterlitz-Thouless (BKT) and other richer quantum phase transitions. However, detecting these transitions is challenging, as they onset at ultralow temperatures near 60 mK and require high magnetization sensitivity. Using a newly developed gradient force magnetometer in a dilution refrigerator, we mapped the magnetic susceptibility phase diagram down to 30 mK. Our results provide a more comprehensive and accurate understanding of BKT melting of spin supersolidity and several field-tunable quantum phase transitions, which establish NBCP as a model platform for frustrated magnetism and highlight potential applications of its giant magnetocaloric effects.

BKT transition↗

Static magnetic order with strong quantum fluctuations in spin-1/2 honeycomb magnet Na 2 Co 2 TeO 6

Kitaev interactions, arising from the interplay of frustration and bond anisotropy, can lead to strong quantum fluctuations and, in an ideal case, to a quantum-spin-liquid state. However, in many nonideal materials, spurious non-Kitaev interactions typically promote a zigzag antiferromagnetic order in the d-orbital transition-metal compounds. Here, by combining neutron scattering with muon-spin rotation and relaxation techniques, we provide mechanism insights into the exotic properties of Na 2 Co 2 TeO 6 , a candidate material of the Kitaev model. Below T N , the zero-field muon-spin relaxation rate becomes almost constant (~0.45 μs –1 ). We attribute this temperature-independent relaxation rate to the strong quantum fluctuations, as well as to the frustrated Kitaev interactions. As the magnetic field increases, neutron scattering data indicate a broader spin-wave excitation at the K-point. Therefore, quantum fluctuations seem not only robust but are even enhanced by the applied magnetic field. Our findings provide valuable hints for understanding the onset of the quantum-spin-liquid state in Kitaev materials.

36 MATERIALS SCIENCE↗

In-situ fabrication and transport properties of (111) Y 2 Ir 2 O 7 epitaxial thin film

We report on the successful fabrication of (111) oriented thin films of pyrochlore iridate Y 2 Ir 2 O 7 by means of solid phase epitaxy. Essentially, we developed an entirely in situ annealing protocol, which is superior to the conventional ex-situ routine that requires multi-hour annealing to stabilize the proper pyrochlore structure. The morphological quality of the films has been confirmed by x-ray diffraction, reflectivity, and reciprocal space mapping, demonstrating their high crystallinity with a pure pyrochlore phase and an expected epitaxial relation to the substrate. Strikingly, below the magnetic phase transition, the temperature dependence of resistivity shows a power-law behavior with the power exponent of similar to 3/2, characteristic of a Weyl semimetal in the presence of impurities and electron-electron correlations. Finally, below 10K, the magneto-transport measurements reveal the emergence of a non-saturated negative magnetoresistance up to 9T with a small "valley" around zero field. These findings are further interpreted in relation to the weak anti-localization effect and the non-collinear antiferromagnetic ordering on the Ir sublattice.

36 MATERIALS SCIENCE↗

Elucidating the Role of Dimensionality on the Electronic Structure of the Van der Waals Antiferromagnet NiPS 3

Abstract The sustained interest in investigating magnetism in the 2D limit of insulating antiferromagnets is driven by the possibilities of discovering, or engineering, novel magnetic phases through layer stacking. However, due to the difficulty of directly measuring magnetic interactions in 2D antiferromagnets, it is not yet understood how intra layer magnetic interactions in insulating , strongly correlated, materials can be modified through layer proximity. Herein, the impact of reduced dimensionality in the model van der Waals antiferromagnet NiPS 3 is explored by measuring electronic excitations in exfoliated samples using Resonant Inelastic X‐ray Scattering (RIXS). The resulting spectra shows systematic broadening of NiS 6 multiplet excitations with decreasing layer count from bulk down to three atomic layers (3L). It is shown that these trends originate from a decrease in transition metal‐ligand and ligand–ligand hopping integrals, and by charge‐transfer energy evolving from Δ = 0.83 eV in the bulk to 0.37 eV in 3L NiPS 3 . Relevant intralayer magnetic exchange integrals computed from the electronic parameters exhibit a decrease in the average interaction strength with thickness. This study underscores the influence of inter layer electronic interactions on intra layer ones in insulating magnets, indicating that magnetic Hamiltonians in few‐layer insulating magnets can greatly deviate from their bulk counterparts.

36 MATERIALS SCIENCE↗

Quantum phases in the honeycomb-lattice J 1 – J 3 ferro-antiferromagnetic model

The significant role of quantum effects in magnets with competing interactions remains at the forefront of condensed matter physics for over 50 years, inspiring a multitude of quests for exotic states, models that can realize them, and real materials that can host them. The elusive spin-liquid states with strong entanglement are but one example; others include valence-bond phases with spatial symmetry breaking, quantum spin nematics that are quantum analogues of liquid crystals, and an especially extensive class of unconventional magnetically ordered phases that do not appear in the classical solutions of the underlying spin models. It is the latter group of phenomena that creates a broader context for the research effort in the present work concerning the search for and an identification of the novel ground states of quantum magnets. In this work, we have studied one of the paradigmatic models in quantum magnetism that is also attracting a significant recent interest because it appears to be providing a tantalizingly close description for many of the newly synthesized materials. We demonstrated that the phase diagram of the quantum ferro-antiferromagnetic model on the honeycomb lattice differs dramatically from the classical one. It hosts the double-zigzag and Ising-z phases as unexpected intermediaries between ferromagnetic and zigzag states that are also extended beyond their classical regions of stability. In broad agreement with quantum order-by-disorder arguments, these collinear phases completely supersede the classical spiral state.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Quantum Spin Torque Driven Transmutation of an Antiferromagnetic Mott Insulator

The basic model of spin-transfer torque (STT) in antiferromagnetic spintronics considers the exchange of angular momentum between quantum spins of flowing electrons and noncollinear-to-them localized spins treated as classical vectors. These vectors are assumed to realize Néel order in equilibrium, ↑ ↓ ∙∙∙ ↑ ↓, and their STT-driven dynamics is described by the Landau-Lifshitz-Gilbert (LLG) equation. However, many experimentally employed materials (such as archetypal NiO) are strongly electron-correlated antiferromagnetic Mott insulators (AFMIs) whose localized spins form a ground state quite different from the unentangled Néel state | ↑ ↓ ∙∙∙ ↑ ↓$\rangle$. The true ground state is entangled by quantum spin fluctuations, leading to the expectation value of all localized spins being zero, so that LLG dynamics of classical vectors of fixed length rotating due to STT cannot even be initiated. Instead, a fully quantum treatment of both conduction electrons and localized spins is necessary to capture the exchange of spin angular momentum between them, denoted as quantum STT. We use a recently developed time-dependent density matrix renormalization group approach to quantum STT to predict how injection of a spin-polarized current pulse into a normal metal layer coupled to an AFMI overlayer via exchange interaction and possibly small interlayer hopping—mimicking, e.g., topological-insulator/NiO bilayer employed experimentally—will induce a nonzero expectation value of AFMI localized spins. This new nonequilibrium phase is a spatially inhomogeneous ferromagnet with a zigzag profile of localized spins. The total spin absorbed by AFMI increases with electron-electron repulsion in AFMIs, as well as when the two layers do not exchange any charge.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Magnetic dilution effect and topological phase transitions in (Mn 1- x Pb x )Bi 2 Te 4

We report, as the first intrinsic antiferromagnetic topological insulator, MnBi 2 Te 4 has provided a material platform to realize various emergent phenomena arising from the interplay of magnetism and band topology. Here, by investigating (Mn 1-x Pb x )Bi 2 Te 4 (0 ≤ x ≤ 0.82) single crystals via the x-ray, electrical transport, magnetometry and neutron measurements, chemical analysis, external pressure, and first-principles calculations, we reveal the magnetic dilution effect on the magnetism and band topology in MnBi 2 Te 4 . With increasing x, both lattice parameters a and c expand linearly by around 2%. All samples undergo the paramagnetic to A-type antiferromagnetic transition with the Néel temperature decreasing lineally from 24 K at x = 0 to 2 K at x = 0.82. Our neutron data refinement of the x = 0.37 sample indicates that the ordered moment is 4.3(1)μ B /Mn at 4.85 K and the amount of the Mn Bi antisites is negligible within the error bars. Isothermal magnetization data reveal a slight decrease of the interlayer plane-plane antiferromagnetic exchange interaction and a monotonic decrease of the magnetic anisotropy due to diluting magnetic ions and enlarging the unit cell. For x = 0.37, the application of external pressures enhances the interlayer antiferromagnetic coupling, boosting the Néel temperature at a rate of 1.4 K/GPa and the saturation field at a rate of 1.8 T/GPa. Furthermore, our first-principles calculations reveal that the band inversion in the two end materials, MnBi 2 Te 4 and PbBi 2 Te 4 , occurs at the Γ and Z point, respectively, while two gapless points appear at x = 0.44 and x = 0.66, suggesting possible topological phase transitions with doping.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Long-range magnetic order induced surface state in GdBi and DyBi

The recent discovery of unconventional surface-state pairs, which give rise to Fermi arcs and spin textures, in antiferromagnetically ordered rare-earth monopnictides attracted the interest in these materials. Here, we use angle-resolved photoemission spectroscopy measurements in conjunction with density functional theory calculations to investigate the evolution of the electronic structure of GdBi and DyBi. We find that new surface states, including a Dirac cone, emerge in the antiferromagnetic (AFM) state. However, they are located along a direction in momentum space that is different than what was found in NdSb, NdBi, and CeBi. The observed changes in the electronic structure are consistent with the presence of AFM-II-A type order.

36 MATERIALS SCIENCE↗