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At least 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Controllable Emergent Spatial Spin Modulation in Sr 2 IrO 4 by In Situ Shear Strain

Symmetric anisotropic interaction can be ferromagnetic and antiferromagnetic at the same time but for different crystallographic axes. We show that the competition of anisotropic interactions of orthogonal irreducible representations can be a general route to obtain new exotic magnetic states. We demonstrate it here by observing the emergence of a continuously tunable 12-layer spatial spin modulation when distorting the square-lattice planes in the quasi-two-dimensional antiferromagnetic Sr 2 IrO 4 under in situ shear strain. Furthermore, this translation-symmetry-breaking phase is a result of an unusual strain-activated anisotropic interaction which is at the fourth order and competing with the inherent quadratic anisotropic interaction. Such a mechanism of competing anisotropy is distinct from that among the ferromagnetic, antiferromagnetic, and/or the Dzyaloshinskii-Moriya interactions, and it could be widely applicable and highly controllable in low-dimensional magnets.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Canted antiferromagnetic order in the monoaxial chiral magnets V 1/3 TaS 2 and V 1/3 NbS 2

The Dzyaloshinskii-Moriya (DM) interaction is present in the transition metal dichalcogenides (TMDC) magnets of form M 1 / 3 T S 2 ( M = 3 d transition metal, T ϵ { Nb , Ta } ), given that the intercalants M form 3 × 3 superlattices within the structure of the parent materials T S 2 and break the centrosymmetry. Competition between DM and ferromagnetic exchange interactions has been shown to stabilize a topological defect known as a chiral soliton in select intercalated TMDCs, initiating interest both in terms of fundamental physics and the potential for technological applications. In the current article we report on our study of the materials V 1 / 3 TaS 2 and V 1 / 3 NbS 2 , using a combination of x-ray powder diffraction, magnetization, and single crystal neutron diffraction. Historically identified as ferromagnets, our diffraction results instead reveal that vanadium spins in these compounds are arranged into an A-type antiferromagnetic configuration at low temperatures. Refined moments are 1.37(6) and 1.50(9) μ B for V 1 / 3 TaS 2 and V 1 / 3 NbS 2 , respectively. Transition temperatures T c = 32 K for V 1 / 3 TaS 2 and 50 K for V 1 / 3 NbS 2 are obtained from the magnetization and neutron diffraction results. We attribute the small net magnetization observed in the low-temperature phases to a subtle ( ~ 2 ° ) canting of XY spins in the out-of-plane direction. These new results are indicative of dominant antiferromagnetic exchange interactions between the vanadium moments in adjacent a b planes, likely eliminating the possibility of identifying stable chiral solitons in the current materials.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Frustrated magnetism in the layered triangular lattice materials K 2 Co(SeO 3 ) 2 and Rb 2 Co(SeO 3 ) 2

A study of the layered triangular lattice materials K 2 Co(SeO 3 ) 2 and Rb 2 Co(SeO 3 ) 2 is reported here. These isostructural compounds crystallize in the trigonal space group R-3m (No. 166). The magnetic Co 2+ ions form a spin-1/2 triangular lattice and display strongly frustrated magnetism. We find no evidence in the susceptibility or heat capacity for in-plane ordering of the spins; rather the in-plane inverse susceptibility is typical of that seen for frustrated magnets. At around 10 K, a ferromagnetic component appears in the magnetic susceptibility perpendicular to the triangular planes. The heat capacity at low applied fields does not show sharp features, but in larger applied fields a sharp ferromagneticlike transition appears. Field- and direction-dependent magnetization measurements at 2 K indicate that both materials have a magnetic easy axis perpendicular to the triangular planes. The magnetic properties are sensitive to the field applied perpendicular to the triangular planes, which induces a metamagnetization transition at 0.75 T. Spin polarization develops along with the increasing out-of-plane field, resulting in a saturated ferromagnetic state at high fields. In contrast, the magnetic properties are resistant to the in-plane field. Our results suggest that these materials are embodiments of Ising spins on triangular lattices with easy-axis anisotropy.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Interlayer magnetism in Fe 3-x GeTe 2

Fe 3 - x GeTe 2 is a layered van der Waals magnetic material with a relatively high ordering temperature and large anisotropy. While most studies have concluded the interlayer ordering to be ferromagnetic, there have also been reports of interlayer antiferromagnetism in Fe 3 - x GeTe 2 . In this work, we investigate the interlayer magnetic ordering by neutron diffraction experiments, scanning tunneling microscopy (STM) and spin-polarized STM measurements, density functional theory plus U calculations, and STM simulations. We conclude that the layers of Fe 3 - x GeTe 2 are coupled ferromagnetically and that in order to capture the magnetic and electronic properties of Fe 3 - x GeTe 2 within density functional theory, Hubbard U corrections need to be taken into account.

2-dimensional systems↗
DOE OSTI2020

Crystal structure and physical properties of Yb 2 In and Eu 2–x Yb x In alloys

While binary R E 2 In , where R E = rare earth , have been reported a few decades ago, recent investigations revealed intriguing new physical insights. For instance, the discovery of a nearly ideal first-order ferromagnetic transition in Eu 2 In calls for further exploration of structures and properties of R E 2 In , in particular for the least-documented R E = Eu and Yb cases. In this work, we investigate Eu 2 – x Yb x In pseudobinaries with nominal values of x = 0.25 , 0.5, 0.75, 1, 1.5, 2 by powder x-ray diffraction (including as function of temperature from 100 to 375 K for Yb 2 In ), magnetization (5–300 K), as well as electrical resistivity (5–300 K) and calorimetric (2–150 K) measurements for Yb 2 In . Compared to other RE , Yb or Eu always raise challenging questions linked to their valence states. From average atomic volume, Yb is anticipated to be divalent in Yb 2 In , at least between 100 and 375 K, which is in line with the absence of 4 f magnetism. In agreement with x-ray diffraction and magnetization data, the resistivity of Yb 2 In is rather featureless and typical of a metal. Establishing Yb 2 In as a nonmagnetic isostructural reference for Eu 2 In allows one to use its heat capacity to revisit that of the latter, and get experimental insights into the exceptional magnetocaloric effect of the compound with Eu. In particular, we show that a third of the total magnetic entropy ( S m ≈ 35.6 J mo l – 1 K – 1 at T = 100 K ) is concentrated in a 3 K temperature window around the T C of Eu 2 In . Starting from the ferromagnetic compound Eu 2 In [ T C = 55.2 ( 5 ) K ] , we show that Yb substitutions in Eu 2 – x Yb x In lead to a decrease in both the Curie temperature [ T C = 41 ( 2 ) and 32(2) K for x = 0.25 and 0.5] and magnetic saturation, while weakening the first-order character of the transition as x increases. A significant isothermal entropy change of 5.1 ( 4 ) J mo l – 1 K – 1 for Δ B = 2 T is found at 44 K in Eu 1.75 Yb 0.25 In , demonstrating that the giant magnetocaloric effect of Eu 2 In can be tuned to lower temperatures by Yb substitutions.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Influence of dislocations and twin walls in BaTiO 3 on the voltage-controlled switching of perpendicular magnetization

In this work, we investigate the influence of dislocations and twin walls in BaTiO 3 on its ferroelectric response and the resulting effect on the perpendicular magnetic anisotropy (PMA) of a strain-coupled [Co\Ni] n film. A dense twinned structure in conjunction with a high dislocation density significantly reduces the converse piezoelectric effect of BaTiO 3 by hindering the propagation of newly nucleated domains with an applied electric field. This, in turn, results in a modest reduction of the PMA of the ferromagnetic layer. On the other hand, the ferroelectric polarization reorients from [100] to [001] direction in a dislocation-free BaTiO 3 , inducing the maximum achievable in-plane compressive strain of 1.1%. A large fraction of this uniaxial strain is transferred to the magnetoelastically coupled ferromagnetic layers whose magnetization switches to in plane via the inverse magnetostriction effect. This work reveals the critical role of the interplay between twin walls and dislocations within a ferroelectric substrate in the performance of multiferroic heterostructures and provides insight into the development of highly energy-efficient magnetoelectric devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Conduction via surface states in antiferromagnetic Mott-insulating Ni S 2 single crystals

Pyrite structure transition-metal disulfides exhibit diverse ground states vs d-band filling, spanning diamagnetic semiconducting, ferromagnetic metallic, antiferromagnetic Mott insulating, and superconducting in FeS 2 , CoS 2 , NiS 2 , and CuS 2 . NiS is particularly interesting and poorly understood as its Mott insulating behavior is accompanied by complex antiferromagnetic ordering below ~38 K and perplexing weak ferromagnetism below ~30 K. Temperature-, pressure-, and composition-dependent insulator-metal transitions also occur, particularly in bandwidth-controlled NiS 2–x Se x , hole-doped Ni 1–x Co x S 2 , etc. Here, we use high-quality chemical-vapor-transport-grown NiS 2 single crystals characterized by x-ray diffraction, energy-dispersive x-ray spectroscopy, magnetometry, and extensive transport and magnetotransport measurements, to generate new insight into this system. In particular, resistivity, magnetoresistance, and Hall effect analyses vs temperature, thickness, and surface preparation, provide unequivocal evidence of surface conduction, where the more conductive surface shunts essentially all current at low temperatures. The surface transport changes from two dimensional and insulating to three dimensional and metallic as the surface preparation is varied (also displaying intriguing sensitivity to magnetic ordering), significantly clarifying literature ambiguities with respect to the electronic ground state. These results have immediate implications. First, the temperature-, pressure-, and composition-dependent insulator-metal transitions deduced in the extensive prior work on NiS 2-x Se x , Ni 1–x Co x S 2 , etc., must clearly be reexamined in light of rife metallic surface conduction, not previously taken into account. Second, NiS 2 now joins FeS 2 and CoS 2 as systems in which bulk and surface electronic behaviors are strikingly different, suggesting that metallic surface states could be a universal feature of pyrite structure transition-metal disulfides.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Challenges to magnetic doping of thin films of the Dirac semimetal Cd 3 As 2

Magnetic doping of topological quantum materials provides an attractive route for studying the effects of time-reversal symmetry breaking. Thus motivated, we explore the introduction of the transition metal Mn into thin films of the Dirac semimetal Cd 3 A s2 during growth by molecular beam epitaxy. Scanning transmission electron microscopy measurements show the formation of a Mn-rich phase at the top surface of Mn-doped Cd 3 A s2 thin films grown using both uniform doping and delta doping. This suggests that Mn acts as a surfactant during epitaxial growth of Cd 3 A s2 , resulting in phase separation. Magnetometry measurements of such samples indicate a ferromagnetic phase with out-of-plane magnetic anisotropy. Electrical magneto-transport measurements of these films as a function of temperature, magnetic field, and chemical potential reveal a lower carrier density and higher electron mobility compared with pristine Cd 3 A s2 films grown under similar conditions. This suggests that the surfactant effect might also serve to remove impurities from the bulk of the film. Further, we observe robust quantum transport (Shubnikov-de Haas oscillations and an incipient integer quantum Hall effect) in very thin (7 nm) Cd 3 A s2 films despite being in direct contact with a structurally disordered surface ferromagnetic overlayer.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Magnetic order and spin liquid behavior in [Mo 3 ] 11+ molecular magnets

Molecular magnets based on [Mo 3 ] 11+ units with one unpaired electron per trimer have attracted recent interest due to the identification of quantum spin liquid candidacy in some family members. Here, we present comprehensive measurements on polycrystalline samples of ZnScMo 3 O 8 , MgScMo 3 O 8 , and Na 3 Sc 2 Mo 5 O 16 with the same Mo 3 O 13 magnetic building blocks. In this work, the crystal structures are characterized with x-ray or neutron powder diffraction and the magnetic ground states are determined by performing ac and dc susceptibility, specific heat, neutron powder diffraction, and muon spin relaxation measurements. Our work indicates that ZnScMo 3 O 8 and MgScMo 3 O 8 have ferromagnetic Curie-Weiss temperatures of 18.5 and 11.9 K, ordered ground states with net moments (low-moment ferromagnetism or canted antiferromagnetism), and zero field ordering temperatures of $T_c$ = 6 K and $T_c$ < 2 K, respectively. On the other hand, Na 3 Sc 2 Mo 5 O 16 hosts a dynamical magnetic ground state with no evidence for magnetic ordering or spin freezing down to 20 mK despite an antiferromagnetic Curie-Weiss temperature of –36.2 K, and therefore is a candidate for quantum spin liquid behavior. By comparing the present results to past work on the same family of materials, we construct a phase diagram which illustrates that the magnetic ground states of these Mo-based molecular magnets are very sensitive to small changes in the nearest-neighbor Mo-Mo distance.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Probing antiferromagnetic coupling in magnetic insulator/metal heterostructures

Using depth- and element-resolved characterization, we report insights into antiferromagnetic coupling in Y 3 ⁢Fe 5 ⁢O 12 /permalloy (YIG/Py) and Y 3 ⁢Fe 5 ⁢O 12 /Co (YIG/Co) thin-film heterostructures grown on Si/SiO 2 and Gd 3⁢ Ga 5⁢ O 12 substrates. We build on recent work demonstrating antiferromagnetic coupling in polycrystalline YIG/metallic-ferromagnetic systems by characterizing differences in the structural and magnetic properties which depend on the choice of ferromagnet (Py vs Co), seed layer (with and without Pt), and substrate (Si/SiO 2 vs Gd 3 ⁢Ga 5 ⁢O 12 ). These differences in the sample structure manifest as notable changes in interface coupling sign, magnetic reversal mechanisms, magnetic depth profiles, and domain structure. Through a combination of magnetometry, polarized neutron reflectometry, and x-ray photoemission electron microscopy, a comprehensive picture of the magnetic interactions is realized, with lateral- and depth resolution at submicrometer and nanometer scales, respectively. These results confirm that both Co and Py share a preference to align antiparallel to polycrystalline YIG grown on some substrates (Si/SiO 2 and Si/SiO 2 /Pt), while coupling ferromagnetically with highly oriented YIG on (111) Gd 3⁢ Ga 5 ⁢O 12 and (110) Gd 3 ⁢Ga 5⁢ O 12 /Pt substrates. The complex interplay among magnetic interactions at the YIG/ferromagnetic interface has important implications for spintronic and magnonic devices based on this platform.

Exchange interaction↗
DOE OSTI2022

Spin-lattice coupling in magnetocaloric Gd 5 ( Ge , Si ) 4 alloys by $in$ $situ$ x-ray pair distribution analysis in magnetic field

Here, using in situ x-ray pair distribution analysis in magnetic field, we study the strong spin-lattice coupling in archetypal magnetocaloric Gd 5 (Ge,Si) 4 alloys manifested by the presence of a first order paramagnetic (PM)-to-ferromagnetic (FM) phase transition that can be triggered by either decreasing temperature in zero magnetic field or increasing magnetic field at constant temperature. We find that the coupling arises from the tendency of Gd-(Si,Ge) slabs in the alloys to reversibly slide against each other to both pack closely and couple ferromagnetically. We also find that, locally, the packing of slabs in FM phases induced by decreasing temperature in zero field is different from that in FM phases of the same chemical composition induced by increasing magnetic field isothermally, indicating that temperature and magnetic field are coupled but not necessarily equivalent control variables for triggering phase transitions in strongly correlated systems.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Relationship between magnetoresistance behavior and magnetic states in intercalated compounds Fe x TiS 2

Here, temperature and field-dependent neutron powder diffraction (NPD) measurements have been performed to reveal the nature of the unusual evolution of the magnetoresistance behavior with increasing Fe content in the intercalated compounds Fe x TiS 2 (with x=0.25,0.33,0.50,0.55) synthesized by solid-phase reaction method with prolonged homogenization heat treatment. As derived from neutron diffraction measurements, both the Fe 0.25 TiS 2 and the Fe 0.50 TiS 2 compound exhibit an antiferromagnetic (AFM) order below their respective Néel temperatures T N ≈52 K and T N ≈140K, which results in the presence of a large magnetoresistance accompanying the field-induced phase transition from AFM to the ferromagnetic (FM) state. At low temperatures, this AFM-FM transition is irreversible, confirmed by the irreversibility of changes in the NPD patterns and the presence of remnant magnetoresistance. In contrast, Fe 0.33 TiS 2 shows short-range magnetic order at T f ≈44 K due to a triangular network of intercalated Fe atoms and frustrations of exchange interactions with a field-induced FM alignment of Fe magnetic moments in an applied magnetic field as revealed by NPD measurements. The field-induced transformations of the cluster glass magnetic state in this compound lead to a significant decrease in electrical resistivity. According to NPD data, a reduced impact of an external magnetic field on the electrical resistivity of the compound Fe 0.55 TiS 2 can be ascribed to the presence of ferromagnetic or ferrimagnetic order in compounds with the Fe concentrations above x=0.50. The results obtained indicate that the distribution of the Fe atoms, along with their concentration in Fe x TiS 2 layered compounds, plays a decisive role in the formation of the magnetic state and the behavior of the magnetoresistance.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Magnetism and T-x phase diagrams of Na- and Ag-substituted EuCd 2 As 2

EuCd 2 As 2 is an antiferromagnetic semimetal, that can host non-trivial topological properties, depending upon its magnetic state and excitations. Here, we report the synthesis and characterization of Eu(Cd 1-x Ag x ) 2 As 2 and Eu 1-y Na y Cd 2 As 2 , and study the evolution and nature of magnetic order with doping. Temperature-substitution phase diagrams are constructed from the electrical resistance and magnetic susceptibility data. We observe a splitting of the magnetic transition into two different transitions, and the gradual increase in one of the transition temperatures with Agand Na-substitution. The other transition remains more or less independent of doping. Further, we show that a magnetic state with a net ferromagnetic moment is stabilized by both Ag and Na doping and this can be explained by considering the changes in band filling due to substitution as suggested by density functional theory (DFT) calculations. We thus show that chemical substitution and the subsequent changes in band filling could be a pathway to tune the magnetic ground state and to stabilize a ferromagnetic phase in EuCd 2 As 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2023

Coupling of magnetism, crystal lattice, and transport in EuCuP and EuCuAs

EuCuP and EuCuAs are members of a family of materials with candidates for realizing magnetically tuned electronic topology. Here, in this work, the magnetic phase transitions and magnetoelastic coupling of EuCuP and EuCuAs have been investigated. Around the Curie temperature, the thermal expansion coefficient and specific-heat capacity of EuCuP are found to have two closely spaced features, at approximately 30 and 31.3 K, which may indicate a cascading magnetic transition or perhaps an electronic transition closely coupled to the magnetic ordering. The zero-field magnetoelastic coupling appears to be stronger in EuCuP than in EuCuAs, and field-dependent measurements suggest this is due to the dominant ferromagnetic interaction in EuCuP as opposed to antiferromagnetic order in EuCuAs below T N =13.5 K. Thermal expansion is anisotropic around T N in EuCuAs, with a maximum expansion along [001] occurring above T N prior to a stiffening of this c -axis component on cooling through T N ; the expansion of the basal plane has a lambda-like peak centered slightly above T N . Matching these behaviors, the ac susceptibility data for EuCuAs suggest the presence of strong ferromagnetic correlations above T N in the vicinity where the c-axis expansion peaks. Both compounds possess similar electrical and thermoelectric transport behaviors, with short-range magnetic order likely playing an important role above T C or T N . Transport properties suggest these are predominantly hole doped due to intrinsic defects, and narrow-gap semiconducting or semimetallic behavior may be achievable if the underlying defects can be tuned.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Superconducting phase diagram in Bi x Ni 1 – x thin films: The effects of Bi stoichiometry on superconductivity

The Bi-Ni binary system has been of interest due to possible unconventional superconductivity aroused therein, such as time-reversal symmetry breaking in Bi/Ni bilayers or the coexistence of superconductivity and ferromagnetism in Bi 3 ⁢Ni crystals. While Ni acts as a ferromagnetic element in such systems, the role of the strong spin-orbit coupling element Bi in superconductivity has remained unexplored. In this work, we systematically studied the effects of Bi stoichiometry on the superconductivity of Bi x ⁢Ni 1–x thin films (x ≈ 0.5–0.9) fabricated via a composition-spread approach. Here, the superconducting phase map of Bi x ⁢Ni 1–x thin films exhibited a superconducting composition region attributable to the intermetallic Bi 3 ⁢Ni phase with different amounts of excess Bi, revealed by synchrotron x-ray diffraction analysis. Interestingly, the mixed-phase region with Bi 3 ⁢Ni and Bi showed unusual increases in the superconducting transition temperature and residual resistance ratio as more Bi impurities were included, with the maximum T c (=4.2K) observed at x ≈ 0.79. A correlation analysis of structural, electrical, and magneto-transport characteristics across the composition variation revealed that the unusual superconducting “dome” is due to two competing roles of Bi: impurity scattering and carrier doping. We found that the carrier doping effect is dominant in the mild doping regime (0.74 ≤ x ≤ 0.79), while impurity scattering becomes more pronounced at larger Bi stoichiometry.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Crystal growth and evolution of magnetism in the EuCuP-EuCuAs solid solution

The hexagonal EuMX (M = Cu, Ag, Au; X = P, As, Sb, Bi) compounds host interesting electronic and magnetic properties, with seemingly intertwined topology and transport properties. One key feature of such behavior is the nature of the ordered magnetic structure. In EuCuAs, a topological Hall effect is caused by a conical spin structure that emerges when a field is applied within the easy-plane (H ⊥ c) of the helical ground state that exists below the Neel temperature of T N = 14 K. On the other hand, EuCuP is an easy-axis ferromagnet with a Curie temperature T C near 31 K. Here, in this study, we investigate the evolution of the magnetic properties in EuCuAs 1-x P x single crystals with 0.16 ≤ x ≤ 0.75. Crystals grown by cooling slowly in a Sn flux possessed macroscale inhomogeneity of As/P, particularly for arsenic-rich crystals. However, growth in a Sn flux via an isothermal dwell at 600 °C produced crystals that were homogeneous within the resolution of the probes utilized to investigate these crystals. The unit cell volumes, Curie-Weiss temperatures, and magnetic transitions trend linearly with composition and the magnetic anisotropy is reduced in the alloys. The magnetization data of crystals with x = 0.16 and 0.24 indicate an easy-plane antiferromagnetic ground state while ferromagneticlike behavior is observed for crystals with x ≥ 0.41. The temperature-dependent magnetization data possess multiple transitions for compositions near EuCuAs 0.75 P 0.25 , revealing a competition of ground states in this arsenic-rich region of the phase diagram. Neutron diffraction data for EuCuP are also presented as a follow up to previous results that revealed a two-step transition at T C ; the observed data were consistent with ferromagnetic order at T = 5K.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Physical properties of intergrowth compound Eu 2 CuZn 2 P 3

Here, the physical properties of single-crystalline Eu 2 ⁢CuZn 2 ⁢P 3 were inspected via thermodynamic, transport, and neutron diffraction measurements. Eu 2 ⁢ CuZn 2⁢ P 3 is composed of EuCuP and EuZn 2 ⁢ P 2 motifs stacked in a one-to-one ratio. The magnetic response of Eu 2 ⁢ CuZn 2 ⁢ P 3 is similar to that of EuZn 2 ⁢ P 2 in its A-type antiferromagnetic (semiconducting) state. A Néel temperature of T N = 40.3K is obtained from the specific heat capacity. Single-crystal neutron diffraction reveals a (001) magnetic propagation vector, with primarily in-plane moments coupled along [001] in an up-up-down-down pattern. This spin structure retains the ferromagnetic EuCuP motifs and antiferromagnetic coupling across the EuZn 2 ⁢P 2 motifs. The electrical resistivity is characterized by metallic behavior above 100 K, an increase in ρ upon cooling below ≈ 75K, and a large negative magnetoresistance below T N . First principles calculations evidence a narrow band gap for antiferromagnetic ordering and semimetallic behavior for the ferromagnetic state. This is consistent with the observed effect of magnetic field on the electrical resistivity. Hall effect measurements reveal a field-induced, negative anomalous Hall effect that increases on cooling down to 2 K. Also, an unconventional contribution to the Hall effect dominates the low-field Hall signal, particularly near T N , and is similar in appearance to a topological Hall effect. However, further work is necessary to understand if any of the transport properties have topological origins or if magnetism-induced modifications to the Fermi surface induce these unusual Hall effect signals in this and related materials.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Site Mixing for Engineering Magnetic Topological Insulators

The van der Waals compound, MnBi 2 Te 4 , is the first intrinsic magnetic topological insulator, providing a materials platform for exploring exotic quantum phenomena such as the axion insulator state and the quantum anomalous Hall effect. However, intrinsic structural imperfections lead to bulk conductivity, and the roles of magnetic defects are still unknown. With higher concentrations of the same types of magnetic defects, the isostructural compound MnSb 2 Te 4 is a better model system for a systematic investigation of the connections among magnetism, topology, and lattice defects. In this work, the impact of antisite defects on the magnetism and electronic structure is studied in MnSb 2 Te 4 . Mn-Sb site mixing leads to complex magnetic structures and tunes the interlayer magnetic coupling between antiferromagnetic and ferromagnetic. The detailed nonstoichiometry and site mixing of MnSb2Te4 crystals depend on the growth parameters, which can lead to ≈40% of Mn sites occupied by Sb and ≈15% of Sb sites by Mn in as-grown crystals. Single-crystal neutron diffraction and electron microscopy studies show nearly random distribution of the antisite defects. Band structure calculations suggest that the Mn-Sb site mixing favors a ferromagnetic interlayer coupling, consistent with experimental observation, but is detrimental to the band inversion required for a nontrivial topology. Overall, our results suggest a long-range magnetic order of Mn ions sitting on Bi sites in MnBi 2 Te 4 . The effects of site mixing should be considered in all layered heterostructures that consist of alternating magnetic and topological layers, including the entire family of MnTe(Bi 2 Te 3 )n, its Sb analogs, and their solid solution.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗