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1.
Nat Commun ; 15(1): 4305, 2024 Jun 11.
Article in English | MEDLINE | ID: mdl-38862480

ABSTRACT

Antiferromagnets (AFMs) have the natural advantages of terahertz spin dynamics and negligible stray fields, thus appealing for use in domain-wall applications. However, their insensitive magneto-electric responses make controlling them in domain-wall devices challenging. Recent research on noncollinear chiral AFMs Mn3X (X = Sn, Ge) enabled us to detect and manipulate their magnetic octupole domain states. Here, we demonstrate a current-driven fast magnetic octupole domain-wall (MODW) motion in Mn3X. The magneto-optical Kerr observation reveals the Néel-like MODW of Mn3Ge can be accelerated up to 750 m s-1 with a current density of only 7.56 × 1010 A m-2 without external magnetic fields. The MODWs show extremely high mobility with a small critical current density. We theoretically extend the spin-torque phenomenology for domain-wall dynamics from collinear to noncollinear magnetic systems. Our study opens a new route for antiferromagnetic domain-wall-based applications.

2.
Sci Adv ; 10(15): eadk1415, 2024 Apr 12.
Article in English | MEDLINE | ID: mdl-38608018

ABSTRACT

Magnetic semimetals form an attractive class of materials because of the nontrivial contributions of itinerant electrons to magnetism. Because of their relatively low-carrier-density nature, a doping level of those materials could be largely tuned by a gating technique. Here, we demonstrate gate-tunable ferromagnetism in an emergent van der Waals magnetic semimetal Cr3Te4 based on an ion-gating technique. Upon doping electrons into the system, the Curie temperature (TC) sharply increases, approaching near to room temperature, and then decreases to some extent. This non-monotonous variation of TC accompanies the switching of the magnetic anisotropy, synchronously followed by the sign changes of the ordinary and anomalous Hall effects. Those results clearly elucidate that the magnetism in Cr3Te4 should be governed by its semimetallic band nature.

3.
J Phys Condens Matter ; 36(27)2024 Apr 08.
Article in English | MEDLINE | ID: mdl-38447148

ABSTRACT

The chiral Majorana fermion is an exotic particle that is its own antiparticle. It can arise in a one-dimensional edge of topological materials, and especially that in a topological superconductor can be exploited in non-Abelian quantum computation. While the chiral Majorana mode (CMM) remains elusive, a promising situation is realized when superconductivity coexists with a topologically non-trivial surface state. Here, we perform fully non-empirical calculation for the CMM considering superconductivity and surface relaxation, and show that hexagonal close-packed thallium (Tl) has an ideal electronic state that harbors the CMM. Thekz=0plane of Tl is a mirror plane, realizing a full-gap band inversion corresponding to a topological crystalline insulating phase. Its surface and hinge are stable and easy to make various structures. Another notable feature is that the surface Dirac point is very close to the Fermi level, so that a small Zeeman field can induce a topological transition. Our calculation indicates that Tl will provide a new platform of the Majorana fermion.

4.
Acta Crystallogr A Found Adv ; 80(Pt 1): 94-103, 2024 Jan 01.
Article in English | MEDLINE | ID: mdl-37994704

ABSTRACT

A spin space group provides a suitable way of fully exploiting the symmetry of a spin arrangement with a negligible spin-orbit coupling. There has been a growing interest in applying spin symmetry analysis with the spin space group in the field of magnetism. However, there is no established algorithm to search for spin symmetry operations of the spin space group. This paper presents an exhaustive algorithm for determining the spin symmetry operations of commensurate spin arrangements. The present algorithm searches for spin symmetry operations from the symmetry operations of a corresponding nonmagnetic crystal structure and determines their spin-rotation parts by solving a Procrustes problem. An implementation is distributed under a permissive free software license in spinspg Version 0.1.1, available at https://github.com/spglib/spinspg.

5.
Nat Commun ; 14(1): 8240, 2023 Dec 12.
Article in English | MEDLINE | ID: mdl-38086819

ABSTRACT

The anomalous Hall effect (AHE) that emerges in antiferromagnetic metals shows intriguing physics and offers numerous potential applications. Magnets with a rutile crystal structure have recently received attention as a possible platform for a collinear-antiferromagnetism-induced AHE. RuO2 is a prototypical candidate material, however the AHE is prohibited at zero field by symmetry because of the high-symmetry [001] direction of the Néel vector at the ground state. Here, we show AHE at zero field in Cr-doped rutile, Ru0.8Cr0.2O2. The magnetization, transport and density functional theory calculations indicate that appropriate doping of Cr at Ru sites reconstructs the collinear antiferromagnetism in RuO2, resulting in a rotation of the Néel vector from [001] to [110] while maintaining a collinear antiferromagnetic state. The AHE with vanishing net moment in the Ru0.8Cr0.2O2 exhibits an orientation dependence consistent with the [110]-oriented Hall vector. These results demonstrate that material engineering by doping is a useful approach to manipulate AHE in antiferromagnetic metals.

6.
Nat Commun ; 14(1): 8239, 2023 Dec 12.
Article in English | MEDLINE | ID: mdl-38086824

ABSTRACT

Electrons at the border of localization generate exotic states of matter across all classes of strongly correlated electron materials and many other quantum materials with emergent functionality. Heavy electron metals are a model example, in which magnetic interactions arise from the opposing limits of localized and itinerant electrons. This remarkable duality is intimately related to the emergence of a plethora of novel quantum matter states such as unconventional superconductivity, electronic-nematic states, hidden order and most recently topological states of matter such as topological Kondo insulators and Kondo semimetals and putative chiral superconductors. The outstanding challenge is that the archetypal Kondo lattice model that captures the underlying electronic dichotomy is notoriously difficult to solve for real materials. Here we show, using the prototypical strongly-correlated antiferromagnet CeIn3, that a multi-orbital periodic Anderson model embedded with input from ab initio bandstructure calculations can be reduced to a simple Kondo-Heisenberg model, which captures the magnetic interactions quantitatively. We validate this tractable Hamiltonian via high-resolution neutron spectroscopy that reproduces accurately the magnetic soft modes in CeIn3, which are believed to mediate unconventional superconductivity. Our study paves the way for a quantitative understanding of metallic quantum states such as unconventional superconductivity.

7.
Nat Commun ; 14(1): 8050, 2023 Dec 05.
Article in English | MEDLINE | ID: mdl-38052859

ABSTRACT

Magnetic skyrmions, topological vortex-like spin textures, garner significant interest due to their unique properties and potential applications in nanotechnology. While they typically form a hexagonal crystal with distinct internal magnetisation textures known as Bloch- or Néel-type, recent theories suggest the possibility for direct transitions between skyrmion crystals of different lattice structures and internal textures. To date however, experimental evidence for these potentially useful phenomena have remained scarce. Here, we discover the polar tetragonal magnet EuNiGe3 to host two hybrid skyrmion phases, each with distinct internal textures characterised by anisotropic combinations of Bloch- and Néel-type windings. Variation of the magnetic field drives a direct transition between the two phases, with the modification of the hybrid texture concomitant with a hexagonal-to-square skyrmion crystal transformation. We explain these observations with a theory that includes the key ingredients of momentum-resolved Ruderman-Kittel-Kasuya-Yosida and Dzyaloshinskii-Moriya interactions that compete at the observed low symmetry magnetic skyrmion crystal wavevectors. Our findings underscore the potential of polar magnets with rich interaction schemes as promising for discovering new topological magnetic phases.

8.
Nat Commun ; 14(1): 6339, 2023 Oct 10.
Article in English | MEDLINE | ID: mdl-37816724

ABSTRACT

The discovery of topological insulators and semimetals triggered enormous interest in exploring emergent electromagnetic responses in solids. Particular attention has been focused on ternary half-Heusler compounds, whose electronic structure bears analogy to the topological zinc-blende compounds while also including magnetic rare-earth ions coupled to conduction electrons. However, most of the research in this system has been in band-inverted zero-gap semiconductors such as GdPtBi, which still does not fully exhaust the large potential of this material class. Here, we report a less-studied member of half-Heusler compounds, HoAuSn, which we show is a trivial semimetal or narrow-gap semiconductor at zero magnetic field but undergoes a field-induced transition to a Weyl semimetal, with a negative magnetoresistance exceeding four orders of magnitude at low temperatures. The combined study of Shubnikov-de Haas oscillations and first-principles calculation suggests that the exchange field from Ho 4f moments reconstructs the band structure to induce Weyl points which play a key role in the strong suppression of large-angle carrier scattering. Our findings demonstrate the unique mechanism of colossal negative magnetoresistance and provide pathways towards realizing topological electronic states in a large class of magnetic half-Heusler compounds.

9.
Angew Chem Int Ed Engl ; 62(42): e202309055, 2023 Oct 16.
Article in English | MEDLINE | ID: mdl-37635091

ABSTRACT

The origin of the bulk photovoltaic effect (BPVE) was considered as a built-in electric field formed by the macroscopic polarization of materials. Alternatively, the "shift current mechanism" has been gradually accepted as the more appropriate description of the BPVE. This mechanism implies that the photocurrent generated by the BPVE is a topological current featuring an ultrafast response and dissipation-less nature, which is very attractive for photodetector applications. Meanwhile, the origin of the BPVE in organic-inorganic hybrid perovskites (OIHPs) has not been discussed and is still widely accepted as the classical mechanism without any experimental evidence. Herein, we observed the BPVE along the nonpolar axis in OIHPs, which is inconsistent with the classical explanation. Furthermore, based on the nonlinear optical tensor correlation, we substantiated that the BPVE in OIHPs is originated in the shift current mechanism.

10.
Phys Rev Lett ; 130(16): 166002, 2023 Apr 21.
Article in English | MEDLINE | ID: mdl-37154662

ABSTRACT

Motivated by cuprate and nickelate superconductors, we perform a comprehensive study of the superconducting instability in the single-band Hubbard model. We calculate the spectrum and superconducting transition temperature T_{c} as a function of filling and Coulomb interaction for a range of hopping parameters, using the dynamical vertex approximation. We find the sweet spot for high T_{c} to be at intermediate coupling, moderate Fermi surface warping, and low hole doping. Combining these results with first principles calculations, neither nickelates nor cuprates are close to this optimum within the single-band description. Instead, we identify some palladates, notably RbSr_{2}PdO_{3} and A_{2}^{'}PdO_{2}Cl_{2} (A^{'}=Ba_{0.5}La_{0.5}), to be virtually optimal, while others, such as NdPdO_{2}, are too weakly correlated.

11.
ACS Nano ; 17(3): 1916-1924, 2023 Feb 14.
Article in English | MEDLINE | ID: mdl-36700561

ABSTRACT

Stacking order is expected to have a significant impact on the properties of van der Waals layered magnets, as it determines the crystallographic and magnetic symmetry. Recent synchrotron-based optical studies on antiferromagnetic MnPS3 have revealed a thickness-dependent symmetry crossover, suggesting possible different stackings in few-layer crystals from the bulk, which, however, has not been explicitly identified. Here, by using a combination of atomic-scale electron microscopy and theoretical calculations, we show that despite the bulk monoclinic stacking persists macroscopically down to bilayer, additional local rippling effect lifts the monoclinic symmetry of the few layers while preserving the trigonal symmetry of individual monolayers, leading to possible monolayer-like behavior in ultrathin MnPS3 samples. This finding reveals the profound impact of rippling on the microscopic symmetry of two-dimensional materials with weak interlayer interactions and raises the possibility of approaching the paradigmatic two-dimensional Néel antiferromagnetic honeycomb lattice in MnPS3 without reaching monolayer thickness.

12.
Nature ; 613(7944): 490-495, 2023 01.
Article in English | MEDLINE | ID: mdl-36653566

ABSTRACT

The tunnelling electric current passing through a magnetic tunnel junction (MTJ) is strongly dependent on the relative orientation of magnetizations in ferromagnetic electrodes sandwiching an insulating barrier, rendering efficient readout of spintronics devices1-5. Thus, tunnelling magnetoresistance (TMR) is considered to be proportional to spin polarization at the interface1 and, to date, has been studied primarily in ferromagnets. Here we report observation of TMR in an all-antiferromagnetic tunnel junction consisting of Mn3Sn/MgO/Mn3Sn (ref. 6). We measured a TMR ratio of around 2% at room temperature, which arises between the parallel and antiparallel configurations of the cluster magnetic octupoles in the chiral antiferromagnetic state. Moreover, we carried out measurements using a Fe/MgO/Mn3Sn MTJ and show that the sign and direction of anisotropic longitudinal spin-polarized current in the antiferromagnet7 can be controlled by octupole direction. Strikingly, the TMR ratio (about 2%) of the all-antiferromagnetic MTJ is much larger than that estimated using the observed spin polarization. Theoretically, we found that the chiral antiferromagnetic MTJ may produce a substantially large TMR ratio as a result of the time-reversal, symmetry-breaking polarization characteristic of cluster magnetic octupoles. Our work lays the foundation for the development of ultrafast and efficient spintronic devices using antiferromagnets8-10.

13.
J Am Chem Soc ; 144(37): 16866-16871, 2022 Sep 21.
Article in English | MEDLINE | ID: mdl-36066406

ABSTRACT

Configurational entropy can impact crystallization processes, tipping the scales between structures of nearly equal internal energy. Using alloyed single crystals of Gd2PdSi3 in the AlB2-type structure, we explore the formation of complex layer sequences made from alternating, two-dimensional triangular and honeycomb slabs. A four-period and an eight-period stacking sequence are found to be very close in internal energy, the latter being favored by entropy associated with covering the full configuration space of interlayer bonds. Possible consequences of polytype formation on magnetism in Gd2PdSi3 are discussed.

14.
Nature ; 607(7919): 474-479, 2022 07.
Article in English | MEDLINE | ID: mdl-35859198

ABSTRACT

Electrical control of a magnetic state of matter lays the foundation for information technologies and for understanding of spintronic phenomena. Spin-orbit torque provides an efficient mechanism for the electrical manipulation of magnetic orders1-11. In particular, spin-orbit torque switching of perpendicular magnetization in nanoscale ferromagnetic bits has enabled the development of stable, reliable and low-power memories and computation12-14. Likewise, for antiferromagnetic spintronics, electrical bidirectional switching of an antiferromagnetic order in a perpendicular geometry may have huge impacts, given its potential advantage for high-density integration and ultrafast operation15,16. Here we report the experimental realization of perpendicular and full spin-orbit torque switching of an antiferromagnetic binary state. We use the chiral antiferromagnet Mn3Sn (ref. 17), which exhibits the magnetization-free anomalous Hall effect owing to a ferroic order of a cluster magnetic octupole hosted in its chiral antiferromagnetic state18. We fabricate heavy-metal/Mn3Sn heterostructures by molecular beam epitaxy and introduce perpendicular magnetic anisotropy of the octupole using an epitaxial in-plane tensile strain. By using the anomalous Hall effect as the readout, we demonstrate 100 per cent switching of the perpendicular octupole polarization in a 30-nanometre-thick Mn3Sn film with a small critical current density of less than 15 megaamperes per square centimetre. Our theory reveals that the perpendicular geometry between the polarization directions of current-induced spin accumulation and of the octupole persistently maximizes the spin-orbit torque efficiency during the deterministic bidirectional switching process. Our work provides a significant basis for antiferromagnetic spintronics.

15.
Phys Rev Lett ; 128(20): 206401, 2022 May 20.
Article in English | MEDLINE | ID: mdl-35657875

ABSTRACT

Using a cluster extension of the dynamical mean-field theory, we show that strongly correlated metals subject to Hund's physics exhibit significant electronic structure modulations above magnetic transition temperatures. In particular, in a ferromagnet having a large local moment due to Hund's coupling (Hund's ferromagnet), the Fermi surface expands even above the Curie temperature (T_{C}) as if a spin polarization occurred. Behind this phenomenon, effective "Hund's physics" works in momentum space, originating from ferromagnetic fluctuations in the strong-coupling regime. The resulting significantly momentum-dependent (spatially nonlocal) electron correlations induce an electronic structure reconstruction involving a Fermi surface volume change and a redistribution of the momentum-space occupation. Our finding will give a deeper insight into the physics of Hund's ferromagnets above T_{C}.

16.
Rep Prog Phys ; 85(5)2022 Mar 28.
Article in English | MEDLINE | ID: mdl-35240593

ABSTRACT

The recent discovery of the superconductivity in the doped infinite layer nickelatesRNiO2(R= La, Pr, Nd) is of great interest since the nickelates are isostructural to doped (Ca, Sr)CuO2having superconducting transition temperature (Tc) of about 110 K. Verifying the commonalities and differences between these oxides will certainly give a new insight into the mechanism of highTcsuperconductivity in correlated electron systems. In this paper, we review experimental and theoretical works on this new superconductor and discuss the future perspectives for the 'nickel age' of superconductivity.

17.
Sci Adv ; 8(2): eabk1480, 2022 Jan 14.
Article in English | MEDLINE | ID: mdl-35030028

ABSTRACT

Anomalous Nernst effect (ANE), converting a heat flow to transverse electric voltage, originates from the Berry phase of electronic wave function near the Fermi energy EF. Thus, the ANE provides a sensitive probe to detect a topological state that produces large Berry curvature. In addition, a magnet that exhibits a large ANE using low-cost and safe elements will be useful to develop a novel energy harvesting technology. Here, we report our observation of a high ANE exceeding 3 microvolts per kelvin above room temperature in the kagome ferromagnet Fe3Sn with the Curie temperature of 760 kelvin. Our theoretical analysis clarifies that a "nodal plane" produces a flat hexagonal frame with strongly enhanced Berry curvature, resulting in the large ANE. Our discovery of the large ANE in Fe3Sn opens the path for the previously unexplored functionality of flat degenerate electronic states and for developing flexible film thermopile and heat current sensors.

18.
J Phys Condens Matter ; 34(18)2022 Mar 03.
Article in English | MEDLINE | ID: mdl-34544070

ABSTRACT

Designing materials with advanced functionalities is the main focus of contemporary solid-state physics and chemistry. Research efforts worldwide are funneled into a few high-end goals, one of the oldest, and most fascinating of which is the search for an ambient temperature superconductor (A-SC). The reason is clear: superconductivity at ambient conditions implies being able to handle, measure and access a single, coherent, macroscopic quantum mechanical state without the limitations associated with cryogenics and pressurization. This would not only open exciting avenues for fundamental research, but also pave the road for a wide range of technological applications, affecting strategic areas such as energy conservation and climate change. In this roadmap we have collected contributions from many of the main actors working on superconductivity, and asked them to share their personal viewpoint on the field. The hope is that this article will serve not only as an instantaneous picture of the status of research, but also as a true roadmap defining the main long-term theoretical and experimental challenges that lie ahead. Interestingly, although the current research in superconductor design is dominated by conventional (phonon-mediated) superconductors, there seems to be a widespread consensus that achieving A-SC may require different pairing mechanisms.In memoriam, to Neil Ashcroft, who inspired us all.

19.
Sci Adv ; 7(47): eabj0498, 2021 Nov 19.
Article in English | MEDLINE | ID: mdl-34788092

ABSTRACT

FeSi is a nonmagnetic narrow-gap insulator, exhibiting peculiar charge and spin dynamics beyond a simple band structure picture. Those unusual features have been attracting renewed attention from topological aspects. Although the surface conduction was demonstrated according to size-dependent resistivity in bulk crystals, its topological characteristics and consequent electromagnetic responses remain elusive. Here, we demonstrate an inherent surface ferromagnetic-metal state of FeSi thin films and its strong spin-orbit coupling (SOC) properties through multiple characterizations of two-dimensional conductance, magnetization, and spintronic functionality. Terminated covalent bonding orbitals constitute the polar surface state with momentum-dependent spin textures due to Rashba-type spin splitting, as corroborated by unidirectional magnetoresistance measurements and first-principles calculations. As a consequence of the spin-momentum locking, nonequilibrium spin accumulation causes magnetization switching. These surface properties are closely related to the Zak phase of the bulk band topology. Our findings propose another route to explore noble metal­free materials for SOC-based spin manipulation.

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