Unlocking surface octahedral tilt in two-dimensional Ruddlesden-Popper perovskites

Molecularly soft organic-inorganic hybrid perovskites are susceptible to dynamic instabilities of the lattice called octahedral tilt, which directly impacts their carrier transport and exciton-phonon coupling. Although the structural phase transitions associated with octahedral tilt has been extensively studied in 3D hybrid halide perovskites, its impact in hybrid 2D perovskites is not well understood. Here, we used scanning tunneling microscopy (STM) to directly visualize surface octahedral tilt in freshly exfoliated 2D Ruddlesden-Popper perovskites (RPPs) across the homologous series, whereby the steric hindrance imposed by long organic cations is unlocked by exfoliation. The experimentally determined octahedral tilts from n = 1 to n = 4 RPPs from STM images are found to agree very well with out-of-plane surface octahedral tilts predicted by density functional theory calculations. The surface-enhanced octahedral tilt is correlated to excitonic redshift observed in photoluminescence (PL), and it enhances inversion asymmetry normal to the direction of quantum well and promotes Rashba spin splitting for n > 1.

Extremely high upper critical field in BiCh2-based (Ch: S and Se) layered superconductor LaO0.5F0.5BiS2−xSex (x = 0.22 and 0.69)

Centrosymmetric compounds with local inversion symmetry breaking have tremendously interesting and intriguing physical properties. In this study, we focus on a BiCh2-based (Ch: S, Se) layered superconductor, as a system with local inversion asymmetry, because spin polarisation based on the Rashba–Dresselhaus-type spin–orbit coupling has been observed in centrosymmetric BiCh2-based LaOBiS2 systems, while the BiCh2 layer lacks local inversion symmetry. Herein, we report the existence of extremely high in-plane upper critical fields in the BiCh2-based system LaO0.5F0.5BiS2−xSex (x = 0.22 and 0.69). The superconducting states are not completely suppressed by the applied magnetic fields with strengths up to 55 T. Thus, we consider that the in-plane upper critical field is enhanced by the local inversion symmetry breaking and its layered structure. Our study will open a new pathway for the discovery of superconductors that exhibit a high upper critical field by focusing on the local inversion symmetry breaking.

Altermagnetism: spin-momentum locked phase protected by non-relativistic symmetries

The search for novel magnetic quantum phases, phenomena and functional materials has been guided by relativistic magnetic-symmetry groups in coupled spin and real space from the dawn of the field in 1950s to the modern era of topological matter. However, the magnetic groups cannot disentangle non-relativistic phases and effects, such as the recently reported unconventional spin physics in collinear antiferromagnets, from the typically weak relativistic spin-orbit coupling phenomena. Here we discover that more general spin symmetries in decoupled spin and crystal space categorize non-relativistic collinear magnetism in three phases: conventional ferromagnets and antiferromangets, and a third distinct phase combining zero net magnetization with an alternating spin-momentum locking in energy bands, which we dub "altermagnetic". For this third basic magnetic phase, which is omitted by the relativistic magnetic groups, we develop a spin-group theory describing six characteristic types of the altermagnetic spin-momentum locking. We demonstrate an extraordinary spin-splitting mechanism in altermagnetic bands originating from a local electric crystal field, which contrasts with the conventional magnetic or relativistic splitting by global magnetization or inversion asymmetry. Based on first-principles calculations, we identify altermagnetic candidates ranging from insulators and metals to a parent crystal of cuprate superconductor. Our results underpin emerging research of quantum phases and spintronics in high-temperature magnets with light elements, vanishing net magnetization, and strong spin-coherence.

Field-free spin-orbit torque-induced switching of perpendicular magnetization in a ferrimagnetic layer with a vertical composition gradient

Current-induced spin-orbit torques (SOTs) are of interest for fast and energy-efficient manipulation of magnetic order in spintronic devices. To be deterministic, however, switching of perpendicularly magnetized materials by SOT requires a mechanism for in-plane symmetry breaking. Existing methods to do so involve the application of an in-plane bias magnetic field, or incorporation of in-plane structural asymmetry in the device, both of which can be difficult to implement in practical applications. Here, we report bias-field-free SOT switching in a single perpendicular CoTb layer with an engineered vertical composition gradient. The vertical structural inversion asymmetry induces strong intrinsic SOTs and a gradient-driven Dzyaloshinskii–Moriya interaction (g-DMI), which breaks the in-plane symmetry during the switching process. Micromagnetic simulations are in agreement with experimental results, and elucidate the role of g-DMI in the deterministic switching processes. This bias-field-free switching scheme for perpendicular ferrimagnets with g-DMI provides a strategy for efficient and compact SOT device design.

Tunable spin-valley coupling in layered polar Dirac metals

In non-centrosymmetric metals, spin-orbit coupling induces momentum-dependent spin polarization at the Fermi surfaces. This is exemplified by the valley-contrasting spin polarization in monolayer transition metal dichalcogenides with in-plane inversion asymmetry. However, the valley configuration of massive Dirac fermions in transition metal dichalcogenides is fixed by the graphene-like structure, which limits the variety of spin-valley coupling. Here, we show that the layered polar metal BaMnX2 (X = Bi, Sb) hosts tunable spin-valley-coupled Dirac fermions, which originate from the distorted X square net with in-plane lattice polarization. We found that BaMnBi2 has approximately one-tenth the lattice distortion of BaMnSb2, from which a different configuration of spin-polarized Dirac valleys is theoretically predicted. This was experimentally observed as a clear difference in the Shubnikov-de Haas oscillation at high fields between the two materials. The chemically tunable spin-valley coupling in BaMnX2 makes it a promising material for various spin-valleytronic devices.