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Abstract:

Antiferromagnetic (AFM) materials provide a platform to couple altermagnetic (AM) spin-splitting with the magneto-optical Kerr effect (MOKE), offering potential for next-generation quantum technologies. In this work, first-principles calculations, symmetry analysis, and ��·�� modeling are employed to show that interlayer sliding in AFM multiferroic bilayers enables control of electronic, magnetic, and magneto-optical properties. This study reveals an intriguing dimension-driven AM crossover: the 2D paraelectric (PE) bilayer exhibits spin-degenerate bands protected by the [C₂∥M_c] spin-space symmetry, whereas the 3D counterpart manifests AM spin-splitting along k_z ≠ 0 paths. Furthermore, interlayer sliding breaks this M_c symmetry and stabilizes a ferroelectric (FE) state with compensated ferrimagnetism, where the Zeeman-like field is responsible for the nonrelativistic spin-splitting. In the FE phase, spin–orbit coupling (SOC) lifts accidental degeneracies and produces “alternating” spin-polarized bands through the interplay of Zeeman and Rashba effects. Crucially, spin polarization, ferrovalley polarization (ΔE_V), and the Kerr angle (θ_k) can all be reversed by switching either sliding ferroelectricity or the Néel vector. Our findings reveal the rich coupling among electronic, magnetic, and optical orders in sliding multiferroics, illustrating new prospects for ultralow-power spintronic and optoelectronic devices.

Abstract:

Antiferromagnetic materials are promising platforms for the development of ultrafast spintronics and magnonics due to their robust magnetism, high-frequency relativistic dynamics, low-loss transport, and the ability to support topological textures. However, achieving deterministic control over antiferromagnetic order in thin films is a major challenge due to the formation of multidomain states stabilized by competing magnetic and destressing interactions. Thus, the successful implementation of antiferromagnetic materials necessitates careful engineering of their anisotropy. Here, we demonstrate strain-based, robust control over multiple antiferromagnetic anisotropies and nanoscale domains in the promising spintronic candidate α-Fe2O3 at room temperature. By applying isotropic and anisotropic in-plane strains across a broad temperature–strain phase space, we systematically tune the interplay between magneto-crystalline and magneto-elastic interactions. We observe that strain-driven control steers the system toward an aligned antiferromagnetic state, while preserving topological spin textures, such as merons, antimerons, and bimerons. We directly map the nanoscale antiferromagnetic order using linear dichroic scanning transmission X-ray microscopy integrated with in situ strain and temperature control. A Landau model and micromagnetic simulations reveal how strain reshapes the magnetic energy landscape. These findings suggest that strain could serve as a versatile control mechanism to reconfigure equilibrium or dynamic antiferromagnetic states on demand in α-Fe2O3 for implementation in next-generation spintronic and magnonic devices.

Abstract:

Molecular piezoelectrics are a potentially disruptive technology, enabling a new generation of self-powered electronics that are flexible, high performing, and inherently low in toxicity. Although significant efforts have been made toward understanding their structural design by targeted manipulation of phase transition behavior, the resulting achievable piezoresponse has remained limited. In this work, we use a low-symmetry, zero-dimensional (0D) inorganic framework alongside a carefully selected ‘quasi-spherical’ organic cation to manipulate organic–inorganic interactions and thus form the hybrid, piezoelectric material [(CH3)3NCH2I]3Bi2I9. Using variable–temperature single crystal X-ray diffraction and solid-state nuclear magnetic resonance spectroscopy, we demonstrate that this material simultaneously exhibits an order–disorder and displacive symmetry-breaking phase transition. This phase transition is mediated by halogen bonding between the organic and inorganic frameworks and results in a large piezoelectric response, d 33 = 161.5 pm/V. This value represents a 4-fold improvement on previously reported halobismuthate piezoelectrics and is comparable to those of commercial inorganic piezoelectrics, thus offering a new pathway toward low-cost, low-toxicity mechanical energy harvesting and actuating devices.