Thin film quantum materials

Abstract:

Magnetron sputtering offers a scalable route to magnetic topological insulators (MTIs) based on Cr-doped Sb2Te3. We combine a range of X-ray diffraction (XRD), reciprocal-space mapping (RSM), scanning transmission electron microscopy (STEM), scanning TEM-energy-dispersive X-ray spectroscopy (STEM-EDS), and X-ray absorption spectroscopy, and X-ray magnetic circular dichroism (XAS/XMCD) techniques to study the structure and magnetism of Cr-doped Sb2Te3 films. Symmetric θ-2θ XRD and RSM establish a solubility window. Layered tetradymite order persists up to ∼10 at.-% Cr, while higher doping yields CrTe/Cr2Te3 secondary phases. STEM reveals nanocrystalline layered stacking at low Cr and loss of long-range layering at higher Cr concentrations, consistent with XRD/RSM. Magnetometry on a 6% film shows soft ferromagnetism at 5 K. XAS and XMCD at the Cr L2,3 edges exhibits a depth dependence: total electron yield (TE; surface sensitive) shows both nominal Cr2+ and Cr3+, whereas fluorescence yield (FY; bulk sensitive) shows a much higher Cr2+ weight. Sum rules applied to TEY give mL=(0.20±0.04) μB/Cr, and mS=(1.6±0.2) μB/Cr, whereby we note that the applied maximum field (3 T) likely underestimates mS. These results define a practical growth window and outline key parameters for MTI films.

Abstract:

Symmetry engineering is an effective approach for generating emergent phases and quantum phenomena. In magnetic systems, the Dzyaloshinskii-Moriya (DM) interaction is essential for stabilizing chiral spin textures. The symmetry manipulation of DM vectors, described in three dimensions, could provide a strategy toward creating abundant topologically magnetic phases. Here, we have achieved breaking the rotational and mirror symmetries of the three-dimensional DM vectors in a strongly correlated ferromagnet, which were directly measured through the nonreciprocal spin-wave propagations in both in-plane and out-of-plane magnetic field geometries. Combining cryogenic magnetic force microscopy and micromagnetic simulations, we discover a bimeron phase that emerges between the spin spiral and skyrmion phases under an applied magnetic field. Such an artificially manipulated DM interaction is shown to play a critical role in the formation and evolution of the large-area bimeron lattice, a phenomenon that could be realized across a broad range of materials. Our findings demonstrate that symmetry engineering of the DM vectors can be practically achieved through epitaxial strain, paving the way for the creation of diverse spin topologies and the exploration of their emergent functionalities.

Abstract:

The synthesis and magnetic properties of the intrinsic magnetic topological insulator MnBi2Te4, grown by magnetron sputtering, are investigated. While this growth method enables smoother morphologies than molecular beam epitaxy and is compatible with scalable processing, the metastable nature of MnBi2Te4 presents considerable challenges in phase control and magnetic uniformity. By systematically varying the relative sputter powers of Mn, Bi2Te3, and Te targets, conditions that favor the formation of near‐stoichiometric MnBi2Te4, as supported by X‐ray diffraction, atomic force microscopy, and energy‐dispersive X‐ray spectroscopy, are identified. These films exhibit reduce surface roughness and lower twin‐domain density compared to Mn‐rich counterparts, which show evidence of phase separation and structural disorder. Magnetometry and X‐ray magnetic circular dichroism reveal that both film types exhibit sizable Mn moments, although signatures of antiferromagnetic order are only weakly expressed and appear sensitive to composition and morphology. Despite producing structurally well‐ordered films, clear linear dichroism attributable to A‐type antiferromagnetic ordering is not observed, suggesting magnetic inhomogeneity or suppression of interlayer coupling. These results highlight the compositional sensitivity of sputtered MnBi2Te4 and underline the difficulties in stabilizing the intrinsic magnetic topological phase in thin‐film form.