Engineering of Magnetically Intercalated Silicene Compound: An Overlooked Polymorph of EuSi₂

Abstract

Silicene, a Si analogue of graphene, is suggested to become a versatile material for nanoelectronics. Being coupled with magnetism, it is predicted to be particularly suitable for spintronic applications. However, experimental realization of free‐standing silicene and its magnetic derivatives is lacking. Fortunately, magnetism can be induced into silicene layers, in particular, by intercalation. Here, a successful synthesis of multilayer silicene intercalated by inherently magnetic Eu ions – a compound expected to exhibit both massless Dirac‐cone states, as its Ca analogue, and a nontrivial magnetic structure – is reported. This new polymorph with EuSi 2 stoichiometry is epitaxially stabilized by continual replication of silicene layers employing Sr‐intercalated multilayer silicene as a template. The atomic structure of the new compound and its sharp interface with the template are confirmed using electron diffraction, X‐ray diffraction, and electron microscopy techniques. Below 80 K, the material demonstrates anisotropic antiferromagnetism coexisting with weak ferromagnetism. The magnetic state is accompanied by an anomalous behavior of magnetoresistivity.