Fabrication of Single‐Crystalline CoCrFeNi Thin Films by DC Magnetron Sputtering: A Route to Surface Studies of High‐Entropy Alloys

Abstract High‐entropy alloys (HEAs) with their almost limitless number of possible compositions have raised widespread attention in material science. Next to wear and corrosion resistive coatings, their application as tunable electrocatalysts has recently moved into the focus. On the other hand, fundamental properties of HEA surfaces like atomic and electronic structure, surface segregation and diffusion as well as adsorption on HEA surfaces are barely explored. The lack of research is caused by the limited availability of single‐crystalline samples. In the present work, the epitaxial growth of face centered cubic (fcc) CoCrFeNi films on MgO(100) is reported. Their characterization by X‐ray diffraction (XRD), energy dispersive X‐ray spectroscopy (EDX), and transmission electron microscopy (TEM) demonstrates that the layers with a homogeneous and close to equimolar elemental composition are oriented in [100] direction and aligned with the substrate to which they form an abrupt interface. X‐ray photoelectron spectroscopy (XPS), low‐energy electron diffraction (LEED), and angle‐resolved photoelectron spectroscopy are employed to study chemical composition and atomic and electronic structure of CoCrFeNi(100). It is demonstrated that epitaxially grown HEA films have the potential to fill the sample gap, allowing for fundamental studies of properties of and processes on well‐defined HEA surfaces over the full compositional space.