Phase diagrams on composition-spread Fey_yTe1−x_{1-x}Sex_x films

Fe$_y$Te$_{1-x}$Se$_x$, an archetypical iron-based high-temperature superconductor with a simple structure but rich physical properties, has attracted lots of attention because the two end compositions, Se content $x = 0$ and 1, exhibit antiferromagnetism and nematicity, respectively, making it an ideal candidate for studying their interactions with superconductivity. However, what is clearly lacking to date is a complete phase diagram of Fe$_y$Te$_{1-x}$Se$_x$ as functions of its chemical compositions since phase separation usually occurs from $x\sim 0.6$ to 0.9 in bulk crystals. Moreover, fine control of its composition is experimentally challenging because both Te and Se are volatile elements. Here we establish a complete phase diagram of Fe$_y$Te$_{1-x}$Se$_x$, achieved by high-throughput film synthesis and characterization techniques. An advanced combinatorial synthesis process enables us to fabricate an epitaxial composition-spread Fe$_y$Te$_{1-x}$Se$_x$ film encompassing the entire Se content $x$ from 0 to 1 on a single piece of CaF$_2$ substrate. The micro-region composition analysis and X-ray diffraction show a successful continuous tuning of chemical compositions and lattice parameters, respectively. The micro-scale pattern technique allows the mapping of electrical transport properties as a function of relative Se content with an unprecedented resolution of 0.0074. Combining with the spin patterns in literature, we build a detailed phase diagram that can unify the electronic and magnetic properties of Fe$_y$Te$_{1-x}$Se$_x$. Our composition-spread Fe$_y$Te$_{1-x}$Se$_x$ films, overcoming the challenges of phase separation and precise control of chemical compositions, provide an ideal platform for studying the relationship between superconductivity and magnetism.Comment: 13 pages,5 figures and Supplementary Material 3 pages,3 figure