Interface Nucleus Complementarity: An Iterative Process for the Discovery of Modular Intermetallics Guided by...

We present an iterative process for the discovery of modular intermetallic structures based on a recently developed interface nucleus approach. The process begins with the proposal of a suitable geometric motif that may serve as an interface nucleus. We then screen crystallographic databases for structures containing this motif as potential intergrowth partners. The extent to which pairs of these structures are likely to combine into more complicated assembles is then assessed with a new chemical pressure-based metric, interface nucleus complementarity (INC). Promising combinations of structures are translated into systems for synthesis, with new compounds providing either support for the importance of the original interface nucleus or new geometrical motifs for the next round of analysis. We demonstrate this process using a fragment derived from the σ-phase structure as a starting point, leading to the synthesis of PrMg_4.13Zn_10.20 and a new motif to seed the next cycle.