Single Crystal Automated Refinement (SCAR): A Data-Driven Method for Solving Inorganic Structures

Abstract

<p>Single crystal diffraction is one of the most common experimental techniques in chemistry for determining a crystal structure. However, the process of crystal structure solution and refinement is not always straightforward. Methods to simplify and rationalize the path to the most optimal crystal structure model have been incorporated into various data processing and crystal structure solution software, with the focus generally on aiding macromolecular or protein structure solution. In this work, we propose a new method that uses single crystal data to solve the crystal structures of inorganic, extended solids called “Single Crystal Automated Refinement (<i>SCAR</i>).” The approach was developed using data mining and machine-learning methods and considers several structural features common in inorganic solids, like atom assignment based on physically reasonable distances, atomic statistical mixing, and crystallographic site deficiency. The output is a tree of possible solutions for the data set with a corresponding fit score indicating the most reasonable crystal structure. Here, the foundation for <i>SCAR</i> is presented followed by the implementation of <i>SCAR</i> to solve two newly synthesized and previously unreported phases, ZrAu<sub>0.5</sub>Os<sub>0.5</sub> and Nd<sub>4</sub>Mn<sub>2</sub>AuGe<sub>4</sub>. The structure solutions are found to be comparable with manually solving the data set, including the same refined mixed occupancies and atomic deficiency, supporting the validity of this automatic structure solution method. The proposed <i>SCAR</i> program is thusly verified to be a fast and reliable assistant in solving even complex single crystal diffraction data for extended inorganic solids.</p>