Leveraging Density Functional Theory in the Design of Novel Metal Organic Chalcogenide Assemblies (MOChAs)

In this work, we use density functional theory (DFT) and geometric algorithms to propose hypothetical low-energy metal organic chalcogenide assemblies (MOChAs) to aid synthesis efforts. MOChAs are hybrid organic-inorganic, self-assembled Van der Waals crystals where low-dimensional transition-metal chalcogenide (TMC) inorganic structures are scaffolded by organic ligands, which insulate the TMC structures from one another. <br/>Despite being bulk crystals, MOChAs, like other low-dimensional TMC materials, host excitonic properties relevant to optoelectronic applications. The choice of organic ligand can control the geometry of the inorganic structure which drives the optoelectronic properties of the MOChAs. This tunability and ease of synthesizability makes MOChAs a compelling material class for exploring structure-property relationships. <br/>We propose hypothetical MOChA structures by systematically generating hypothetical combinations of inorganic structures, organic ligands, and corresponding stacking patterns and evaluating their energetics with DFT. We benchmark our methods on experimentally synthesized MOChAs. In this talk we (i) discuss the efficacy of using DFT as a computational aid to evaluate MOChA structure feasibility, (ii) relate changes in MOChA geometry to electronic properties, and (iii) present a library of energetically favorable hypothetical MOChAs.