The energy landscape concept and its implications for synthesis planning

Abstract

AbstractSynthesis of novel solids, in a chemical sense, is one of the spearheads of innovation in materials research. However, such an undertaking is substantially impaired by lack of control and predictability. We present a concept that points the way towards rational planning of syntheses in solid state and materials chemistry. The foundation of our approach is the representation of the whole material world, i.e., the known and not-yet-known chemical compounds, on an energy landscape, which implies information about the free energies of these configurations. From this it follows at once that all chemical compounds capable of existence (both thermodynamically stable and metastable ones) are already present in virtuo in this landscape. For the first step of synthesis planning, i.e., the identification of candidates that are capable of existence, we computationally search the respective potential energy landscapes for (meta)stable structure candidates. Recently we have extended our techniques to finite temperatures and pressures and calculated phase diagrams, including metastable manifestations of matter, without resorting to any experimental pre-information. The conception developed is physically consistent, and its feasibility has been proven. Applying appropriate experimental tools has enabled us to realize, e.g., elusive Na3 N, including almost all of its predicted polymorphs, many years after the predictions were published.