title: Evaluating structure selection in the hydrothermal growth of FeS2pyrite and marcasite.
abstract: While the ab initio prediction of the properties of solids and their optimization towards new proposed materials is becoming established, little predictive theory exists as to which metastable materials can be made and how, impeding their experimental realization. Here we propose a quasi-thermodynamic framework for predicting the hydrothermal synthetic accessibility of metastable materials and apply this model to understanding the phase selection between the pyrite and marcasite polymorphs of FeS2. We demonstrate that phase selection in this system can be explained by the surface stability of the two phases as a function of ambient pH within nano-size regimes relevant to nucleation. This result suggests that a first-principles understanding of nano-size phase stability in realistic synthesis environments can serve to explain or predict the synthetic accessibility of structural polymorphs, providing a guideline to experimental synthesis via efficient computational materials design.
authors.affiliation: Department of Materials Science and Engineering, MIT, Cambridge, Massachusetts 02139, USA.
authors.forename: Daniil A
authors.initials: DA
authors.lastname: Kitchaev
authors.affiliation: Department of Materials Science and Engineering, MIT, Cambridge, Massachusetts 02139, USA.|Department of Materials Science and Engineering, UC Berkeley, Berkeley, Calirfornia 94720, USA.|Materials Science Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
authors.forename: Gerbrand
authors.initials: G
authors.lastname: Ceder