title: In situ studies of a platform for metastable inorganic crystal growth and materials discovery.
abstract: Rapid shifts in the energy, technological, and environmental demands of materials science call for focused and efficient expansion of the library of functional inorganic compounds. To achieve the requisite efficiency, we need a materials discovery and optimization paradigm that can rapidly reveal all possible compounds for a given reaction and composition space. Here we provide such a paradigm via in situ X-ray diffraction measurements spanning solid, liquid flux, and recrystallization processes. We identify four new ternary sulfides from reactive salt fluxes in a matter of hours, simultaneously revealing routes for ex situ synthesis and crystal growth. Changing the flux chemistry, here accomplished by increasing sulfur content, permits comparison of the allowable crystalline building blocks in each reaction space. The speed and structural information inherent to this method of in situ synthesis provide an experimental complement to computational efforts to predict new compounds and uncover routes to targeted materials by design.
authors.affiliation: Materials Science Division.
authors.forename: Daniel P
authors.identifier: http://orcid.org/0000-0003-3650-7551
authors.initials: DP
authors.lastname: Shoemaker
authors.affiliation: Chemical Sciences and Engineering Division, and.
authors.forename: Yung-Jin
authors.initials: YJ
authors.lastname: Hu
authors.affiliation: Materials Science Division.
authors.forename: Duck Young
authors.initials: DY
authors.lastname: Chung
authors.affiliation: X-ray Science Division, Argonne National Laboratory, Argonne, IL 60439; and.
authors.forename: Gregory J
authors.initials: GJ
authors.lastname: Halder
authors.affiliation: X-ray Science Division, Argonne National Laboratory, Argonne, IL 60439; and.
authors.forename: Peter J
authors.initials: PJ
authors.lastname: Chupas
authors.affiliation: Chemical Sciences and Engineering Division, and.
authors.forename: L
authors.initials: L
authors.lastname: Soderholm
authors.affiliation: Materials Science Division.
authors.forename: J F
authors.initials: JF
authors.lastname: Mitchell
authors.affiliation: Materials Science Division,Department of Chemistry, Northwestern University, Evanston, IL 60208 m-kanatzidis@northwestern.edu.
authors.forename: Mercouri G
authors.initials: MG
authors.lastname: Kanatzidis