Synthesis of a mixed-valent tin nitride and considerations of its possible crystal structures Christopher M. Caskey,1,2,3 Aaron Holder,1 Sarah Shulda2, Steve Christensen,1 David Diercks,2 Craig P. Schwartz,4 David Biagioni,1 Dennis Nordlund,4 Alon Kukliansky,5 Amir Natan,5 David Prendergast,6 Bernardo Orvananos,7 Wenhao Sun,6 Xiuwen Zhang,8 Gerbrand Ceder,7 David S. Ginley,1 William Tumas,1 John D. Perkins,1 Vladan Stevanovic,1,2 Svitlana Pylypenko,2 Stephan Lany,1 Ryan M. Richards,2 Andriy Zakutayev1* 1) National Renewable Energy Laboratory, Golden, CO, USA 2) Colorado School of Mines, Golden, CO, USA 3) Larix Chemical Science, Golden, CO, USA 4) SLAC National Accelerator Laboratory, Menlo Park, CA, USA 5) Tel Aviv University, Israel 6) Lawrence Berkeley National Laboratory, Berkley, CA, USA 7) Massachusetts Institute of Technology, Cambridge, MA, USA 8) University of Colorado, Boulder, CO, USA * e-mail:
[email protected] Abstract Recent advances in theoretical structure prediction methods and high-throughput computational techniques are revolutionizing experimental discovery of the thermodynamically stable inorganic materials. Metastable materials represent a new frontier for studies, since even simple binary non ground state compounds of common elements may be awaiting discovery. However, there are significant research challenges related to non-equilibrium thin film synthesis and crystal structure predictions, such as small strained crystals in the experimental samples and energy minimization based theoretical algorithms. Here we report on experimental synthesis and characterization, as well as theoretical first-principles calculations of a previously unreported mixed-valent binary tin nitride. Thin film experiments indicate that this novel material is N- deficient SnN with tin in the mixed II/IV valence state and a small low-symmetry unit cell.