Tetrel-pnictides of rare-earth and transition metals, R(M)-T-Pn (M = transition metal; T = Si, Ge; Pn = P, As), represent a scarcely investigated class of compound with complex structural chemistry and potentially interesting properties. By combining rare-earth and transition metals, new quaternary tetrel-pnictide phases (R-M-T-Pn), both doping phases and new structural types, can be formed. The synthesis of these compounds is a challenge prompted us to look for new approach. Due to the volatility of phosphorus and arsenic, it is not possible to directly melt the reactants without strong depleting of sample with pnictogen due to evaporation. Target phases decompose peritectically below 1000oC, below this temperature Si and Ge are inert. Multicomponent nature of the target phase prevents effective use of molten flux reactions due to different solubility and dissolution rates of constituent components, Pn&gt;R&gt;M&gt;&gt;T. Gas transport reactions also appeared to be ineffective for quaternary systems. As such, a synthesis using pre-reacted {R, M, and T} quasi- or true ternary compositions with phosphorus or arsenic becomes very appealing. Although R-M-T binaries and ternaries typically have melting points above 1000oC, our in-situ X-ray diffraction studies show that they are reactive in the presence of a pnictogen-rich atmosphere at temperatures as low as 650oC, thereby forming desired tetrel-pnictide compounds. Therefore, careful optimization of the starting reactant ratios can yield phase-pure single-phase compounds, where excess P and As can be sublimed away from the phase of interest. Furthermore, this method can generate single crystals for structural characterization due to the P and As acting as transport agents in addition to being reactants. The structural chemistry, polymorphism, and properties of the family of {R,T}-Si-Pn compounds will be discussed.

Non-centrosymmetric metal tetrel-pnictides: Synthesis, structure, and Pproperties

Macromolecular Chemistry: The Second Century

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