First-principles investigation of novel polymorphs of Mg2C

Abstract

On the basis of the evolutionary methodology for crystal structure prediction, the potential crystal structures of magnesium carbide with a chemical composition of Mg₂C are explored. Except the known cubic phase (Fmm), two novel tetragonal structures (P4₂/mnm and I4₁/Amd) and two novel hexagonal structures (P6₃/mmc and PM2) of Mg₂C are found. All these four new phases are mechanically and dynamically stable by the calculated elastic constants and phonon dispersions. Furthermore, the effects of pressure and temperature on the phase transitions among different Mg₂C polymorphs are investigated, implying that some new phases especially the P4₂/mnm phase may be synthesized in future. The ratio values of B/G are also calculated in order to analyze the brittle and ductile nature of these Mg₂C phases. In addition, electronic structure calculations suggest that the I4₁/Amd phase is semimetallic and the other three new phases are all metallic, which is different from the previously proposed magnesium carbides. Meanwhile, the calculated electronic density maps reveal that strong ionic bonding exists between the Mg and C atoms.