Nitrogen Dissolution in Liquid Ga and Fe: Comprehensive Ab Initio Analysis, Relevance for Crystallization of GaN

Materials

Jacek Piechota¹  Izabella Grzegory¹  Bohdan Sadovyi¹  Sylwester Porowski¹  Petro Sadovyi¹  Stanislaw Krukowski¹ 

[1] Institute of High Pressure Physics, Polish Academy of Sciences, 29/37, Sokolowska Street, 01-142 Warsaw, Poland;

关键词: ab initio;    calculations;    nitrogen solubility;    liquid gallium;    liquid iron;    gallium nitride;   

DOI  :  10.3390/ma14051306

来源: DOAJ

【 摘 要 】

The dissolution of molecular nitrogen in Ga and Fe was investigated by ab initio calculations and some complementary experiments. It was found that the N bonding inside these solvents is fundamentally different. For Ga, it is between Ga4s and Ga4p and N2p states whereas for Fe this is by N2p to Fe4s, Fe4p and Fe3d states. Accordingly, the energy of dissolution of N${}_2$ for arbitrarily chosen starting atomic configurations was 0.535 eV/mol and −0.299 eV/mol for Ga and Fe, respectively. For configurations optimized with molecular dynamics, the difference between the corresponding energy values, 1.107 eV/mol and 0.003 eV/mol, was similarly large. Full thermodynamic analysis of chemical potential was made employing entropy-derived terms in a Debye picture. The entropy-dependent terms were obtained via a normal conditions path to avoid singularity of ideal gas entropy at zero K. Nitrogen solubility as a function of temperature and N${}_2$ pressure was evaluated, being much higher for Fe than for Ga. For $T=1800$ K and $p={10}^4$ bar, the N concentration in Ga was $3\times {10}^{-3}$ at. fr. whereas for Fe, it was $9\times {10}^{-2}$ at. fr. in very good agreement with experimental data. It indicates that liquid Fe could be a prospective solvent for GaN crystallization from metallic solutions.

【 授权许可】

Unknown