Spin-glass behavior in the antiperovskite manganese nitride Mn3CuN codoped with Ge and Si

Antiperovskite manganese nitrides ${\mathrm{Mn}}_3\left({\mathrm{Cu}}_{0.6}{\mathrm{Si}}_x{\mathrm{Ge}}_{0.4?x}\right)N$ ($x=0.05$, 0.1, 0.15) were prepared and their negative thermal expansion, magnetic and specific heat properties were investigated. A frozen state with a freezing temperature was found at ～207 K in ${\mathrm{Mn}}_3\left({\mathrm{Cu}}_{0.6}{\mathrm{Si}}_{0.15}{\mathrm{Ge}}_{0.25}\right)N$. This indicates that ${\mathrm{Mn}}_3\left({\mathrm{Cu}}_{0.6}{\mathrm{Si}}_{0.15}{\mathrm{Ge}}_{0.25}\right)N$ exhibits a spin glass state at low temperatures. We discussed the cause of spin glass behavior and correlated this spin glass behavior with broadening of the negative thermal expansion operation-temperature window of the manganese nitrides ${\mathrm{Mn}}_3\left({\mathrm{Cu}}_{0.6}{\mathrm{Si}}_{0.15}{\mathrm{Ge}}_{0.25}\right)N$.