Tunable negative thermal expansion related with the gradual evolution of antiferromagnetic ordering in antiperovskite manganese nitrides Ag1-xNMn3+x (0<x<0.6)

The thermal expansion and magnetic properties of antiperovskite manganese nitrides Ag1-xNMn3+x were reported. The substitution of Mn for Ag effectively broadens the temperature range of negative thermal expansion and drives it to cryogenic temperatures. As x increases, the paramagnetic (PM) to antiferromagnetic (AFM) phase transition temperature (TN) decreases. At x~0.2, the PM-AFM transition overlaps with the AFM to glass-like state transition. Above x=0.2, two new distinct magnetic transitions were observed: one occurs above room temperature from PM to ferromagnetic (FM), and the other one evolves at a lower temperature (T*) below which both AFM and FM orderings are involved. Further electron spin resonance measurement suggests that the broadened volume change near T* is closely related with the evolution of {\Gamma}5g AFM ordering.