The pressure dependence of magnetic moment in CeMg3 and PrMg3 has been studied through ab initio electronic structure calculations based on density functional theory (DFT). Positive as well as negative pressure conditions were simulated by different degrees of unit cell compression or expansion and a fit of the total energy to the Birch–Murnaghan equation of state. At ambient and negative pressures, the calculated magnetic moments for both the compounds reveal localized behaviour of 4f electrons. For increasing positive pressures, the magnetic moment of Ce in CeMg3 has been observed to diminish smoothly, becoming zero at a critical pressure of PC∼ 18 GPa indicative of pressure induced moment instability caused by an increase of f-conduction electron hybridization leading to delocalization of the 4f electrons. In contrast, the magnetic moment of Pr in PrMg3 does not show appreciable change with pressure, indicating strongly localized nature of the 4f electrons.
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