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Neutron powder diffraction patterns measured above T  C   have been used to determine the location of the excess Mn in Mn x Ga (1.15 ≤ x ≤ 1.8). This information has then been used to constrain the fits to neutron powder diffraction patterns measured at ambient temperature and so determine unambiguously the Mn moments in this system. We find that Mn randomly occupies the two Ga sites (2 a  and 2 b ) in the I4/ mmm  structure and propose that it is more appropriate to use a simpler structure based on the P4/ mmm  space group with a reduced unit cell. In this structure the two Ga sites are formally equivalent (they occupy the 1 a  site while Mn occupies the 1 d  site). Our experimental observations are supported by DFT calculations. Below T  C   we find that the Mn(1 d ) moment is constant at 2.45(3)  μ    B  , while Mn on the 1 a  site carries a slightly larger moment (~3  μ    B  ) that is coupled antiparallel to the Mn(1 d ) moments, leading to the observed drop in magnetisation with increasing Mn content in Mn x Ga.

The Magnetic and Crystal Structure of MnxGa (1.15 ≤ x ≤ 1.8) Alloys