Tuneable Magnetic Phase Transitions in Layered CeMn2Ge2-xSix Compounds

The structural and magnetic properties of seven CeMn2Ge(2-x)Six compounds with x = 0.0-2.0 have been investigated in detail. Substitution of Ge with Si leads to a monotonic decrease of both a and c along with concomitant contraction of the unit cell volume and significant modifications of the magnetic states - a crossover from ferromagnetism at room temperature for Ge-rich compounds to antiferromagnetism for Si-rich compounds. The magnetic phase diagram has been constructed over the full range of CeMn2Ge(2-x)Six compositions and co-existence of ferromagnetism and antiferromagnetism has been observed in CeMn2Ge1.2Si0.8, CeMn2Ge1.0Si1.0 and CeMn2Ge0.8Si1.2 with novel insight provided by high resolution neutron and X-ray synchrotron radiation studies. CeMn2Ge(2-x)Six compounds (x = 0, 0.4 and 0.8) exhibit moderate isothermal magnetic entropy accompanied with a second-order phase transition around room temperature. Analysis of critical behaviour in the vicinity of TC(inter) for CeMn2Ge2 compound indicates behaviour consistent with three-dimensional Heisenberg model predictions.