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The layered fluoride Cs 2 AgF 4  has been found to undergo a ferromagnetic-like phase transition below  T  C  ≈ 14.5 K leading to magnetic saturation already at very low magnetic fields ( H  ≥ 10 kOe). We have explored the nature of this phase transition by studying the magnetization and specific heat under magnetic field and by evaluating the spin exchange interactions of Cs 2 AgF 4  on the basis of density functional calculations as well as the magnetic dipole-dipole interaction energies for several ordered spin arrangements of Cs 2 AgF 4 . The magnetization exhibits an almost rectangular behavior with a small hysteresis indicating Cs 2 AgF 4  to be a very soft ferromagnet with a coercitive field of  H  ≤ 20 Oe. The magnetization saturates at a value of ∼0.9  μ  B , in good agreement with the 4d 9  configuration and a  S  = ½ ground state of Ag 2+ . Without applied external magnetic field ( H  = 0 Oe) the specific heat  C p   exhibits an anomaly at  T  C  that deviates considerably from a  λ -type anomaly. When  H  is increased from 0, the  C p   anomaly is smeared out without shifting its position, and eventually disappears for  H  &gt; 200 Oe. This observation is ascribed to the presence of weak magnetic dipole-dipole inter-layer interactions which favor a weak antiferromagnetic coupling and just outweigh weak ferromagnetic inter-layer spin exchange interaction found from the density functional calculations.

The layered ferromagnet Cs 2 AgF 4 : Antiferromagnetic inter-layer coupling driven by magnetic dipole-dipole interactions