Abstract

Abstract Magnetic properties and the specific heat of a series of new compounds, KV 1− x Cr x P 2 S 7 have been investigated. They are antiferromagnets with the Neel temperatures T N , determined from a specific heat, 19, 15 and 17 K for x =0, 0.75 and 1.0, respectively. The magnetic susceptibility shows a broad peak at T p above T N , 26, 18 and 20 K for x =0, 0.75 and 1.0, respectively. The easy magnetization axis is parallel to the c * -axis for x =0 and 0.75, while it is perpendicular to the c * -axis for x =1.0. The effective magnetic moment μ eff is about 1.8 μ B for KVP 2 S 7 , which is smaller than the spin only value of V 3+ ion and cannot be explained by the simple crystalline electric field effects. On the other hand, μ eff is about 4.0 μ B , which almost corresponds to the spin only value of Cr 3+ ion for KCrP 2 S 7 . The magnetization curve at 2 K is not linear below 7 T for three compounds and a curious hysteresis is observed for KVP 2 S 7 . The another marked magnetic behavior of the present system is a very large diamagnetism χ dia ≈−10 −3 (emu/mol) for three compounds. Anomalous magnetic properties of the present system are considered to originate in the covalency of S–S and S–(V,Cr) bonds, the network of which may produce the large diamagnetism. The overlapping of the 3d orbitals of V and Cr ions with surrouding S 3p orbitals may affect the magnetic moment of these ions.

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