We present the results of magnetization and AC susceptibility measurements performed on ferrimagnetic Mn(3)(2+)[Cr(III)(CN)(6)](2)·12H(2)O and ferromagnetic Ni(3)(2+)[Cr(III)(CN)(6)](2)·12H(2)O systems under pressures up to 0.9 GPa in a commercial SQUID magnetometer. The magnetization process is affected by pressure: magnetization saturates at higher magnetic field, saturated magnetization μ(s) of Ni(3)[Cr(CN)(6)](2) is reduced and almost unaffected for Mn(3)[Cr(CN)(6)](2) at low temperatures. The Curie temperature T(C) of Mn(3)[Cr(CN)(6)](2) increases with the applied pressure, ΔT(C)/Δp = 25.5 K GPa(-1), due to a strengthened super-exchange antiferromagnetic interaction J(AF), but it is not affected significantly in the case of Ni(3)[Cr(CN)(6)](2) with a dominant ferromagnetic J(F) super-exchange interaction. The increase in the J(AF) interaction is attributed to the enhanced value of the single electron overlapping integral S and the energy gap Δ of the mixed molecular orbitals t(2g) (Mn(2+)) and t(2g) (Cr(III)) induced by pressure.

In the present study we report the structural and magnetic response of the 3-D cyano-bridged magnetic sponge-like system {[Mn^II(pydz)(H₂O)₂][Mn^II(H₂O)₂][Nb^IV(CN)₈]·3H₂O}_nA to external pressure up to 1.8 GPa using single-crystal crystallography and magnetic measurements. The observed pressure-induced structural changes: shrinkage of the Nb–C bonds and bending of Mn–NC–Nb linkages are responsible for the strengthening of the antiferromagnetic interactions between Mn and Nb centers and consequently for the substantial increase of the magnetic ordering temperature from 43 K to 51 K under 0.57 GPa. The observed magneto-structural response to external pressure is similar in nature to the removal of guest molecules and confirms the significant susceptibility of molecular magnetic sponges to mechanical stress.