Abstract

The pentacyanidonitrosylmetalate [M(CN)5(NO)] (M = metal ion) is an attractive building block for bimetal assemblies exhibiting a long‐range magnetic ordering. In this work, a cyanido‐bridged bimetal assembly based on a pentacyanidonitrosylmolybdate, Cs1.26Mn0.87[Mo(CN)5(NO)]·0.6H2O, was prepared. This compound has a noncentrosymmetric cubic crystal structure in the F43m space group and a lattice constant of 10.8970(3) Å. It exhibits ferrimagnetism with a Curie temperature (TC) of 65 K due to the antiparallel ordering of the MnII (S = 5/2) and MoI (S = 1/2) magnetic spins. Owing to the piezoelectric crystal structure, this compound exhibits second harmonic generation (SHG) and magnetization‐induced second harmonic generation (MSHG).

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