Abstract
The crystal structures of Cs2Na[Fe(CN)6](I) and Cs2K[Fe(CN)6](II) have been elucidated by single-crystal X-ray analysis and compared with that of Cs2Li[Fe(CN)6]. Crystals of both are monoclinic, space group P21/n, with Z= 2 in unit cells of dimensions: (I), a= 10.870(1), b= 7.709(1), c= 7.573(1)Å, β= 89.994(6)°: (II), a= 11.140(1), b= 8.131(1), c= 7.660(1)Å, β= 90.165(7)°. The Mössbauer spectra of the series are discussed with particular reference to lattice dynamics, and to electronic spin-relaxation of the t2g 5 S =½ configuration.

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