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The hybrids of M(en) 3 Ag 2 I 4 (M = Zn or Ni) are isostructural to each other and crystallize in space group P 6 3 22 with quite similar lattice parameters. The hybrid solid solutions Zn α Ni 1-α (en) 3 Ag 2 I 4 (0 &lt; α &lt; 1) have been prepared via self-assembly in the mixed N , N -dimethylformamide solution of AgNO 3 , KI, and ethylenediamine, meanwhile, with certain relative amount of [Zn(en) 3 ] 2+ and [Ni(en) 3 ] 2+ ions at ambient condition. All hybrid solid solutions are isostructural to the parent hybrids M(en) 3 Ag 2 I 4 (M = Zn or Ni). The UV-vis-near IR diffuse reflection spectra in solid state, thermogravimetric analysis, variable-temperature magnetic susceptibility, and dielectrics have been investigated for Zn α Ni 1-α (en) 3 Ag 2 I 4 (0 &lt; α &lt; 1). The intensity of bands centered at 540 and 860 nm in UV-vis-near IR spectra, arising from the d-d electron transition in Ni 2+ ion, as well as the Curie constant decreases linearly with the molar fraction of Zn (α)/Ni (1 - α), whereas the c -axis length, the C-N and C-C bond lengths in the ethylenediamine, the frequency-independent dielectric permittivity and the onset temperature of dielectric relaxation, and so forth show nonmonotonical alternation with the fraction of Zn (α)/Ni (1 - α) in the solid solution, and the origin for these differences is further discussed.

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Structural, Optical, Magnetic, and Dielectric Properties in Hybrid Solid Solutions of ZnαNi1−α(en)3Ag2I4 (0 &lt; α &lt; 1) by Varying the Relative Zn/Ni Content