| Summary: | An Ag(I)formamidine cluster Ag<sub>6</sub><b>L1</b><sub>6</sub> (<b>1)</b> and an Ag(I)formamidine coordination polymer Ag<sub>7</sub>(<b>L2</b>)<sub><b>2</b></sub> <b>2</b> (<b>L1</b> = <i>N</i>,<i>N</i>′-bis(2,6-disopropylphenyl) formamidine dithiocarbamate and <b>L2</b> = <i>N</i>,<i>N</i>′-mesityl formamidine dithiocarbamate) have been synthesized from the reactions of <b>L1</b> and <b>L2</b> with AgNO<sub>3</sub> respectively. The complexes were characterized using spectroscopic and analytical methods, including single-crystal X-ray diffraction. In the structure of <b>1</b>, a six vertex distorted square bi-pyramidal octahedron is formed from an Ag<sub>6</sub> core. The <i>N</i>,<i>N</i>′-bis(2,6-disopropylphenyl) formamidine dithiocarbamate ligands stabilize this core through two main –CS<sub>2</sub> bridging modes giving a propeller like structure. In the structure of <b>2</b>, each of the two Ag(I) centers are bridged by two <i>N</i>,<i>N</i>′-mesityl formamidine dithiocarbamate ligands forming 8-member Ag<sub>2</sub>(CS<sub>2</sub>)<sub>2</sub> metallacycles with an inversion center in the middle of the Ag—Ag argentophilic bond. The metallacycles are connected through Ag—S bonds forming ribbons in the crystallographic <i>a</i>-axis. The Ag(I) centers are coordinated to two <i>N</i>,<i>N</i>′-mesitylformamidine dithiocarbamates through the dithiocarbamate S atoms. The thermal decomposition of complexes <b>1</b> and <b>2</b> had similar thermograms with one major weight loss activity and the formation of elemental silver particles thereafter.
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