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In [K(18\u2010crown\u20106)][Ni(\u03b1\u2010tpdt)<jats:sub>2<\/jats:sub>], the anion has a square planar coordination geometry with ligand disorder and the cations and anions are segregated in alternating layers in the crystal structure, as was found in the previous [Ni(\u03b1\u2010tpdt)<jats:sub>2<\/jats:sub>]<jats:sup>\u2013<\/jats:sup> salts. Two salts were obtained with the [K(15\u2010crown\u20105)<jats:sub>2<\/jats:sub>]<jats:sup>+<\/jats:sup> cation. The expected 1:1 salt was obtained, which had the usual anion square planar coordination geometry for [Ni(\u03b1\u2010tpdt)<jats:sub>2<\/jats:sub>]<jats:sup>\u2013<\/jats:sup> but that had a new molecular arrangement based on an anion double chain. In addition, a 2:1 salt was obtained, which had a new anionic geometry, namely, [Ni<jats:sub>4<\/jats:sub>(\u03b1\u2010tpdt)<jats:sub>6<\/jats:sub>]<jats:sup>2\u2013<\/jats:sup>, which is an unprecedented example of an in\u2010line mixed\u2010valence Ni<jats:sub>4<\/jats:sub> dithiolene (Ni<jats:sub>4<\/jats:sub>\u2013S<jats:sub>12<\/jats:sub>) cluster. A compound with an eight\u2010membered tetrasulfide ring, namely a bis(thiophene\u20102,3\u2010diyl) bis(sulfide), was also obtained. The salts that are based on the paramagnetic [Ni(\u03b1\u2010tpdt)<jats:sub>2<\/jats:sub>]<jats:sup>\u2013<\/jats:sup> anion presented interesting magnetic properties that resulted from the competition between the antiferromagnetic (AFM) and ferromagnetic (FM) interactions with a low\u2010temperature cluster glass behaviour, which was associated with the <jats:italic>cis<\/jats:italic>\u2010<jats:italic>trans<\/jats:italic> ligand disorder.<\/jats:p>","DOI":"10.1002\/ejic.201100797","type":"journal-article","created":{"date-parts":[[2011,9,15]],"date-time":"2011-09-15T11:42:28Z","timestamp":1316086948000},"page":"4807-4815","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":12,"title":["Ni\u20102,3\u2010thiophenedithiolate Anions in New Architectures: An In\u2010Line Mixed\u2010Valence Ni Dithiolene (Ni<sub>4<\/sub>\u2013S<sub>12<\/sub>) Cluster"],"prefix":"10.1002","volume":"2011","author":[{"given":"Ana I. 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