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Compounds <jats:bold>1<\/jats:bold> and <jats:bold>2<\/jats:bold> are isostructural with a crystal structure characterized by segregated chains of side\u2010by\u2010side donor dimers and acceptors, and compound <jats:bold>3<\/jats:bold> presents donors in dimerized stacks. In spite of the different structural types and stoichiometries, all of these compounds have C\u2013N<jats:bold>\u00b7\u00b7\u00b7<\/jats:bold>H pairing interactions associated with R<jats:sup>2<\/jats:sup><jats:sub>2<\/jats:sub>(10) synthons between donors in nearby chains. All compounds are poor semiconductors, and the magnetic susceptibility of <jats:bold>1<\/jats:bold> is dominated by the contribution of the paramagnetic [Ni(mnt)<jats:sub>2<\/jats:sub>] anions with small antiferromagnetic interactions. The magnetic susceptibility of <jats:bold>3<\/jats:bold> is dominated by the paramagnetic FeBr<jats:sub>4<\/jats:sub> anions and follows a Curie\u2013Weiss law with a Weiss temperature <jats:italic>\u03b8<\/jats:italic> = \u201319 K, which denotes significant antiferromagnetic interactions that are most likely mediated by the donors.<\/jats:p>","DOI":"10.1002\/ejic.201501343","type":"journal-article","created":{"date-parts":[[2016,2,16]],"date-time":"2016-02-16T06:27:23Z","timestamp":1455604043000},"page":"1287-1292","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":10,"title":["Charge\u2010Transfer Salts Based on a Dissymmetrical Cyano\u2010Substituted Tetrathiafulvalene Donor"],"prefix":"10.1002","volume":"2016","author":[{"given":"Sandrina","family":"Oliveira","sequence":"first","affiliation":[]},{"given":"Isabel C.","family":"Santos","sequence":"additional","affiliation":[]},{"given":"Elsa B.","family":"Lopes","sequence":"additional","affiliation":[]},{"given":"Joana T.","family":"Coutinho","sequence":"additional","affiliation":[]},{"given":"Laura C. 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