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In spite of the different structural types of these compounds, the three compounds present donors in dimerized stacks. The crystal structures of <jats:bold>1<\/jats:bold> and <jats:bold>3<\/jats:bold> consist of segregated head\u2010to\u2010tail donor dimer stacks and dianion columns. The structural motif of <jats:bold>2<\/jats:bold> is mixed columns of alternating head\u2010to\u2010tail donor dimers and dianions. The three salts present C\u2013N<jats:bold>\u00b7\u00b7\u00b7<\/jats:bold>H\u2013C interactions, which in <jats:bold>2<\/jats:bold> and <jats:bold>3<\/jats:bold> can be described as a R<jats:sup>2<\/jats:sup><jats:sub>2<\/jats:sub>(10) synthon. The magnetic susceptibility of the salts with the paramagnetic (Cu<jats:sub>2<\/jats:sub>Cl<jats:sub>6<\/jats:sub>)<jats:sup>2\u2013<\/jats:sup> dianion (<jats:bold>1<\/jats:bold> and <jats:bold>2<\/jats:bold>) show that they behave as paramagnets where the Cu<jats:sup>2+<\/jats:sup> atoms of the dianion are antiferromagnetically coupled with magnetic exchange values <jats:italic>J\/k<\/jats:italic><jats:sub>B<\/jats:sub> of \u201358.8 and \u2013155.6 K, respectively. The different <jats:italic>J<\/jats:italic> values are associated with differences in dianion geometry.<\/jats:p>","DOI":"10.1002\/ejic.201900146","type":"journal-article","created":{"date-parts":[[2019,3,7]],"date-time":"2019-03-07T10:44:27Z","timestamp":1551955467000},"page":"1875-1883","update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Radical Cation Salts of Cyanobenzene\u2010Ethylenedithio\u2010TTF Electron Donors with Halide (Cu and Hg) Binuclear Anions"],"prefix":"10.1002","volume":"2019","author":[{"given":"Gon\u00e7alo","family":"Lopes","sequence":"first","affiliation":[{"name":"C<sup>2<\/sup>TN, Centro de Ci\u00eancias e Tecnologias Nucleares Instituto Superior T\u00e9cnico Universidade de Lisboa  E.N. 10 ao km 139,7 2695\u2010066 Bobadela LRS Portugal"}]},{"given":"Ana Cristina","family":"Gon\u00e7alves","sequence":"additional","affiliation":[{"name":"C<sup>2<\/sup>TN, Centro de Ci\u00eancias e Tecnologias Nucleares Instituto Superior T\u00e9cnico Universidade de Lisboa  E.N. 10 ao km 139,7 2695\u2010066 Bobadela LRS Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5741-3373","authenticated-orcid":false,"given":"Vasco","family":"da Gama","sequence":"additional","affiliation":[{"name":"C<sup>2<\/sup>TN, Centro de Ci\u00eancias e Tecnologias Nucleares Instituto Superior T\u00e9cnico Universidade de Lisboa  E.N. 10 ao km 139,7 2695\u2010066 Bobadela LRS Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5493-8158","authenticated-orcid":false,"given":"Dulce","family":"Sim\u00e3o","sequence":"additional","affiliation":[{"name":"Centro de Qu\u00edmica Estrutural Instituto Superior T\u00e9cnico Universidade de Lisboa  1049\u2010001 Lisboa Portugal"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8350-480X","authenticated-orcid":false,"given":"Isabel Cordeiro","family":"Santos","sequence":"additional","affiliation":[{"name":"C<sup>2<\/sup>TN, Centro de Ci\u00eancias e Tecnologias Nucleares Instituto Superior T\u00e9cnico Universidade de Lisboa  E.N. 10 ao km 139,7 2695\u2010066 Bobadela LRS Portugal"}]},{"given":"Laura C. 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