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Similar reactions using LiHMDS led to the recrystallization of the starting materials. The crystal structures of <jats:bold>1<\/jats:bold>\u2013<jats:bold>4<\/jats:bold> reveal the formation of one\u2010dimensional chains composed of dimeric [{M(HMDS)}<jats:sub>2<\/jats:sub>] aggregates, which are bridged through neutral ferrocene molecules by \u03b7<jats:sup>5<\/jats:sup>\u2010cation\u2013\u03c0 interactions. In addition, compounds <jats:bold>3<\/jats:bold> and <jats:bold>4<\/jats:bold> also contain interchain agostic M\uf8ffC interactions, producing two\u2010dimensional 4<jats:sup>4<\/jats:sup>\u2010nets. Whereas <jats:bold>1<\/jats:bold> and <jats:bold>2<\/jats:bold> were prepared from toluene, the syntheses of <jats:bold>3<\/jats:bold> and <jats:bold>4<\/jats:bold> required the use of <jats:italic>tert\u2010<\/jats:italic>butylbenzene as the reaction media. The attempted crystallization of <jats:bold>3<\/jats:bold> and <jats:bold>4<\/jats:bold> from toluene resulted in formation of the mixed toluene\/ferrocene solvated complexes [{(Me<jats:sub>3<\/jats:sub>Si)<jats:sub>2<\/jats:sub>NM)<jats:sub>2<\/jats:sub>}<jats:sub>2<\/jats:sub><jats:bold>\u22c5<\/jats:bold> (Cp<jats:sub>2<\/jats:sub>Fe)<jats:sub><jats:italic>x<\/jats:italic><\/jats:sub><jats:bold>\u22c5<\/jats:bold>(Tol)<jats:sub><jats:italic>y<\/jats:italic><\/jats:sub>]<jats:sub>\u221e<\/jats:sub> (in which M=Rb, <jats:italic>x<\/jats:italic>=0.6, <jats:italic>y<\/jats:italic>=0.8, <jats:bold>5<\/jats:bold>; M=Cs, <jats:italic>x<\/jats:italic>=0.5, <jats:italic>y<\/jats:italic>=1, <jats:bold>6<\/jats:bold>). The extended solid\u2010state structures of <jats:bold>5<\/jats:bold> and <jats:bold>6<\/jats:bold> are closely related to the 4<jats:sup>4<\/jats:sup>\u2010sheets <jats:bold>3<\/jats:bold> and <jats:bold>4<\/jats:bold>, but are now assembled from a combination of cation\u2013\u03c0, agostic, and \u03c0\u2013\u03c0 interactions. The charge\u2010separated complex [K{(C<jats:sub>6<\/jats:sub>H<jats:sub>6<\/jats:sub>)<jats:sub>2<\/jats:sub>Cr}<jats:sub>1.5<\/jats:sub>(Mes)][Mg(HMDS)<jats:sub>3<\/jats:sub>] (<jats:bold>15<\/jats:bold>) was also structurally characterized and found to adopt an anionic two\u2010dimensional 6<jats:sup>3<\/jats:sup>\u2010network through doubly \u03b7<jats:sup>3<\/jats:sup>\u2010coordinated bis(benzene)chromium molecules. DFT calculations at the B3\u2009LYP\/6\u201331G* level of theory indicate that the binding energies of both ferrocene and toluene to the M(HMDS) dimers increases in the sequence Li&lt;Na&lt;K. This pattern is a consequence of the larger metals allowing more open coordination spheres to support cation\u2013\u03c0 contacts. By comparison, binding of the isolated metal cations to the aromatic groups follow the reverse order K&lt;Na&lt;Li. A combined analysis of theoretical and experimental data suggest that ferrocene is a stronger cation\u2013\u03c0 donor than toluene for the lighter metals, but that this difference is eliminated on descending the group.<\/jats:p>","DOI":"10.1002\/chem.200700219","type":"journal-article","created":{"date-parts":[[2007,4,23]],"date-time":"2007-04-23T11:54:39Z","timestamp":1177329279000},"page":"4418-4432","source":"Crossref","is-referenced-by-count":61,"title":["Organometallic Polymers Assembled from Cation\u2013\u03c0 Interactions: Use of Ferrocene as a Ditopic Linker Within the Homologous Series [{(Me<sub>3<\/sub>Si)<sub>2<\/sub>NM}<sub>2<\/sub>\u22c5(Cp<sub>2<\/sub>Fe)]<sub>\u221e<\/sub> (M=Na, K, Rb, Cs; 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