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Here, we manipulate the type and degree of solvation in this system and find that either a one\u2010 or two\u2010step spin transition can be specifically targeted. The chloroform clathrate <jats:bold>1\u22c5<\/jats:bold>4\u2009CHCl<jats:sub>3<\/jats:sub> undergoes a relatively abrupt one\u2010step SCO, in which the two equivalent Fe<jats:sup>II<\/jats:sup> sites within the dinuclear molecule crossover simultaneously. Partial desolvation of <jats:bold>1\u22c5<\/jats:bold>4\u2009CHCl<jats:sub>3<\/jats:sub> to form <jats:bold>1\u22c5<\/jats:bold>3\u2009CHCl<jats:sub>3<\/jats:sub> and <jats:bold>1\u22c5<\/jats:bold>CHCl<jats:sub>3<\/jats:sub> occurs through single\u2010crystal\u2010to\u2010single\u2010crystal processes (monoclinic <jats:italic>C<\/jats:italic>2\/<jats:italic>c<\/jats:italic> to <jats:italic>P<\/jats:italic>2<jats:sub>1<\/jats:sub>\/<jats:italic>n<\/jats:italic> to <jats:italic>P<\/jats:italic>2<jats:sub>1<\/jats:sub>\/<jats:italic>n<\/jats:italic>) in which the two equivalent Fe<jats:sup>II<\/jats:sup> sites become inequivalent sites within the dinuclear molecule of each phase. Both <jats:bold>1\u22c5<\/jats:bold>3\u2009CHCl<jats:sub>3<\/jats:sub> and <jats:bold>1\u22c5<\/jats:bold>CHCl<jats:sub>3<\/jats:sub> undergo one\u2010step spin transitions, with the former having a significantly higher SCO temperature than <jats:bold>1\u22c5<\/jats:bold>4\u2009CHCl<jats:sub>3<\/jats:sub> and the latter, and each has a broader SCO transition than <jats:bold>1\u22c5<\/jats:bold>4\u2009CHCl<jats:sub>3<\/jats:sub>, attributable to the overlap of two SCO steps in each case. Further magnetic manipulation can be carried out on these materials through reversibly resolvating the partially desolvated material with chloroform to produce the original one\u2010step SCO, or with dichloromethane to produce a two\u2010step SCO reminiscent of that seen for <jats:bold>1\u22c5<\/jats:bold>4\u2009CH<jats:sub>2<\/jats:sub>Cl<jats:sub>2<\/jats:sub>. Furthermore, we investigate the light\u2010induced excited spin state trapping (LIESST) effect on <jats:bold>1\u22c5<\/jats:bold>4\u2009CH<jats:sub>2<\/jats:sub>Cl<jats:sub>2<\/jats:sub> and <jats:bold>1\u22c5<\/jats:bold>CH<jats:sub>2<\/jats:sub>Cl<jats:sub>2<\/jats:sub> and observe partial LIESST activity for the former and no activity for the latter.<\/jats:p>","DOI":"10.1002\/chem.200901809","type":"journal-article","created":{"date-parts":[[2009,12,22]],"date-time":"2009-12-22T03:08:16Z","timestamp":1261451296000},"page":"1973-1982","source":"Crossref","is-referenced-by-count":48,"title":["Thermal\u2010 and Light\u2010Induced Spin Crossover in a Guest\u2010Dependent Dinuclear Iron(II) 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