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The crystal structures of [CrLnL<jats:sub>3<\/jats:sub>](CF<jats:sub>3<\/jats:sub>SO<jats:sub>3<\/jats:sub>)<jats:sub>6<\/jats:sub> (Ln=Nd, Eu, Yb, Lu) and [RuLnL<jats:sub>3<\/jats:sub>](CF<jats:sub>3<\/jats:sub>SO<jats:sub>3<\/jats:sub>)<jats:sub>5<\/jats:sub> (Ln=Eu, Lu) demonstrate that the helical structure can accommodate metal ions of different sizes, without sizeable change in the intermetallic M\u22c5\u22c5\u22c5Ln distances. These systems are ideally suited for unravelling the molecular factors affecting the intermetallic <jats:italic>n<\/jats:italic>d\u21924f communication. Visible irradiation of the Cr<jats:sup>III<\/jats:sup>N<jats:sub>6<\/jats:sub> and Ru<jats:sup>II<\/jats:sup>N<jats:sub>6<\/jats:sub> chromophores in <jats:italic>HHH<\/jats:italic>\u2010[MLnL<jats:sub>3<\/jats:sub>]<jats:sup>5\/6+<\/jats:sup> (Ln=Nd, Yb, Er; M=Cr, Ru) eventually produces lanthanide\u2010based near infrared (NIR) emission, after directional energy migration within the complexes. Depending on the kinetic regime associated with each specific d\u2013f pair, the NIR luminescence decay times can be tuned from micro\u2010 to milliseconds. The origin of this effect, together with its rational control for programming optical functions in discrete heterobimetallic entities, are discussed.<\/jats:p>","DOI":"10.1002\/chem.200401158","type":"journal-article","created":{"date-parts":[[2005,3,18]],"date-time":"2005-03-18T10:01:36Z","timestamp":1111140096000},"page":"3228-3242","source":"Crossref","is-referenced-by-count":186,"title":["Tuning the Decay Time of Lanthanide\u2010Based Near Infrared Luminescence from Micro\u2010 to Milliseconds through d\u2192f Energy Transfer in Discrete Heterobimetallic 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