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This study focuses on the synthesis and study of 2,3,7,8,12,13,17,18\u2010octaethylporphyrin (OEP)\u2013Tb\n                    <jats:sup>III<\/jats:sup>\n                    double\u2010decker complexes with different electronic structures comprising protonated, anionic, and radical forms. Magnetic susceptibility measurements revealed that only the anionic and radical forms of the OEP\u2013Tb\n                    <jats:sup>III<\/jats:sup>\n                    double\u2010decker complexes exhibited SMM properties. The barrier heights for magnetic moment reversal were estimated to be 207 and 215\u2005cm\n                    <jats:sup>\u22121<\/jats:sup>\n                    for the anionic and radical forms, respectively. Scanning tunneling microscopy (STM) investigations revealed that these OEP\u2013Tb\n                    <jats:sup>III<\/jats:sup>\n                    complexes form well\u2010ordered monolayers upon simple dropcasting from dilute dichloromethane solutions. All three complexes form an isomorphic pseudo\u2010hexagonal 2D pattern, regardless of the differences in the electronic structures of their porphyrin\u2013Tb cores. This finding is of interest for SMM technology as ultrathin films of these materials undergoing chemical transformations will not require any detrimental reorganization. Finally, we demonstrate self\u2010assembly of the protonated 5,15\u2010bisdodecylporphyrin (BDP)\u2013Tb\n                    <jats:sup>III<\/jats:sup>\n                    double\u2010decker complex as an example of successful supramolecular design to achieve controlled alignment of SMM\u2010active sites.\n                  <\/jats:p>","DOI":"10.1002\/chem.201402669","type":"journal-article","created":{"date-parts":[[2014,7,7]],"date-time":"2014-07-07T12:59:27Z","timestamp":1404737967000},"page":"11362-11369","source":"Crossref","is-referenced-by-count":31,"title":["Switching of Single\u2010Molecule Magnetic Properties of Tb\n                    <sup>III<\/sup>\n                    \u2013Porphyrin Double\u2010Decker Complexes and Observation of Their Supramolecular Structures on a Carbon 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