The geometric structures of 3 and 4 were determined using SCXRD (refinement details are provided in Table and). Detailed structural analyses of 2-4 revealed that 3 and 4 had similar structures (Figures and), both of which were significantly different from 2. Specifically, all three possessed a 13 atom Au12Pt icosahedral core protected by Au-thiolate staple moieties. However, the size and orientation of these staples varied (Figure ). As an example, 2 had a total of six SR-Au-SR-Au-SR staples wrapped around its 13-atom icosahedral core. In contrast, 3 and 4 had two such staples joined by a dithiolate (TDT and PDT, respectively) to form a new, longer staple: S(R)-Au-S(R)-Au-S-CH2-(S or CH2)-CH2-S-Au-S(R)-Au-S(R) (where R = 4-t BuPh-). A total of three such staples were formed by three dithiolates (TDT or PDT).