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To account for the charge transfer and covalent character in bonding between P and Bi centers, the electronic structures of [P(C 6 H 4 - o -CH 2 SCH 3 ) 3 BiCl  n  ] (3- n )+ ( n = 0-3) model species have been investigated computationally. On the basis of this survey a synthetic target compound with a dative P→Bi bond has been selected. Consecutively, the highly reactive bismuth cage [P(C 6 H 4 - o -CH 2 SCH 3 ) 3 Bi] 3+ has been accessed experimentally and characterized. Importantly, our experiments (single-crystal X-ray diffraction and solid-state NMR spectroscopy) and computations (NBO and AIM analysis) reveal that the P···Bi bonding in this trication can be described as a dative bond. Here we have shown that our accordion-like molecular framework allows for tuning of the interaction between P and Bi centers.

Tweaking the Charge Transfer: Bonding Analysis of Bismuth(III) Complexes with a Flexidentate Phosphane Ligand