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Abstract
The experimental realization of actinide-actinide bonding in isolable molecules has been one of the main targets of synthetic actinide chemistry for decades. Very recently, Boronski et al. reported the first thorium-thorium bonding in a crystalline cluster (3) prepared and isolated under normal experimental conditions. The electron spin resonance and the superconducting quantum-interference device magnetometry revealed a diamagnetic ground-state with two electrons equally distributed over the tri-thorium ring at the heart of 3, and the recorded Raman spectrum allegedly confirmed the existence of a three-center two-electron (3c-2e) bond. However, the observed broad inelastic scattering bands between 60 and 135 cm-1, originally assigned by the authors to thorium-thorium vibrations, represent in fact the combination of thorium-chlorine stretching modes, and they establish the existence of a unique charge-shift actinide-halogen bonding rather than the σ-aromatic (delocalized) actinide-actinide bonding as claimed in the original article.
