Figure 1.

a) The selected vibration modes calculated for the model clusters 3′′ (neutral) and 3* (dication without the 3c–2e HOMO) with the corresponding Raman scattering activities in brackets in units A⁴AMU⁻¹ (atoms outside the Th₃Cl₆ cage were excluded). b) Critical points from the analysis of the electron density calculated for the model cluster 3′′ (left and right columns depict top and side view of the Th₃Cl₆ fragment, respectively). c) The linearized side‐view of two orbital conjugation topologies in which the overlap of the 6d (Th) and 3p (Cl) atomic orbitals in the Th₃Cl₆ cage is particularly effective; below the resonance Lewis structures that rationalize the delocalized (“resonating”) nature of the thorium‐chlorine bonding in the Th₃Cl₆ cage in 3′′. d) Isosurfaces (at 0.003e) and the corresponding electron populations of the EDDB function calculated for the Th₃Cl₆ cage (ignoring the metal–metal interactions) and the Th₃ subunit in 3′′ (K atoms were excluded).