*2.4. Computational Details*

The single point calculations based on the experimental X-ray geometry of (**ASZ**)3·(**1,4-FIB**)<sup>4</sup> have been carried out at the DFT level of theory using the dispersion-corrected hybrid functional ωB97XD [26] with the help of the Gaussian-09 [27] program package. The Douglas–Kroll–Hess 2nd order scalar relativistic calculations requested relativistic core Hamiltonian were carried out using the DZP-DKH basis sets [28–31] for all atoms. The topological analysis of the electron density distribution with the help of the atoms in molecules (QTAIM) method developed by Bader [32] has been performed by using the Multiwfn program [33]. The Cartesian atomic coordinates of a model supramolecular cluster are presented in Supporting Information, Table S4.
