Computational Methods. Periodic Density Functional Theory (DFT) calculations were performed on the solid-state structures of the three hybrid inorganic-organic complexes within the Vienna Ab Initio Simulation Package (VASP). The projector augmented wave method was used to describe the interactions between core and valence electrons, and using scalar-relativistic pseudopotentials for all atoms. The Bi 5d electrons were included in the valence set. Due to the size and complexity of the crystal structures of the three compounds, GGA DFT was used for geometric relaxation -the Perdew, Burke and Ernzerhof (PBE) functional with the addition of Grimme's D3 (PBE+D3) correction as well was the revised PBE functional for solids (PBEsol) used for this purpose due to their prior success in describing the crystal structures of extended organic-inorganic complexes. As semiconductor band gaps are severely underestimated in GGA DFT, the hybrid DFT functional HSE06 was used for the calculation of the electronic structures of the three systems. Spin-orbit coupling was additionally included to evaluate the relativistic renormalization of the band structure in each case (HSE06+SOC).