To determine the influence these GBs have on the electronic properties of the solid electrolytes, we calculated the projected density of states (PDOS) using the hybrid-DFT functional HSE06 for each GB alongside a bulk-like region in the center of the grain. All of the considered GBs exhibit reduced band gaps in the vicinity of the boundary (Figure ), with the change in the Li 3 OCl Σ3{112} GB being very small. In general, this corresponds to states appearing above the valence band maximum (VBM), except for in the cases of the Li 3 OCl Σ5{310} and Li 3 InCl 6 Σ3{112} GBs, where there are significant contributions from states appearing below the conduction band minimum (CBM). Narrowed band gaps may also imply that the GBs contain charge traps in their equilibrium geometry. In order to visualize the band edges, we add an electron and create a hole in each system without optimizing the geometry; the spin density isosurfaces associated with each case show where charge will prefer to localize. Evidence of electron trapping is not especially prevalent; whilst the Li 3 InCl 6 Σ3{112} GB shows some localization of electrons around In sites that form part of the edge-sharing octahedra, the electron density in the Li 3 OCl Σ5{310} is sufficiently diffuse that it does not appear in the isosurface plots. Conversely, evidence of hole trapping is far more pronounced and, in all cases where states appear above the VBM, there are highly localized holes centered on the anions in the vicinity of the GB.