Looking at the electronic structure, the DFT one-electron eigenvalues either increase, decrease or remain constant when going from 0 to 60 , depending on whether the interaction across the bond connecting the phenyl rings is bonding, anti-bonding or non-bonding. The highest occupied molecular orbital (HOMO, see Figure ) increases in energy when the angle goes towards 0 , while the lowest unoccupied molecular orbital (LUMO, see Figure ) decreases in energy, and the HOMO-LUMO gap at 0 is thus 0.17 eV smaller than at the optimum angle for the neutral molecule (0.30 eV with PBE0). Since the highest occupied and lowest unoccupied crystalline orbitals in UiO-67 primarily consist of the HOMO and LUMO of the isolated linkers (c.f. Figure