The molecular structure of TCS was taken from a previous X-ray diffraction study. In the crystal structure, the TCS hydroxyl groups simultaneously act as hydrogen bond donors and acceptors, resulting in one-dimensional chains of hydrogen-bonded TCS molecules. Moreover, the phenyl rings of neighboring molecules interact through π-π stacking interactions. Since it can be expected that the equilibrium molecular structure will be considerably different in the absence of intermolecular interactions, a conformational screening was carried out, using the Materials Studio (MS) Conformer module and the pcff force field 43 (see Electronic Supplementary Information [ESI], Table for pcff parameters). Local energy minima were re-optimized using DFT calculations with the CP2K code (see subsection on DFT calculations for further details). In the lowest-energy conformer identified on the basis of these calculations, the hydroxyl group forms an intramolecular hydrogen bond to the central oxygen atom Oc (Figure , 𝑟(H ••• O ) = 2.181 Å). A vibrational calculation confirmed the absence of imaginary frequencies. The DFT-calculated electrostatic potential (bottom panel of Figure ) shows the comparatively strong positive polarization of the Hh proton of the hydroxyl group, which exceeds that of other positively polarized areas of the molecule (aromatic protons). This TCS conformer was used as reference for the calculation of adsorption energies and as starting point for the generation of TCS@Zeo adsorption complexes.