In silico assessment of the color modulation in hybrid organic/inorganic columnar mesophases

We investigated the modulation of UV–Vis absorption features and perceived color in hybrid organic/inorganic columnar mesophases obtained by blending a metal-organic triphenylene metallomesogen with bipyridine or phenanthroline metal complexes. This blending results in complementary π-electron donor-acceptor interactions between triphenylene groups and metal-bipyridine/phenanthroline acceptor units through charge-transfer interactions. Our approach involved tuning the LUMO energy level of the acceptor molecule, covering a total of 140 acceptor molecules, by varying the metal (Pt or Pd), the aromatic nature of the ligand (bipyridine or phenanthroline) and the functionalization of the ligand with common electron-donor or electron-withdrawing functional groups. We employed a combined methodology based on extended tight-binding methods (xTB) and Time-Dependent Density Functional Theory (TD-DFT) to characterize UV–Vis absorption features and perceived color of hybrid organic/inorganic columnar mesophases as influenced by the chemical structure of the acceptor unit. • We present a strategy to modulate the color of hybrid organic/inorganic columnar mesophases through charge-transfer interactions. • UV–Vis absorption features and the color of these mesophases are fine-tuned through the molecular design of the acceptor units. • Quantum chemical methods allow efficient screening and rational design of liquid crystal materials. • This approach offers a cost- and time-efficient alternative to experimental methods.