Inspecting the electronic architecture and semiconducting properties of a rosette-like supramolecular columnar liquid crystal

Computational and experimental studies unravel the structural and electronic properties of a novel supramolecular liquid crystal built through a hierarchical assembly process resulting in an H‐bonded melamine rosette decorated with peripheral triphenylenes. The six‐fold symmetry of the mesogen facilitates the formation of a highly organized hexagonal columnar mesophase stable at room temperature. X‐ray diffraction and electron density maps confirm additional intra‐ and intercolumn segregation of functional subunits, and this paves the way for 1D charge transport. Indeed, hole mobility has been measured and found to be higher than for related mesogens. DFT calculations of HOMO and LUMO levels and parameters such as reorganization energy and transfer integral of the rosette structure have been achieved, and not only validate the columnar organization but also establish the way it translates into a favorable electronic architecture and molecular orbital interactions to promote charge carrier mobility.This work was financially supported by the MINECO‐FEDER funds (projects MAT2015‐66208‐C3‐1‐P, CTQ2015‐70174‐P), the Gobierno de Aragón‐FSE (E47_17R and B.F. grant B084/13), the Consejería de Economía y Conocimiento, Junta de Andalucía (FQM‐337), and the Universidad de Jaén (Acción 1_PIUJA 2017‐18). A.G. thanks support from the ELIOTROPO project (PON03PE_00092_2). R.T. was supported by the MERAVIGLIE project (CUP J28C17000080006).Peer reviewe