Flat-on ambipolar triphenylamine/C₆₀ nano-stacks formed from the self-organization of a pyramid-sphere-shaped amphiphile

A giant amphiphile, which is constructed with an amorphous nano-pyramid (triphenylamine, TPA) and a crystalline nano-sphere (C₆₀), was synthesized. Structural characterization indicates that this pyramid-sphere-shaped amphiphile (TPA-C₆₀) forms a solvent-induced ordered phase, in which the two constituent units self-assemble into alternating stacks of two-dimensional (2D) TPA and C₆₀ nano-sheets. Due to the complexity of the molecular structure and the amorphous nature of the nano-pyramid, phase formation was driven by intermolecular C₆₀-C₆₀ interactions and the ordered phase could not be reformed from the TPA-C₆₀ melt. Oriented crystal arrays of TPA-C₆₀, which contain flat-on TPA/C₆₀ nano-stacks, can be obtained via a PDMS-assisted crystallization (PAC) technique. The flat-on dual-channel supramolecular structure of TPA-C₆₀ delivered ambipolar and balanced charge-transport characteristics with an average μ_e of 2.11 × 10^-4 cm² V^-1 s^-1 and μ_h of 3.37 × 10^-4 cm² V^-1 s^-1. The anisotropic charge-transport ability of the pyramid-sphere-shaped amphiphile was further understood based on the lattice structure and the lattice orientation of TPA-C₆₀ revealed from electron diffraction analyses.