C$_{60}$ building blocks with tuneable structures for tailored functionalities

Abstract

We show that C$_{60}$ fullerene molecules can serve as promising building blocks in the construction of versatile crystal structures with unique symmetries using first-principles calculations. These phases include quasi-2D layered structures and 3D van der Waals crystals where the molecules adopt varied orientations. The interplay of molecular arrangement and lattice symmetry results in a variety of tuneable crystal structures with distinct properties. Specifically, the electronic structures of these phases vary significantly, offering potential for fine-tuning the band gap for electronics and optoelectronics. Additionally, the optical properties of these materials are strongly influenced by their crystalline symmetry and molecular alignment, providing avenues for tailoring optical responses for photonics. Our findings highlight the potential of fullerene-based building blocks in the rational design of functional materials.