Thermal Property of Fullerene Fibers: One‐Dimensional Material with Exceptional Thermal Performance

The recent groundbreaking achievement in the synthesis of large‐sized single crystal C60 monolayer, which is covalently bonded in a plane using C60 as building blocks. The asymmetric lattice structure endows it with anisotropic phonon modes and conductivity. If these C60 are arranged in form of 1D fiber, the improved manipulation of phonon conduction along the fiber axis could be anticipated. Here, thermal properties of C60‐fiber, including thermal transfer along the C60‐fiber axis and across the interlayer interface are investigated using molecular dynamic simulations. Taking advantage of the distinctively hollow spherical structure of C60 building blocks, the spherical structure deformation and encapsulation induced thermal reduction can be up to 56% and 80%, respectively. By applying external electronic fields in H2O@C60 model, its thermal conductivity decreases up to 60%, which realizes the contactless thermal regulation. ln particular, the thermal rectification phenomenon is discovered by inserting atoms/molecules in C60 with a rational designed mass‐gradient, and its maximum thermal rectification factor is predicted to ≈45%. These investigations aim to achieve effective regulation of the thermal conductivity of C60‐fibers. This work showcases the potential of C60‐fiber in the realms of thermal management and thermal sensing, paving the way to C60‐based functional materials. Drawing inspiration from the unique hollow structure of C60, various techniques for thermal regulation of endohedral C60 are explored. These techniques include strain engineering, mass‐gradient, and external electronic fields. The objective is to identify an effective approach for modulating the thermal conductivity of C60‐fibers. The results highlight the promising potential of C60‐fibers in the field of thermal management.