Single pair of charge-two high-fold fermions in ultralight chiral crystals

The realization of single-pair chiral fermions in Weyl systems remains challenging in topology physics, especially for the systems with higher chiral charges $|C|$. In this work, based on the symmetry analysis and low-energy effective model, we propose that single-pair high-fold topological fermions with $C$ = $\pm{2}$ can be achieved in chiral space groups P2$_1$3, P4$_3$32, and P4$_1$32. Here, a single pair of Weyl points with the oppositely chiral charges of $|C| = 2$ has been proved by the minimal lattice model and shows the unique characteristics compared to multi-pair Weyl fermionic systems, including the larger nontrivial energy window and the ultralong double Fermi arcs extended to the whole Brillouin zone. Furthermore, we show the first ultralight chiral crystal P4$_3$32-type LiC$_2$ and its inversion enantiomer as high-quality candidate materials, whose Weyl nodes exhibit the large linear energy range to surmount the interruption of irrelevant bands, and we observe a reversal of their Fermi-arc velocities. Our work not only provides a promising platform for detecting ultralong chiral fermi arcs but also certainly leads to continued exploration of unconventional fermions.