Superconductivity in an Orbital-Reoriented SnAs Square Lattice: A Case Study of Li_0.6Sn₂As₂ and NaSnAs

Searching for functional square lattices in layered superconductor systems offers an explicit clue to modify the electron behavior and find exotic properties. The trigonal SnAs₃ structural units in SnAs-based systems are relatively conformable to distortion, which provides the possibility to achieve structurally topological transformation and higher superconducting transition temperatures. In the present work, the functional As square lattice was realized and activated in Li_0.6Sn₂As₂ and NaSnAs through a topotactic structural transformation of trigonal SnAs₃ to square SnAs₄ under pressure, resulting in a record-high T_c among all synthesized SnAs-based compounds. Meanwhile, the conductive channel transfers from the out-of-plane p_z orbital to the in-plane p_x+p_y orbitals, facilitating electron hopping within the square 2D lattice and boosting the superconductivity. The reorientation of p-orbital following a directed local structure transformation provides an effective strategy to modify layered superconducting systems.