Antiferromagnetic Frustration Behavior with Face-Sharing CuAs4 Tetrahedrons in Conducting ACu6As3 (A = Li and Na).

New mixed-valence copper pnictides ACu6As3 (A = Li and Na) adopt a quasi-2D structure type, featuring alkalis and [Cu6As3]- slabs along the c-axis alternatively. The face-sharing connection between CuAs4 polyhedra leads to a higher valence state for the inside Cu ions than that of Cu ions with the other connectivity way. This is confirmed by X-ray photoemission spectroscopy results. The Cu2+ with near spin 1/2 located on bilayer triangular lattice is found to exhibit a peculiar hump in magnetic susceptibility along the c-axis and, most strikingly, nearly a constant at low temperatures from 1.8 K down to 0.4 K. Besides, high hole mobilities, 68.58 and 645.16 cm2 V-1 S-1, are observed in LiCu6As3 and NaCu6As3, respectively. These compounds provide a novel material system for researching the relationship among structure, valence state, and spin correlation in frustrated lattice.