Polytypic Two-Dimensional FeAs with High Anisotropy.

In the realm of two-dimensional (2D) crystal growth, the chemical composition often determines the thermodynamically favored crystallographic structures. This relationship poses a challenge in synthesizing novel 2D crystals without altering their chemical elements, resulting in the rarity of achieving specific crystallographic symmetries or lattice parameters. We present 2D polymorphic FeAs crystals that completely differ from bulk orthorhombic FeAs ( Pnma ), differing in the stacking sequence, i.e., polytypes. Preparing polytypic FeAs outlines a strategy for independently controlling each symmetry operator, which includes the mirror plane for 2 Q -FeAs ( I 4/ mmm ) and the glide plane for 1 Q -FeAs ( P 4/ nmm ). As such, compared to bulk FeAs, polytypic 2D FeAs shows highly anisotropic properties such as electrical conductivity, Young's modulus, and friction coefficient. This work represents a concept of expanding 2D crystal libraries with a given chemical composition but various crystal symmetries.