This transition also leads to promising applications such as electronic homojunction and photonic memory devices, as well as catalytic energy materials ( 16– 18). In particular, most transition metal dichalcogenides exhibit the polymorphic phase transition that opens up access to diverse properties, including superconducting and topological states ( 15). The temperature-, pressure-, and electrostatic doping–induced structural phase transitions have been a core subject for exploring a novel crystal structure and switching material properties of 2D materials ( 12– 14).

In the context of a new material discovery, the transformation of a crystal structure has been widely recognized as a key factor ( 10, 11). This dimensional manipulation of a crystal structure thus provides a rational design strategy to search for new 2D layered materials in various compounds, enabling unlimited expansion of 2D libraries and corresponding physical properties. The bidimensional polymorphism is a previously unobserved phenomenon at ambient pressure in Zintl families and can be a common feature of transition metal pnictides. Using structural analysis combined with theoretical calculation, it is found that the 2D-ZnSb has a stable and robust layered structure. Here, through the dimensional manipulation of a crystal structure from sp 3-hybridized 3D-ZnSb, we create an unprecedented layered structure of Zintl phase, which is constructed by the staking of sp 2-hybridized honeycomb ZnSb layers.

However, it has been challenging to artificially develop layered materials with honeycomb atomic lattice structure composed of multicomponents such as hexagonal boron nitride. The discovery of new families, beyond graphene, of two-dimensional (2D) layered materials has always attracted great attention.

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