Semimetals with extremely large magnetoresistance have attracted significant interest because of their possible nontrivial electronic structures, unusual transport properties, and also deep connections to high-energy physics.

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The discovery of new families, beyond graphene, of two-dimensional (2D) layered materials has always attracted great attention. However, it has been challenging to artificially develop layered materials with honeycomb atomic lattice structure composed of multicomponents such as hexagonal boron nitride. Here, through the dimensional manipulation of a crystal structure from sp3-hybridized 3D-ZnSb, we create an unprecedented layered structure of Zintl phase, which is constructed by the staking of sp2-hybridized honeycomb ZnSb layers. Using structural analysis combined with theoretical calculation, it is found that the 2D-ZnSb has a stable and robust layered structure. The bidimensional polymorphism is a previously unobserved phenomenon at ambient pressure in Zintl families and can be a common feature of transition metal pnictides. 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.

Topological Dirac semimetals have emerged as a platform to engineer Berry curvature with time-reversal symmetry breaking, which allows to access diverse quantum states in a single material system. It is of interest to realize such diversity in Dirac semimetals that provides insight on correlation between Berry curvature and quantum transport phenomena. Here, we report the transition between anomalous Hall and chiral fermion states in three-dimensional topological Dirac semimetal KZnBi, which is demonstrated by tuning the direction and flux of Berry curvature. Angle-dependent magneto-transport measurements show that both anomalous Hall resistance and positive magnetoresistance are maximized at 0° between net Berry curvature and rotational axis. We find that the unexpected crossover of anomalous Hall resistance and negative magnetoresistance suddenly occurs when the angle reaches to ~70°, indicating that Berry curvature strongly correlates with quantum transports of Dirac and chiral fermions. It would be interesting to tune Berry curvature within other quantum phases such as topological superconductivity.