Multilayer A17 Black Antimonene via van der Waals Epitaxy

Metastable layered antimony in the black phosphorus-like A17 phase exhibits promising electronic properties arising from pronounced spin–orbit coupling and suppressed phonon scattering. However, charge transport characterization has been severely constrained by insufficient crystal dimensions. Here, the dielectric-mediated van der Waals epitaxy of multilayer A17 black antimonene is reported, with the as-grown rectangular nanosheets exceeding 10 μm in length and exhibiting layer-dependent phase stability up to 16-layer stacking. Structural analysis reveals that monolayer nucleation favors zigzag and diagonal edge formation and shows that the multilayer structure adopts an AB-stacking configuration. Angle-dependent Raman vibration signatures are resolved, and the spectral benchmark is validated for identifying the zigzag crystal orientation. Structural stability in air over 3 weeks is confirmed through Raman modes. In the zigzag direction, the p -type carrier mobilities of 170 cm 2 ·V –1 ·s –1 at room temperature and 287 cm 2 ·V –1 ·s –1 at 10 K are corroborated using back-gate field-effect devices. With decent carrier mobilities in multilayer A17 black antimonene, this work offers an experimental platform for investigating exotic electronic properties in monolayer and few-layer A17 black antimonene.