Self‐Limiting Synthesis of Ultrathin Ge(110) Single Crystal via Liquid Metal

Abstract Germanium, the prime applied semiconductor, is widely used in solid‐state electronics and photoelectronics. Unfortunately, since the 3D diamond‐like structure with strong covalent bonds impedes the 2D anisotropic growth, only the examples of ultrathin Ge along the (111) plane have been investigated, much less to the controllable synthesis along another crystal surface. Meanwhile, Ge(111) flakes are limited in semiconductor applications because of their gapless property. Here, ultrathin Ge(110) single crystal is synthesized with semiconductive property via gallium‐associated self‐limiting growth. The obtained ultrathin Ge(110) single crystal exhibits anisotropic honeycomb structure, uniformly incremental lattice, wide tunable direct‐bandgap, blue‐shifted photoluminescence emission, and unique phonon modes, which are consistent with the previous theoretical predictions. It also confirms excellent second harmonic generation and high hole mobility of 724 cm² V⁻¹ s⁻¹. The realization of ultrathin Ge(110) single crystal will provide an excellent candidate for application in electronics and optoelectronics.