Growth of bilayer MoTe₂ single crystals with strong non-linear Hall effect

The reduced symmetry in strong spin-orbit coupling materials such as transition metal ditellurides (TMDTs) gives rise to non-trivial topology, unique spin texture, and large charge-to-spin conversion efficiencies. Bilayer TMDTs are non-centrosymmetric and have unique topological properties compared to monolayer or trilayer, but a controllable way to prepare bilayer MoTe₂ crystal has not been achieved to date. Herein, we achieve the layer-by-layer growth of large-area bilayer and trilayer 1T′ MoTe₂ single crystals and centimetre-scale films by a two-stage chemical vapor deposition process. The as-grown bilayer MoTe₂ shows out-of-plane ferroelectric polarization, whereas the monolayer and trilayer crystals are non-polar. In addition, we observed large in-plane nonlinear Hall (NLH) effect for the bilayer and trilayer T_d phase MoTe₂ under time reversal-symmetric conditions, while these vanish for thicker layers. For a fixed input current, bilayer T_d MoTe₂ produces the largest second harmonic output voltage among the thicker crystals tested. Our work therefore highlights the importance of thickness-dependent Berry curvature effects in TMDTs that are underscored by the ability to grow thickness-precise layers.