Vertically stacked Bi₂Se₃/MoTe₂ heterostructure with large band offsets for nanoelectronics

In recent years, two-dimensional material-based tunneling heterojunctions are emerging as a multi-functional architecture for logic circuits and photodetection owing to the flexible stacking, optical sensitivity, tunable detection band, and highly controllable conductivity behaviors. However, the existing structures are mainly focused on transition or post-transition metal chalcogenides and have been rarely investigated as topological insulator (such as Bi₂Se₃ or Bi₂Te₃)-based tunneling heterostructures. Meanwhile, it is challenging to mechanically exfoliate the topological insulator thin nanoflakes because of the strong layer-by-layer interaction with shorter interlayer spacing. Herein, we report Au-assisted exfoliation and non-destructive transfer method to fabricate large-scale Bi₂Se₃ thin nanosheets. Furthermore, a novel broken-gap tunneling heterostructure is designed by combing 2H-MoTe₂ and Bi₂Se₃via the dry-transfer method. Thanks to the realized band alignment, this ambipolar-n device shows a clear rectifying behavior at V_ds of 1 V. A built-in potential exceeding ∼0.7 eV is verified owing to the large band offsets by comparing the numerical solution of Poisson's equation and the experimental data. Carrier transport is governed by the majority carrier including thermionic emission and the tunneling process through the barrier height. At last, the device shows an ultralow dark current of ∼0.2 pA and a superior optoelectrical performance of I_light/I_dark ratio ≈10⁶, a fast response time of 21 ms, and a specific detectivity of 7.2 × 10¹¹ Jones for a visible light of 405 nm under zero-bias. Our work demonstrates a new universal method to fabricate a topological insulator and paves a new strategy for the construction of novel van der Waals tunneling structures.