Abstract 2D van der Waals layered heterostructures allow for a variety of energy band offsets, which help in developing valuable multifunctional devices. However, p–n diodes, which are typical and versatile, are still limited by the material choice due to the fixed band structures. Here, the vanadium dopant concentration is modulated in monolayer WSe2 via chemical vapor deposition to demonstrate tunable multifunctional quantum tunneling diodes by vertically stacking SnSe2 layers at room temperature. This is implemented by substituting tungsten atoms with vanadium atoms in WSe2 to provoke the p‐type doping effect in order to efficiently modulate the Fermi level. The precise control of the vanadium doping concentration is the key to achieving the desired quantum tunneling diode behaviors by tuning the proper band alignment for charge transfer across the heterostructure. By constructing a p–n diode for p‐type V‐doped WSe2 and heavily degenerate n‐type SnSe2, the type‐II band alignment at low V‐doping concentration is clearly shown, which evolves into the type‐III broken‐gap alignment at heavy V‐doping concentration to reveal a variety of diode behaviors such as forward diode, backward diode, negative differential resistance, and ohmic resistance.
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