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2D heterostructures are more than a sum of the parent 2D materials, but arealso a product of the interlayer coupling, which can induce new properties. Inthis paper we present a method to tune the interlayer coupling in Bi2Se3/MoS22D heterostructures by regulating the oxygen presence in the atmosphere, whileapplying laser or thermal energy. Our data suggests the interlayer coupling istuned through the diffusive intercalation and de-intercalation of oxygenmolecules. When one layer of Bi2Se3 is grown on monolayer MoS2, an influentialinterlayer coupling is formed that quenches the signature photoluminescence(PL) peaks. However, thermally annealing in the presence of oxygen disrupts theinterlayer coupling, facilitating the emergence of the MoS2 PL peak. DFTcalculations predict intercalated oxygen increases the interlayer separation~17%, disrupting the interlayer coupling and inducing the layers to behave moreelectronically independent. The interlayer coupling can then be restored bythermally annealing in N2 or Ar, where the peaks will re-quench. Hence, this isan interesting oxygen-induced switching between "non-radiative" and "radiative"exciton recombination. This switching can also be accomplished locally,controllably, and reversibly using a low-power focused laser, while changingthe environment from pure N2 to air. This allows for the interlayer coupling tobe precisely manipulated with submicron spatial resolution, facilitatingsite-programmable 2D light-emitting pixels whose emission intensity could beprecisely varied by a factor exceeding 200x. Our results show that theseatomically-thin 2D heterostructures may be excellent candidates for oxygensensing.

Oxygen-induced in-situ manipulation of the interlayer coupling and exciton recombination in Bi2Se3/MoS2 2D heterostructures