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Despite their importance, chemical reactions confined in a low dimensionalspace are elusive and experimentally intractable. In this work, we reportdoubly anisotropic, in-plane and out-of-plane, oxidation reactions oftwo-dimensional crystals, by resolving interface-confined thermal oxidation ofa single and multilayer MoS2 supported on silica substrates from theirconventional surface reaction. Using optical second-harmonic generationspectroscopy of artificially stacked multilayers, we directly proved thatcrystallographically oriented triangular oxides (TOs) were formed in thebottommost layer while triangular etch pits (TEs) were generated in the topmostlayer and that both structures were terminated with zigzag edges. The formationof the Mo oxide layer at the interface demonstrates that O2 diffusesefficiently through the van der Waals (vdW) gap but not MoO3, which wouldotherwise sublime. The fact that TOs are several times larger than TEsindicates that oxidation is greatly enhanced when MoS2 is in direct contactwith silica substrates, which suggests a catalytic effect. This study indicatesthat the vdW-bonded interfaces are essentially open to mass transport and canserve as a model system for investigating chemistry in low dimensional spaces.

Interface-Confined Doubly Anisotropic Oxidation of Two-Dimensional MoS2