DNA-driven dynamic assembly of MoS₂ nanosheets

Controlling the assembly of molybdenum disulfide (MoS₂) layers into static and dynamic superstructures can impact on their use in optoelectronics, energy, and drug delivery. Toward this goal, we present a strategy to drive the assembly of MoS₂ layers via the hybridization of complementary DNA linkers. By functionalizing the MoS₂ surface with thiolated DNA, MoS₂ nanosheets were assembled into mulitlayered superstructures, and the complementary DNA strands were used as linkers. A disassembly process was triggered by the formation of an intramolecular i-motif structure at a cystosine-rich sequence in the DNA linker at acidic pH values. We tested the versatility of our approach by driving the disassembly of the MoS₂ superstructures through a different DNA-based mechanism, namely strand displacement. This study demonstrates how DNA can be employed to drive the static and dynamic assembly of MoS₂ nanosheets in aqueous solution.