Thickness sorting of two-dimensional transition metal dichalcogenides via copolymer-assisted density gradient ultracentrifugation

Abstract
Two-dimensional transition metal dichalcogenides have emerged as leading successors to graphene due to their diverse properties, which depend sensitively on sample thickness. Although solution-based exfoliation methods hold promise for scalable production of these materials, existing techniques introduce irreversible structural defects and/or lack sufficient control over the sample thickness. In contrast, previous work on carbon nanotubes and graphene has shown that isopycnic density gradient ultracentrifugation can produce structurally and electronically monodisperse nanomaterial populations. However, this approach cannot be directly applied to transition metal dichalcogenides due to their high intrinsic buoyant densities when encapsulated with ionic small molecule surfactants. Here, we overcome this limitation and thus demonstrate thickness sorting of pristine molybdenum disulfide (MoS2) by employing a block copolymer dispersant composed of a central hydrophobic unit flanked by hydrophilic chains that effectively reduces the overall buoyant density in aqueous solution. The resulting solution-processed monolayer MoS2 samples exhibit strong photoluminescence without further chemical treatment.