Isotope-Engineering the Thermal Conductivity of Two-Dimensional MoS2

Xufan Li, Jingjie Zhang, Alexander A. Puretzky, Anthony Yoshimura, Xiahan Sang, Qiannan Cui, Yuanyuan Li, Liangbo Liang, Avik W. Ghosh, Hui Zhao, Raymond R. Unocic, Vincent Meunier, Christopher M. Rouleau, Bobby G. Sumpter, David B. Geohegan, and Kai Xiao, ACS Nano , 13 (2) :2481 (2019).

Abstract

Isotopes represent a degree of freedom that might be exploited to tune the physical properties of materials while preserving their chemical behaviors. Here, we demonstrate that the thermal properties of two-dimensional (2D) transition-metal dichalcogenides can be tailored through isotope engineering. Monolayer crystals of MoS2 were synthesized with isotopically pure 100Mo and 92Mo by chemical vapor deposition employing isotopically enriched molybdenum oxide precursors. The in-plane thermal conductivity of the 100MoS2 monolayers, measured using a non-destructive, optothermal Raman technique, is found to be enhanced by ∼50% compared with the MoS2 synthesized using mixed Mo isotopes from naturally occurring molybdenum oxide. The boost of thermal conductivity in isotopically pure MoS2 monolayers is attributed to the combined effects of reduced isotopic disorder and a reduction in defect-related scattering, consistent with observed stronger photoluminescence and longer exciton lifetime. These results shed light on the fundamentals of 2D nanoscale thermal transport important for the optimization of 2D electronic devices.