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; Kai Xiao

doi:10.1021/acsnano.8b09448

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, Kai Xiao

Research output: Contribution to journal › Article › peer-review

63 Scopus citations

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.

Original language	English
Pages (from-to)	2481-2489
Number of pages	9
Journal	ACS Nano
Volume	13
Issue number	2
DOIs	https://doi.org/10.1021/acsnano.8b09448
State	Published - Feb 26 2019

Funding

The material synthesis was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences (BES), Materials Sciences and Engineering Division. The optical characterization, optothermal Raman measurements, theoretical calculations, and analysis were performed at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. The transient absorption measurement was supported by the NSF grant (DMR-1505852). L.L. was supported by the Eugene P. Wigner Fellowship at the Oak Ridge National Laboratory (ORNL). J.Z. was supported by the “GO” program at ORNL. Part of the computations were performed using the resources of the Center for Computational Innovation at Rensselaer Polytechnic Institute.

Funders	Funder number
National Science Foundation	1505852, DMR-1505852
U.S. Department of Energy
Office of Science
Basic Energy Sciences
Oak Ridge National Laboratory
Division of Materials Sciences and Engineering

Keywords

2D materials
Isotope
MoS
Optothermal Raman technique
Thermal conductivity

Access to Document

10.1021/acsnano.8b09448

Cite this

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title = "Isotope-engineering the thermal conductivity of two-dimensional MoS2",

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.",

keywords = "2D materials, Isotope, MoS, Optothermal Raman technique, Thermal conductivity",

author = "Xufan Li and Jingjie Zhang and Puretzky, {Alexander A.} and Anthony Yoshimura and Xiahan Sang and Qiannan Cui and Yuanyuan Li and Liangbo Liang and Ghosh, {Avik W.} and Hui Zhao and Unocic, {Raymond R.} and Vincent Meunier and Rouleau, {Christopher M.} and Sumpter, {Bobby G.} and Geohegan, {David B.} and Kai Xiao",

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AU - Li, Xufan

AU - Zhang, Jingjie

AU - Puretzky, Alexander A.

AU - Yoshimura, Anthony

AU - Sang, Xiahan

AU - Cui, Qiannan

AU - Li, Yuanyuan

AU - Liang, Liangbo

AU - Ghosh, Avik W.

AU - Zhao, Hui

AU - Unocic, Raymond R.

AU - Meunier, Vincent

AU - Rouleau, Christopher M.

AU - Sumpter, Bobby G.

AU - Geohegan, David B.

AU - Xiao, Kai

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