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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. In this work, 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. Finally, these results shed light on the fundamentals of 2D nanoscale thermal transport important for the optimization of 2D electronic devices.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [1];  [3]; ORCiD logo [1];  [4];  [4]; ORCiD logo [1];  [5]; ORCiD logo [4]; ORCiD logo [1];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Virginia, Charlottesville, VA (United States)
  3. Rensselaer Polytechnic Inst., Troy, NY (United States)
  4. Univ. of Kansas, Lawrence, KS (United States)
  5. Univ. of Virginia, Charlottesville, VA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1528724
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 13; Journal Issue: 2; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; thermal conductivity; isotope; MoS2; optothermal Raman technique; 2D materials

Citation Formats

Li, Xufan, Zhang, Jingjie, Puretzky, Alexander A., Yoshimura, Anthony, Sang, Xiahan, Cui, Qiannan, Li, Yuanyuan, Liang, Liangbo, Ghosh, Avik W., Zhao, Hui, Unocic, Raymond R., Meunier, Vincent, Rouleau, Christopher M., Sumpter, Bobby, Geohegan, David B., and Xiao, Kai. Isotope-Engineering the Thermal Conductivity of Two-Dimensional MoS2. United States: N. p., 2019. Web. doi:10.1021/acsnano.8b09448.
Li, Xufan, Zhang, Jingjie, Puretzky, Alexander A., Yoshimura, Anthony, Sang, Xiahan, Cui, Qiannan, Li, Yuanyuan, Liang, Liangbo, Ghosh, Avik W., Zhao, Hui, Unocic, Raymond R., Meunier, Vincent, Rouleau, Christopher M., Sumpter, Bobby, Geohegan, David B., & Xiao, Kai. Isotope-Engineering the Thermal Conductivity of Two-Dimensional MoS2. United States. https://doi.org/10.1021/acsnano.8b09448
Li, Xufan, Zhang, Jingjie, Puretzky, Alexander A., Yoshimura, Anthony, Sang, Xiahan, Cui, Qiannan, Li, Yuanyuan, Liang, Liangbo, Ghosh, Avik W., Zhao, Hui, Unocic, Raymond R., Meunier, Vincent, Rouleau, Christopher M., Sumpter, Bobby, Geohegan, David B., and Xiao, Kai. Wed . "Isotope-Engineering the Thermal Conductivity of Two-Dimensional MoS2". United States. https://doi.org/10.1021/acsnano.8b09448. https://www.osti.gov/servlets/purl/1528724.
@article{osti_1528724,
title = {Isotope-Engineering the Thermal Conductivity of Two-Dimensional MoS2},
author = {Li, Xufan and Zhang, Jingjie and Puretzky, Alexander A. and Yoshimura, Anthony and Sang, Xiahan and Cui, Qiannan and Li, Yuanyuan and Liang, Liangbo and Ghosh, Avik W. and Zhao, Hui and Unocic, Raymond R. and Meunier, Vincent and Rouleau, Christopher M. and Sumpter, Bobby and Geohegan, David B. and Xiao, Kai},
abstractNote = {Isotopes represent a degree of freedom that might be exploited to tune the physical properties of materials while preserving their chemical behaviors. In this work, 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. Finally, these results shed light on the fundamentals of 2D nanoscale thermal transport important for the optimization of 2D electronic devices.},
doi = {10.1021/acsnano.8b09448},
journal = {ACS Nano},
number = 2,
volume = 13,
place = {United States},
year = {Wed Jan 23 00:00:00 EST 2019},
month = {Wed Jan 23 00:00:00 EST 2019}
}

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Works referencing / citing this record:

The role of mid-gap phonon modes in thermal transport of transition metal dichalcogenides
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