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Thermal conductivity of isotopically modified graphene

Nature Materials volume 11, pages 203–207 (2012)Cite this article

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Abstract

In addition to its exotic electronic properties1,2 graphene exhibits unusually high intrinsic thermal conductivity3,4,5,6. The physics of phonons—the main heat carriers in graphene—has been shown to be substantially different in two-dimensional (2D) crystals, such as graphene, from in three-dimensional (3D) graphite7,8,9,10. Here, we report our experimental study of the isotope effects on the thermal properties of graphene. Isotopically modified graphene containing various percentages of 13C were synthesized by chemical vapour deposition (CVD). The regions of different isotopic compositions were parts of the same graphene sheet to ensure uniformity in material parameters. The thermal conductivity, K, of isotopically pure 12C (0.01% 13C) graphene determined by the optothermal Raman technique3,4,5,6,7,10, was higher than 4,000 W mK−1 at the measured temperature Tm~320 K, and more than a factor of two higher than the value of K in graphene sheets composed of a 50:50 mixture of 12C and 13C. The experimental data agree well with our molecular dynamics (MD) simulations, corrected for the long-wavelength phonon contributions by means of the Klemens model. The experimental results are expected to stimulate further studies aimed at a better understanding of thermal phenomena in 2D crystals.

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Figure 1: Micro-Raman characteristics of the isotopically modified graphene.
Figure 2: Thermal conductivity K of the suspended graphene film with 13C isotope concentrations of 0.01%, 1.1% (natural abundance), 50% and 99.2%, respectively, as a function of the temperature measured with the micro-Raman spectrometer.
Figure 3: Thermal conductivity of graphene as a function of its isotopic composition.

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Acknowledgements

The authors appreciate comments by L. Shi and H. Zhao. The work at UTA was supported by the National Science Foundation grant no. 1006350, the W. M. Keck Foundation, and the Office of Naval Research. The work at XMU was supported by the National Natural Science Foundation of China through grant nos. 91123009, 111104228, 10975115, 60827004 and 90921002 and the ‘973’ program 2012CB619301 and 2011CB925600. The work at UCR was supported, in part, by the Semiconductor Research Corporation—Defense Advanced Research Project Agency FCRP Functional Engineered Nano Architectonic centre, National Science Foundation and US Office of Naval Research. K.C. was supported by the NRF of Korea through WCU program grant no. R-31-2008-000-10083-0. R.S.R. acknowledges the support of the W.M. Keck Foundation.

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Authors and Affiliations

  1. Department of Physics, Fujian Key Laboratory of Semiconductor Materials and Application, Xiamen University, Xiamen 361005, China

    Shanshan Chen, Junyong Kang & Weiwei Cai

  2. Department of Mechanical Engineering and the Materials Science and Engineering Program, University of Texas at Austin, Austin, Texas 78712, USA

    Shanshan Chen, Qingzhi Wu, Columbia Mishra, Weiwei Cai & Rodney S. Ruoff

  3. Department of Materials Science and Engineering and Department of Physics, University of Texas at Dallas, Richardson, Texas 75080, USA

    Hengji Zhang & Kyeongjae Cho

  4. Division of WCU Multiscale Mechanical Design, School of Mechanical and Aerospace Engineering, Seoul National University, Seoul 151-742, Republic of Korea

    Kyeongjae Cho

  5. Department of Electrical Engineering and Materials Science and Engineering Program, University of California at Riverside, Riverside, California 92521, USA

    Alexander A. Balandin

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Contributions

R.S.R. coordinated the project and data analysis; A.A.B. led the thermal data analysis; S.C. performed sample growth, measurements and data analysis; W.C. carried out the Raman optothermal measurement and data analysis. Q.W. assisted on the sample transfer. C.M. and J.K. contributed to the discussion of the data analysis. H.Z. and K.C. performed MD simulations; S.C., W.C., R.S.R. and A.A.B. wrote the manuscript.

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Correspondence to Weiwei Cai or Alexander A. Balandin.

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Chen, S., Wu, Q., Mishra, C. et al. Thermal conductivity of isotopically modified graphene. Nature Mater 11, 203–207 (2012). https://doi.org/10.1038/nmat3207

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