Department of Physics, Seoul National University , Seoul 08826, Korea.
Theory and Simulation of Materials (THEOS), and National Centre for Computational Design and Discovery of Novel Materials (MARVEL), École Polytechnique Fédérale de Lausanne , 1015 Lausanne, Switzerland.
Nano Lett. 2016 Apr 13;16(4):2439-43. doi: 10.1021/acs.nanolett.5b05288. Epub 2016 Mar 3.
Graphene, as a semimetal with the largest known thermal conductivity, is an ideal system to study the interplay between electronic and lattice contributions to thermal transport. While the total electrical and thermal conductivity have been extensively investigated, a detailed first-principles study of its electronic thermal conductivity is still missing. Here, we first characterize the electron-phonon intrinsic contribution to the electronic thermal resistivity of graphene as a function of doping using electronic and phonon dispersions and electron-phonon couplings calculated from first-principles at the level of density-functional theory and many-body perturbation theory (GW). Then, we include extrinsic electron-impurity scattering using low-temperature experimental estimates. Under these conditions, we find that the in-plane electronic thermal conductivity κe of doped graphene is ∼300 W/mK at room temperature, independently of doping. This result is much larger than expected and comparable to the total thermal conductivity of typical metals, contributing ∼10% to the total thermal conductivity of bulk graphene. Notably, in samples whose physical or domain sizes are of the order of few micrometers or smaller, the relative contribution coming from the electronic thermal conductivity is more important than in the bulk limit, because lattice thermal conductivity is much more sensitive to sample or grain size at these scales. Last, when electron-impurity scattering effects are included we find that the electronic thermal conductivity is reduced by 30 to 70%. We also find that the Wiedemann-Franz law is broadly satisfied at low and high temperatures but with the largest deviations of 20-50% around room temperature.
石墨烯作为热导率最大的半导体,是研究电子和晶格对热输运的相互作用的理想体系。虽然总电导率和热导率已经得到了广泛的研究,但对其电子热导率的详细第一性原理研究仍然缺失。在这里,我们首先利用第一性原理计算的电子和声子色散以及电子-声子耦合,在密度泛函理论和多体微扰理论(GW)水平上,来表征掺杂石墨烯中电子热电阻率的电子-声子固有贡献随掺杂的变化。然后,我们使用低温实验估算来包含电子-杂质散射的外效应。在这些条件下,我们发现室温下掺杂石墨烯的面内电子热导率κe约为 300 W/mK,与掺杂无关。这一结果远远大于预期,与典型金属的总热导率相当,对块状石墨烯的总热导率的贡献约为 10%。值得注意的是,在物理或畴尺寸为几微米或更小的样品中,电子热导率的相对贡献比在体相极限中更重要,因为在这些尺度下,晶格热导率对样品或晶粒尺寸更加敏感。最后,当包含电子-杂质散射效应时,我们发现电子热导率降低了 30%到 70%。我们还发现,在低温和高温下,维德曼-弗朗兹定律都得到了广泛的满足,但在室温附近偏离最大,为 20-50%。