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Extremely High Thermal Conductivity of Graphene: Experimental Study

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 Added by Alexander Balandin
 Publication date 2008
  fields Physics
and research's language is English




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We report on the first measurement of the thermal conductivity of a suspended single layer graphene. The measurements were performed using a non-contact optical technique. The near room-temperature values of the thermal conductivity in the range ~ 4840 to 5300 W/mK were extracted for a single-layer graphene. The extremely high value of the thermal conductivity suggests that graphene can outperform carbon nanotubes in heat conduction.



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AlN is an ultra-wide bandgap semiconductor which has been developed for applications including power electronics and optoelectronics. Thermal management of these applications is the key for stable device performance and allowing for long lifetimes. AlN, with its potentially high thermal conductivity, can play an important role serving as a dielectric layer, growth substrate, and heat spreader to improve device performance. However, the intrinsic high thermal conductivity of bulk AlN predicted by theoretical calculations has not been experimentally observed because of the difficulty in producing materials with low vacancy and impurity levels, and other associated defect complexes in AlN which can decrease the thermal conductivity. This work reports the growth of thick AlN layers by MOCVD with an air-pocketed AlN layer and the first experimental observation of intrinsic thermal conductivity from 130 K to 480 K that matches density-function-theory calculations for single crystal AlN, producing some of the highest values ever measured. Detailed material characterizations confirm the high quality of these AlN samples with one or two orders of magnitude lower impurity concentrations than seen in commercially available bulk AlN. Measurements of these commercially available bulk AlN substrates from 80 K to 480 K demonstrated a lower thermal conductivity, as expected. A theoretical thermal model is built to interpret the measured temperature dependent thermal conductivity. Our work demonstrates that it is possible to obtain theoretically high values of thermal conductivity in AlN and such films may impact the thermal management and reliability of future electronic and optoelectronics devices.
The low-temperature thermal conductivity in polycrystalline graphene is theoretically studied. The contributions from three branches of acoustic phonons are calculated by taking into account scattering on sample borders, point defects and grain boundaries. Phonon scattering due to sample borders and grain boundaries is shown to result in a $T^{alpha}$-behaviour in the thermal conductivity where $alpha$ varies between 1 and 2. This behaviour is found to be more pronounced for nanosized grain boundaries. PACS: 65.80.Ck, 81.05.ue, 73.43.Cd
The authors proposed a simple model for the lattice thermal conductivity of graphene in the framework of Klemens approximation. The Gruneisen parameters were introduced separately for the longitudinal and transverse phonon branches through averaging over phonon modes obtained from the first-principles. The calculations show that Umklapp-limited thermal conductivity of graphene grows with the increasing linear dimensions of graphene flakes and can exceed that of the basal planes of bulk graphite when the flake size is on the order of few micrometers. The obtained results are in agreement with experimental data and reflect the two-dimensional nature of phonon transport in graphene.
We have investigated thermal conductivity of graphene laminate films deposited on polyethylene terephthalate substrates. Two types of graphene laminate were studied - as deposited and compressed - in order to determine the physical parameters affecting the heat conduction the most. The measurements were performed using the optothermal Raman technique and a set of suspended samples with the graphene laminate thickness from 9 to 44 micrometers. The thermal conductivity of graphene laminate was found to be in the range from 40 W/mK to 90 W/mK at room temperature. It was found unexpectedly that the average size and the alignment of graphene flakes are more important parameters defining the heat conduction than the mass density of the graphene laminate. The thermal conductivity scales up linearly with the average graphene flake size in both uncompressed and compressed laminates. The compressed laminates have higher thermal conductivity for the same average flake size owing to better flake alignment. The possibility of up to 600X enhancement of the thermal conductivity of plastic materials by coating them with the thin graphene laminate films has important practical implications.
We investigated thermal conductivity of free-standing reduced graphene oxide films subjected to a high-temperature treatment of up to 1000 C. It was found that the high-temperature annealing dramatically increased the in-plane thermal conductivity, K, of the films from 3 W/mK to 61 W/mK at room temperature. The cross-plane thermal conductivity, Kc, revealed an interesting opposite trend of decreasing to a very small value of 0.09 W/mK in the reduced graphene oxide films annealed at 1000 C. The obtained films demonstrated an exceptionally strong anisotropy of the thermal conductivity, K/Kc ~ 675, which is substantially larger even than in the high-quality graphite. The electrical resistivity of the annealed films reduced to 1 - 19 Ohms/sq. The observed modifications of the in-plane and cross-plane thermal conductivity components resulting in an unusual K/Kc anisotropy were explained theoretically. The theoretical analysis suggests that K can reach as high as ~500 W/mK with the increase in the sp2 domain size and further reduction of the oxygen content. The strongly anisotropic heat conduction properties of these films can be useful for applications in thermal management.
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