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Phonon Transport in Suspended Single Layer Graphene

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 Publication date 2010
  fields Physics
and research's language is English




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We report the first temperature dependent phonon transport measurements in suspended Cu-CVD single layer graphene (SLG) from 15K to 380K using microfabricated suspended devices. The thermal conductance per unit cross section $sigma$/A increases with temperature and exhibits a peak near T~280K ($pm$10K) due to the Umklapp process. At low temperatures (T<140K), the temperature dependent thermal conductivity scales as ~T^{1.5}, suggesting that the main contribution to thermal conductance arises from flexural acoustic (ZA) phonons in suspended SLG. The $sigma$/A reaches a high value of 1.7$times10^5 T^{1.5}$ W/m^2K, which is approaching the expected ballistic phonon thermal conductance for two-dimensional graphene sheets. Our results not only clarify the ambiguity in the thermal conductance, but also demonstrate the potential of Cu-CVD graphene for heat related applications.



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Graphene exhibits extraordinary electronic and mechanical properties, and extremely high thermal conductivity. Being a very stable atomically thick membrane that can be suspended between two leads, graphene provides a perfect test platform for studying thermal conductivity in two-dimensional systems, which is of primary importance for phonon transport in low-dimensional materials. Here we report experimental measurements and non-equilibrium molecular dynamics simulations of thermal conduction in suspended single layer graphene as a function of both temperature and sample length. Interestingly and in contrast to bulk materials, when temperature at 300K, thermal conductivity keeps increasing and remains logarithmic divergence with sample length even for sample lengths much larger than the average phonon mean free path. This result is a consequence of the two-dimensional nature of phonons in graphene and provides fundamental understanding into thermal transport in two-dimensional materials.
Recent experiments have shown surprisingly large thermal time constants in suspended graphene ranging from 10 to 100 ns in drums with a diameter ranging from 2 to 7 microns. The large time constants and their scaling with diameter points towards a thermal resistance at the edge of the drum. However, an explanation of the microscopic origin of this resistance is lacking. Here, we show how phonon scattering at a kink in the graphene, e.g. formed by sidewall adhesion at the edge of the suspended membrane, can cause a large thermal time constant. This kink strongly limits the fraction of flexural phonons that cross the suspended graphene edge, which causes a thermal interface resistance at its boundary. Our model predicts thermal time constants that are of the same order of magnitude as experimental data, and shows a similar dependence on the circumference. Furthermore, the model predicts the relative in-plane and out-of-plane phonon contributions to graphenes thermal expansion force, in agreement with experiments. We thus show, that in contrast to conventional thermal (Kapitza) resistance which occurs between two different materials, in 2D materials another type of thermal interface resistance can be geometrically induced in a single material.
Using electrical transport experiments and shot noise thermometry, we investigate electron-phonon heat transfer rate in a suspended bilayer graphene. Contrary to monolayer graphene with heat flow via three-body supercollision scattering, we find that regular electron - optical phonon scattering in bilayer graphene provides the dominant scattering process at electron energies $ gtrsim 0.15$ eV. We determine the strength of these intrinsic heat flow processes of bilayer graphene and find good agreement with theoretical estimates when both zone edge and zone center optical phonons are taken into account.
Phonon self-energy corrections have mostly been studied theoretically and experimentally for phonon modes with zone-center (q = 0) wave-vectors. Here, gate-modulated Raman scattering is used to study phonons of a single layer of graphene (1LG) in the frequency range from 2350 to 2750 cm-1, which shows the G* and the G-band features originating from a double-resonant Raman process with q ot= 0. The observed phonon renormalization effects are different from what is observed for the zone-center q = 0 case. To explain our experimental findings, we explored the phonon self-energy for the phonons with non-zero wave-vectors (q ot= 0) in 1LG in which the frequencies and decay widths are expected to behave oppositely to the behavior observed in the corresponding zone-center q = 0 processes. Within this framework, we resolve the identification of the phonon modes contributing to the G* Raman feature at 2450 cm-1 to include the iTO+LA combination modes with q ot= 0 and the 2iTO overtone modes with q = 0, showing both to be associated with wave-vectors near the high symmetry point K in the Brillouin zone.
Using electrical transport experiments and shot noise thermometry, we find strong evidence that supercollision scattering processes by flexural modes are the dominant electron-phonon energy transfer mechanism in high-quality, suspended graphene around room temperature. The power law dependence of the electron-phonon coupling changes from cubic to quintic with temperature. The change of the temperature exponent by two is reflected in the quadratic dependence on chemical potential, which is an inherent feature of two-phonon quantum processes.
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