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Register a new userTuning thermal transport in graphene via combinations of molecular antiresonances
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We propose a method to engineer the phonon thermal transport properties of low dimensional systems. The method relies on introducing a predetermined combination of molecular adsorbates, which give rise to antiresonances at frequencies specific to the molecular species. Despite their dissimilar transmission spectra, thermal resistances due to individual molecules remain almost the same for all species. On the other hand, thermal resistance due to combinations of different species are not additive and show large differences depending on the species. Using a toy model, the physics underlying the violation of resistance summation rule is investigated. It is demonstrated that equivalent resistance of two scatterers having the same resistances can be close to the sum of the constituents or $sim$70% of it depending on the relative positions of the antiresonances. The relative positions of the antiresonances determine the net change in transmission, therefore the equivalent resistance. Since the entire spectrum is involved in phonon spectrum changes in different parts of the spectrum become important. Performing extensive first-principles based computations, we show that these distinctive attributes of phonon transport can be useful to tailor the thermal transport through low dimensional materials, especially for thermoelectric and thermal management applications.
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Understanding and controlling heat transport in molecular junctions would provide new routes to design nanoscale coupled electronic and phononic devices. Using first principles full quantum calculations, we tune thermal conductance of a molecular junction by mechanically compressing and extending a short alkane chain connected to graphene leads. We find that the thermal conductance of the compressed junction drops by half in comparison to the extended junction, making it possible to turn on and off the heat current. The low conductance of the off state does not vary by further approaching the leads and stems from the suppression of the transmission of the in--plane transverse and longitudinal channels. Furthermore, we show that misalignment of the leads does not reduce the conductance ratio. These results also contribute to the general understanding of thermal transport in molecular junctions.
Step junctions are often present in layered materials, i.e. where single-layer regions meet multi-layer regions, yet their effect on thermal transport is not understood to date. Here, we measure heat flow across graphene junctions (GJs) from monolayer to bilayer graphene, as well as bilayer to four-layer graphene for the first time, in both heat flow directions. The thermal conductance of the monolayer-bilayer GJ device ranges from ~0.5 to 9.1x10^8 Wm-2K-1 between 50 K to 300 K. Atomistic simulations of such GJ device reveal that graphene layers are relatively decoupled, and the low thermal conductance of the device is determined by the resistance between the two dis-tinct graphene layers. In these conditions the junction plays a negligible effect. To prove that the decoupling between layers controls thermal transport in the junction, the heat flow in both directions was measured, showing no evidence of thermal asymmetry or rectification (within experimental error bars). For large-area graphene applications, this signifies that small bilayer (or multilayer) islands have little or no contribution to overall thermal transport.
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In this work, we report on hot carrier diffusion in graphene across large enough length scales that the carriers are not thermalized across the crystal. The carriers are injected into graphene at one site and their thermal transport is studied as a function of applied power and distance from the heating source, up to tens of micrometers away. Superconducting contacts prevent out-diffusion of hot carriers to isolate the electron-phonon coupling as the sole channel for thermal relaxation. As local thermometers, we use the amplitude of the Universal Conductance Fluctuations, which varies monotonically as a function of temperature. By measuring the electron temperature simultaneously along the length we observe a thermal gradient which results from the competition between electron-phonon cooling and lateral heat flow.
We study the electronic contribution to the main thermoelectric properties of a molecular junction consisting of a single quantum dot coupled to graphene external leads. The system electrical conductivity (G), Seebeck coefficient ($S$), and the thermal conductivity ($kappa$), are numerically calculated based on a Greens function formalism that includes contributions up to the Hartree-Fock level. We consider the system leads to be made either of pure or gapped-graphene. To describe the free electrons in the gapped-graphene electrodes we used two possible scenarios, the massive gap scenario, and the massless gap scenario, respectively. In all cases, the Fano effect is responsible for a strong violation of the Wiedemann-Franz law and we found a substantial increase of the system figure of merit $ZT$ due to a drastic reduction of the system thermal coefficient. In the case of gapped-graphene electrodes, the system figure of merit presents a maximum at an optimal value of the energy gap of the order of $Delta/Dsim$ 0.002 (massive gap scenario) and $Delta/Dsim$ 0.0026 (massless gap scenario). Additionally, for all cases, the system figure of merit is temperature dependent.
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