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Register a new userMechanistic Transition from Phonon Propagation to Thermal Hopping in Two-Dimensional Solids
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Thermal transport in solids changes its nature from phonon propagation that suffers from perturbative scattering to thermally activated hops between localized vibrational modes as the level of disorder increases. Models have been proposed to understand these two distinct extremes that predict opposite temperature dependence of the thermal conductivity, but not for the transition or the intermediate regime. Here we explore thermal transport in two-dimensional crystalline and amorphous silica with varying levels of disorder, {alpha}, by performing atomistic simulations as well as analysis based on the kinetic and Allen-Feldman theories. We demonstrate the crossover between the crystalline and amorphous regimes at {alpha} ~ 0.3, which can be identified by a turnover of the temperature dependence in thermal conductivity, and explained by the dominance of thermal hopping processes. The determination of this critical disorder level is also validated by the analysis of the participation ratio of localized vibrational modes, and the spatial localization of heat flux. These factors can serve as key indicators in characterizing the transition in heat transport mechanisms.
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We report results of investigation of the phonon and thermal properties of the exfoliated films of layered single crystals of antiferromagnetic FePS3 and MnPS3 semiconductors. The Raman spectroscopy was conducted using three different excitation lasers with the wavelengths of 325 nm (UV), 488 nm (blue), and 633 nm (red). The resonant UV-Raman spectroscopy reveals new spectral features, which are not detectable via visible Raman light scattering. The thermal conductivity of FePS3 and MnPS3 thin films was measured by two different techniques: the steady-state Raman optothermal and transient time-resolved magneto-optical Kerr effect. The Raman optothermal measurements provided the orientation-average thermal conductivity of FePS3 to be 1.35 W/mK at room temperature. The transient measurements revealed that the through-plane and in-plane thermal conductivity of FePS3 is 0.85 W/mK and 2.7 W/mK, respectively. The films of MnPS3 have higher thermal conductivity of 1.1 W/mK through-plane and 6.3 W/mK in-plane. The data obtained by both techniques reveal strong thermal anisotropy of the films and the dominant contribution of phonons to heat conduction. Our results are important for the proposed applications of the antiferromagnetic semiconductor thin films in spintronic devices.
We investigated theoretically the phonon thermal conductivity of single layer graphene. The phonon dispersion for all polarizations and crystallographic directions in graphene lattice was obtained using the valence-force field method. The three-phonon Umklapp processes were treated exactly using an accurate phonon dispersion and Brillouin zone, and accouting for all phonon relaxation channels allowed by the momentum and energy conservation laws. The uniqueness of graphene was reflected in the two-dimensional phonon density of states and restrictions on the phonon Umklapp scattering phase-space. The phonon scattering on defects and graphene edges has been also included in the model. The calculations were performed for the Gruneisen parameter, which was determined from the ab initio theory as a function of the phonon wave vector and polarization branch, and for a range of values from experiments. It was found that the near room-temperature thermal conductivity of single layer graphene, calculated with a realistic Gruneisen parameter, is in the range ~ 2000 - 5000 W/mK depending on the defect concentration and roughness of the edges. Owing to the long phonon mean free path the graphene edges produce strong effect on thermal conductivity even at room temperature. The obtained results are in good agreement with the recent measurements of the thermal conductivity of suspended graphene.
In stark contrast with three-dimensional (3D) nanostructures, we show that boundary scattering in two-dimensional (2D) nanoribbons alone does not lead to a finite phonon mean free path. If combined with an intrinsic scattering mechanism, 2D boundary scattering does reduce the overall mean free path, however the latter does not scale proportionally to the ribbon width, unlike the well known Casimir regime occurring in 3D nanowires. We show that boundary scattering can be accounted for by a simple Mathiessen type approach for many different 3D nanowire cross sectional shapes, however this is not possible in the 2D nanoribbon case, where a complete solution of the Boltzmann transport equation is required. These facts have strong implications for the thermal conductivity of suspended nanostructures.
While crystalline two-dimensional materials have become an experimental reality during the past few years, an amorphous 2-D material has not been reported before. Here, using electron irradiation we create an sp2-hybridized one-atom-thick flat carbon membrane with a random arrangement of polygons, including four-membered carbon rings. We show how the transformation occurs step-by-step by nucleation and growth of low-energy multi-vacancy structures constructed of rotated hexagons and other polygons. Our observations, along with first-principles calculations, provide new insights to the bonding behavior of carbon and dynamics of defects in graphene. The created domains possess a band gap, which may open new possibilities for engineering graphene-based electronic devices.
We use the time-resolved magneto-optical Kerr effect (TRMOKE) to measure the local temperature and heat flow dynamics in ferromagnetic SrRuO3 thin films. After heating by a pump pulse, the film temperature decays exponentially, indicating that the heat flow out of the film is limited by the film/substrate interface. We show that this behavior is consistent with an effective boundary resistance resulting from disequilibrium between the spin and phonon temperatures in the film.
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