No Arabic abstract
In two-dimensional materials, structure difference induces the difference in phonon dispersions, leading to the anisotropy of in-plane thermal transport. Here, we report an exceptional case in layered PdSe2, where the bonding, force constants, and lattice constants are nearly-equal along the in-plane crystallographic axis directions. The phonon dispersions show significant differences between the Gamma-X and Gamma-Y directions, leading to the anisotropy of in-plane thermal conductivity with a ratio up to 1.8. Such anisotropy is not only unexpected in equilaterally structured (in-plane) materials but also comparable to the record in the non-equilaterally structured material reported to date. By combining inelastic X-ray scattering and first-principles calculations, we attribute such anisotropy to the low-energy phonons along Gamma-X, in particular, their lower group velocities and avoided-crossing behavior. The different bucking structures between a- (zigzag-type) and b-axis (flat-type) are mainly responsible for the unique phonon dynamics properties of PdSe2. The present results illustrate the unusual thermal conduction mechanism of the equilaterally structured materials and provide valuable insights on thermal management in electronic 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.
We have investigated the anisotropic thermal expansion of graphite using ab-initio calculation of lattice dynamics and anharmonicity of the phonons, which reveal that the negative thermal expansion (NTE) in the a-b plane below 600 K and very large positive thermal expansion along the c-axis up to high temperatures arise due to various phonons polarized along the c-axis. While the NTE arises from the anharmonicity of transverse phonons over a broad energy range up to 60 meV, the large positive expansion along the c-axis occurs largely due to the longitudinal optic phonon modes around 16 meV and a large linear compressibility along the c-axis. The hugely anisotropic bonding in graphite is found to be responsible for wide difference in the energy range of the transverse and longitudinal phonon modes polarized along the c-axis, which are responsible for the anomalous thermal expansion behavior. This behaviour is in contrast to other nearly isotropic hexagonal structures like water-ice, which show anomalous thermal expansion in a small temperature range arising from a narrow energy range of phonons.
We study heat conduction in one dimensional (1D) anharmonic lattices analytically and numerically by using an effective phonon theory. It is found that every effective phonon mode oscillates quasi-periodically. By weighting the power spectrum of the total heat flux in the Debye formula, we obtain a unified formalism that can explain anomalous heat conduction in momentum conserved lattices without on-site potential and normal heat conduction in lattices with on-site potential. Our results agree very well with numerical ones for existing models such as the Fermi-Pasta-Ulam model, the Frenkel-Kontorova model and the $phi^4$ model etc.
Understanding microscopic heat conduction in thin films is important for nano/micro heat transfer and thermal management for advanced electronics. As the thickness of thin films is comparable to or shorter than a phonon wavelength, phonon dispersion relations and transport properties are significantly modulated, which should be taken into account for heat conduction in thin films. Although phonon confinement and depletion effects have been considered, it should be emphasized that surface-localized phonons (surface phonons) arise whose influence on heat conduction may not be negligible due to the high surface-to-volume ratio. However, the role of surface phonons in heat conduction has received little attention thus far. In the present work, we performed anharmonic lattice dynamics calculations to investigate the thickness and temperature dependence of in-plane thermal conductivity of silicon thin films with sub-10-nm thickness in terms of surface phonons. Through systematic analysis of the influences of surface phonons, we found that anharmonic coupling between surface and internal phonons localized in thin films significantly suppresses overall in-plane heat conduction in thin films. We also discovered that specific low-frequency surface phonons significantly contribute to surface--internal phonon scattering and heat conduction suppression. Our findings are beneficial for the thermal management of electronics and phononic devices and may lead to surface phonon engineering for thermal conductivity control.
Nuclear resonant inelastic x-ray scattering on quartz structured 57FePO4 as a function of pressure, up to 8 GPa reveals hardening of the low-energy phonons under applied pressures up to 1.5 GPa, followed by a large softening at 1.8 GPa upon approaching the phase transition pressure of ~2 GPa. The pressure-induced phase transitions in quartz-structured compounds have been predicted to be related to a soft phonon mode at the Brillouin-zone boundary (1/3, 1/3, 0) and to the break-down of the Born-stability criteria. Our results provide the first experimental evidence of this predicted phonon softening.