Pressure is an effective way to regulate physical properties of ABO3 perovskites, such as thermal conductivity κ of SrTiO3, which can enhance fundamental understanding of structure–property relationships. In this Letter, κ of SrTiO3 was investigated up to ∼20 GPa using high-pressure time domain thermoreflectance together with Raman spectroscopy and first-principles calculations. Our theoretical predictions effectively explain the measured results. In both cubic and tetragonal phases, κ increased with compression, and optical phonons are the dominant heat carriers. The phonon group velocity and relaxation time make prominent contributions to κ with compression in the cubic phase, while the reduction in the anharmonicity of phonon modes and the phonon scattering channels dominates the increase in κ in the tetragonal phase. Especially, during the transition from cubic to tetragonal phases, there is a significant drop in κ, which originally results from the TiO6 octahedral distortion induced by the soft-phonon-mode, which markedly reduces the phonon group velocity. Our results not only help reveal the pressure effect on κ of complex oxides but also pave their way for applications on high-temperature superconductors and spin devices.
Nanofilms (NFs) have been widely used in many emerging applications, such as microelectronic devices, spintronics, and optical instruments. Characterizing the thermal conductivity (k) of NFs, kNFs, is nontrivial for both fundamental science and industrial applications. Time-domain thermoreflectance (TDTR) is a powerful technique for thermal characterizations under nano-to-micro-scales. However, both the kNFs and the interface thermal resistance between layers are generally unknown parameters when analyzing TDTR signals. So that an effective thermal resistance model (ETRM) is often utilized, where the impact of heat capacity of NFs, cNFs, has been always ignored. Previous studies have proposed viewpoints on how to validate this assumption, however, which still needs to be verified further by considering the parameters' sensitivities for TDTR signals. In this work, we have highlighted the significance of sensitivity analysis for the investigation of the impact of cNFs with the example experiments on Ni NFs. The error of ETRM has been quantitatively and systematically studied. We found that the application requirements of ETRM in TDTR data analysis rely on the sensitivity relations between kNFs and interface thermal resistance. Finally, suggestions for future characterization of the kNFs have been discussed for reference. Our results and conclusions deepen the understanding of both the transient thermal transport process of multilayer NFs and the ability of TDTR on characterizing kNFs.
The thickness of the metal-transducer nano-film is an essential parameter for high-pressure time-domain-thermoreflectance (TDTR) measurements. In this article, an accurate method was proposed to determine the transducer thickness in high-pressure conditions using the pressure–volume equation of state combined with an image processing method. Both the elastic and plastic deformation of the sample squeezed in diamond anvil cells were considered in this method. High-pressure TDTR measurements on thermal conductivity of MgO and mica were further taken for comparing the influence from different thickness-characterization methods up to ∼18 GPa, and the proposed method accurately captured the effect of plastic deformation on thermal conductivity for the first time. This work can not only help achieve more accurate TDTR measurements under high-pressure but also provide valuable guidance for the diamond anvil cell application in nanoscale research.
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