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Amorphous-Like Ultralow Thermal Transport in Crystalline Argyrodite Cu7PS6
Due to their amorphous-like ultralow lattice thermal conductivity both below and above the superionic phase transition, crystalline Cu- and Ag-based superionic argyrodites have garnered widespread attention as promising thermoelectric materials. However, despite their intriguing properties, quantifying their lattice thermal conductivities and a comprehensive understanding of the microscopic dynamics that drive these extraordinary properties are still lacking. Here, an integrated experimental and theoretical approach is adopted to reveal the presence of Cu-dominated low-energy optical phonons in the Cu-based argyrodite Cu7PS6. These phonons yield strong acoustic-optical phonon scattering through avoided crossing, enabling ultralow lattice thermal conductivity. The Unified Theory of thermal transport is employed to analyze heat conduction and successfully reproduce the experimental amorphous-like ultralow lattice thermal conductivities, ranging from 0.43 to 0.58 W m−1 K−1, in the temperature range of 100–400 K. The study reveals that the amorphous-like ultralow thermal conductivity of Cu7PS6 stems from a significantly dominant wave-like conduction mechanism. Moreover, the simulations elucidate the wave-like thermal transport mainly results from the contribution of Cu-associated low-energy overlapping optical phonons. This study highlights the crucial role of low-energy and overlapping optical modes in facilitating amorphous-like ultralow thermal transport, providing a thorough understanding of the underlying complex dynamics of argyrodites.
Peculiarities of the Acoustic Wave Propagation in Diamond-Based Multilayer Piezoelectric Structures as “Me1/(Al,Sc)N/Me2/(100) Diamond/Me3” and “Me1/AlN/Me2/(100) Diamond/Me3” under Metal Thin-Film Deposition
New theoretical and experimental results of microwave acoustic wave propagation in diamond-based multilayer piezoelectric structures (MPS) as “Me1/(Al,Sc)N/Me2/(100) diamond/Me3” and “Me1/AlN/Me2/(100) diamond/Me3” under three metal film depositions, including the change in the quality factor Q as a result of Me3 impact, were obtained. Further development of our earlier studies was motivated by the necessity of creating a sensor model based on the above fifth layered MPS and its in-depth study using the finite element method (FEM). Experimental results on the change in operational checkpoint frequencies and quality factors under the effect of film deposition are in satisfactory accordance with FEM data. The relatively small decrease in the quality factor of diamond-based high overtone bulk acoustic resonator (HBAR) under the metal layer effect observed in a wide microwave band could be qualified as an important result. Changes in operational resonant frequencies vs. film thickness were found to have sufficient distinctions. This fact can be quite explained in terms of the difference between acoustic impedances of diamond and deposited metal films.
High-temperature electromechanical loss in piezoelectric langasite and catangasite crystals
Temperature-dependent acoustic loss Q−1 is studied in partially disordered langasite (LGS, La3Ga5SiO14) and ordered catangasite (CTGS, Ca3TaGa3Si2O14) crystals and compared with previously reported CTGS and langatate (LGT, La3Ga5.5Ta0.5O14) data. Two independent techniques, a contactless tone-burst excitation technique and contacting resonant piezoelectric spectroscopy, are used in this study. Contributions to the measured Q−1(T) are determined through fitting to physics-based functions, and the extracted fit parameters, including the activation energies of the processes, are discussed. It is shown that losses in LGS and CTGS are caused by a superposition of several mechanisms, including intrinsic phonon–phonon loss, point-defect relaxations, and conductivity-related relaxations.
Transport and Electromechanical Properties of Ca3TaGa3Si2O14 Piezoelectric Crystals at Extreme Temperatures
Transport mechanisms in structurally ordered piezoelectric Ca3TaGa3Si2O14 (CTGS) single crystals are studied in the temperature range of 1000-1300 °C by application of the isotope 18O as a tracer and subsequent analysis of diffusion profiles of this isotope using secondary ion mass spectrometry (SIMS). Determined oxygen self-diffusion coefficients enable calculation of oxygen ion contribution to the total conductivity, which is shown to be small. Since very low contributions of the cations have to be expected, the total conductivity must be dominated by electron transport. Ion and electron conductivities are governed by different mechanisms with activation energies (1.9±0.1) eV and (1.2±0.07) eV, respectively. Further, the electromechanical losses are studied as a function of temperature by means of impedance spectroscopy on samples with electrodes and a contactless tone-burst excitation technique. At temperatures above 650 °C the conductivity-related losses are dominant. Finally, the operation of CTGS resonators is demonstrated at cryogenic temperatures and materials piezoelectric strain constants are determined from 4.2 K to room temperature. Copyright © Materials Research Society 2019.
Unveiling the phonon scattering mechanisms in half-Heusler thermoelectric compounds
Half-Heusler (HH) compounds are among the most promising thermoelectric (TE) materials for large-scale applications due to their superior properties such as high power factor, excellent mechanical and thermal reliability, and non-toxicity. Their only drawback is the remaining-high lattice thermal conductivity. Various mechanisms were reported with claimed effectiveness to enhance the phonon scattering of HH compounds including grain-boundary scattering, phase separation, and electron–phonon interaction. In this work, however, we show that point-defect scattering has been the dominant mechanism for phonon scattering other than the intrinsic phonon–phonon interaction for ZrCoSb and possibly many other HH compounds. Induced by the charge-compensation effect, the formation of Co/4d Frenkel point defects is responsible for the drastic reduction of lattice thermal conductivity in ZrCoSb1−xSnx. Our work systematically depicts the phonon scattering profile of HH compounds and illuminates subsequent material optimizations.