Manipulating a crystalline material's configurational entropy through the introduction of unique atomic species can produce novel materials with desirable mechanical and electrical properties. From a thermal transport perspective, large differences between elemental properties such as mass and interatomic force can reduce the rate at which phonons carry heat and thus reduce the thermal conductivity. Recent advances in materials synthesis are enabling the fabrication of entropy-stabilized ceramics, opening the door for understanding the implications of extreme disorder on thermal transport. Measuring the structural, mechanical, and thermal properties of single-crystal entropy-stabilized oxides, it is shown that local ionic charge disorder can effectively reduce thermal conductivity without compromising mechanical stiffness. These materials demonstrate similar thermal conductivities to their amorphous counterparts, in agreement with the theoretical minimum limit, resulting in this class of material possessing the highest ratio of elastic modulus to thermal conductivity of any isotropic crystal.
CeramicsHigh-entropy alloys (HEAs), consisting of five or more approximately equimolar compositions of elements, [1,2] have proven to exhibit unique physical properties such as high hardness, [3] thermal stability, [4] structural stability, [5] as well as corrosion, oxidation, and wear resistance. [6][7][8] While microstructure and mechanical properties have been extensively studied, thermal
We present experimental
measurements of the thermal boundary conductance
(TBC) from 78–500 K across isolated heteroepitaxially grown
ZnO films on GaN substrates. This data provides an assessment of the
underlying assumptions driving phonon gas-based models, such as the
diffuse mismatch model (DMM), and atomistic Green’s function
(AGF) formalisms used to predict TBC. Our measurements, when compared
to previous experimental data, suggest that TBC can be influenced
by long wavelength, zone center modes in a material on one side of
the interface as opposed to the ‘“vibrational mismatch”’
concept assumed in the DMM; this disagreement is pronounced at high
temperatures. At room temperature, we measure the ZnO/GaN TBC as 490[+150,–110]
MW m–2 K–1. The disagreement among
the DMM and AGF, and the experimental data at elevated temperatures,
suggests a non-negligible contribution from other types of modes that
are not accounted for in the fundamental assumptions of these harmonic
based formalisms, which may rely on anharmonicity. Given the high
quality of these ZnO/GaN interfaces, these results provide an invaluable,
critical, and quantitative assessment of the accuracy of assumptions
in the current state of the art computational approaches used to predict
phonon TBC across interfaces.
We present data for epitaxial thin films of the prototypical entropy-stabilized oxide (ESO), Mg 0.2 Ni 0.2 Co 0.2 Cu 0.2 Zn 0.2 O, that reveals a systematic trend in lattice parameter and properties as a function of substrate temperature during film growth with negligible changes in microstructure. A larger net Co valence in films grown at substrate temperatures below 350 °C results in a smaller lattice parameter, a smaller optical band gap, and stronger magnetic exchange bias. Observation of this phenomena suggests a complex interplay between thermodynamics and kinetics during ESO synthesis; specifically thermal history, oxygen chemical potential, and entropy. In addition to the compositional degrees of freedom available to ESO systems, subtle nuances in atomic structure at constant metallic element proportions can strongly influence properties, simultaneously complicating physical characterization and providing opportunities for property tuning and development.
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