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- Nature Communications
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Observation of suppressed diffuson and propagon thermal conductivity of hydrogenated amorphous silicon filmsHydrogenated amorphous silicon (a-Si:H) has drawn keen interest as a thin-film semiconductor and superb passivation layer in high-efficiency silicon solar cells due to its low cost, low processing temperature, high compatibility with substrates, and scalable manufacturing. Although the impact of hydrogenation on the structural, optical, and electronic properties of a-Si:H has been extensively studied, the underlying physics of its impact on the thermal properties is still unclear. Here, we synthesize a-Si:H films with well-controlled hydrogen concentrations using plasma-enhanced chemical vapor deposition and systematically study the thermal conductivity of these a-Si:H films using time-domain thermoreflectance. We find that the reduction of thermal conductivity of a-Si:H films is attributed to the suppression of diffuson and propagon contributions as the hydrogen concentration increases. At the maximum hydrogen concentration of 25.4 atomic percentage, the contributions from diffusons and propagons to the thermal conductivity are decreased by 40% (from 1.10 to 0.67 W m −1 K −1 ) and 64% (from 0.61 to 0.22 W m −1 K −1 ), respectively. Such a significant reduction in the thermal conductivity of a-Si:H originates from the hydrogen induced material softening, the decrease in density, and phonon-defect scattering. The results of this work provide fundamental insights into themore »
The thermal properties of Ba 3 Cu 2 Sn 3 Se 10 were investigated by measurement of the thermal conductivity and heat capacity. The chemical bonding in this diamagnetic material was investigated using structural data from Rietveld refinement and calculated electron localization. This quaternary chalcogenide is monoclinic ( P 2 1 / c ), has a large unit cell with 72 atoms in the primitive cell, and a high local coordination environment. The Debye temperature (162 K) and average speed of sound (1666 m s −1 ) are relatively low with a very small electronic contribution to the heat capacity. Ultralow thermal conductivity (0.46 W m −1 K −1 at room temperature) is attributed to the relatively weak chemical bonding and intrinsic anharmonicity, in addition to a large unit cell. This work is part of the continuing effort to explore quaternary chalcogenides with intrinsically low thermal conductivity and identify the features that result in a low thermal conductivity.
Ultralow lattice thermal conductivity of chalcogenide perovskite CaZrSe3 contributes to high thermoelectric figure of merit
An emerging chalcogenide perovskite, CaZrSe3, holds promise for energy conversion applications given its notable optical and electrical properties. However, knowledge of its thermal properties is extremely important, e.g. for potential thermoelectric applications, and has not been previously reported in detail. In this work, we examine and explain the lattice thermal transport mechanisms in CaZrSe3using density functional theory and Boltzmann transport calculations. We find the mean relaxation time to be extremely short corroborating an enhanced phonon–phonon scattering that annihilates phonon modes, and lowers thermal conductivity. In addition, strong anharmonicity in the perovskite crystal represented by the Grüneisen parameter predictions, and low phonon number density for the acoustic modes, results in the lattice thermal conductivity to be limited to 1.17 W m−1 K−1. The average phonon mean free path in the bulk CaZrSe3sample (
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Organic–inorganic hybrids have found increasing applications for thermal management across various disciplines. Such materials can achieve thermal conductivities below the so-called “amorphous limit” of their constituents’ thermal conductivity. Despite their technological significance, a complete understanding of the origins of this thermal conductivity reduction remains elusive in these materials. In this paper, we develop a prototypical cross-linked organic–inorganic layered system, to investigate the spectral origins of its sub-amorphous thermal conductivity. Initially, we study the atomic structure of the model and find that besides polymer chain length, the relative drift of the layers governs the reduction in computed basal spacing, in agreement with experimental measurements. We, subsequently, find that organic cross-linking results in up to 40% reduction in thermal conductivity compared to inorganic samples. An in-depth investigation of vibrational modes reveals that this reduction is the result of reduced mode diffusivities, which in turn is a consequence of a vibrational mismatch between the organic and inorganic constituents. We also show that the contribution of propagating modes to the total thermal conductivity is not affected by organic cross-linking. Our approach paves the path toward a physics-informed analysis and design of a wide range of multifunctional hybrid nanomaterials for thermal management applications among others.