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In this study, the effects of stress relaxation on the thermoelectric properties (carrier concentration n, Hall mobility μH, weighted mobility μW, density-of-state mass md*, Seebeck coefficient S, and thermopower factor PF) of undoped ZnO films were rationalized in terms of native defects (VO-related defects and Zni-related donors) induced through the deposition temperature (TD) during the sputtering process. All investigated ZnO films exhibited compressive stress and tended to become less compressive with increasing TD. The stress relaxation at high TD resulted in improved film crystallization and decreased native defect concentration, thus significantly enhancing md* through the reduction of intrinsic lattice defects, while less carriers were trapped and scattered by defects. Therefore, n and μ increased simultaneously (by 28 times and one order of magnitude, respectively), markedly enhancing the PF of dopant-free ZnO films. [ABSTRACT FROM AUTHOR]

Segmentation of thermoelectric (TE) materials is a widely used solution to improve the efficiency of thermoelectric generators over a wide working temperature range. However, the improvement can only be obtained with appropriate material selections. In this work, we provide an overview of the theoretical efficiency of the best performing unicouples designed from segmenting the state-of-the-art TE materials. The efficiencies are evaluated using a 1D numerical model which includes all thermoelectric effects, heat conduction, Joule effects and temperature dependent material properties, but neglects contact resistance and heat losses. The calculations are performed for a fixed cold side temperature of 300 K and different hot side temperatures of 700, 900, and 1100 K. We confirm that without taking into account the compatibility of TE materials, segmentation can even decrease the total efficiency. Choosing the TE materials carefully, one is, however, rewarded by a significant improvement in the total efficiency. [ABSTRACT FROM AUTHOR]

The performance of thermoelectric materials is typically assessed using the dimensionless figure of merit, zT. Increasing zT is challenging due to the intricate relationships between electrical and thermal transport properties. This study focuses on Y2Te3‐based thermoelectric materials, which are predicted to be promising for high‐temperature applications due to their inherently low lattice thermal conductivity. A series of Y2+xTe3 compositions with excess Y is synthesized to explore the effects on electronic and structural characteristics. Density functional theory calculations suggest that additional Y atoms increase charge carriers, thereby enhancing electrical conductivity and boosting thermoelectric performance. X‐ray diffraction analysis reveals that the presence of excess Y reduces lattice volume and alters bonding structures. Furthermore, the addition of Bi significantly enhances the power factor by promoting the segregation of elemental Bi particles and the formation of Y‐Bi‐rich grain boundaries, which improve weighted mobility. This microstructural optimization leads to a fourfold increase in the Seebeck coefficient, resulting in a peak zT of 1.23 at 973 K and a predicted maximum conversion efficiency of 10.3% under a temperature difference of 673 K. These findings highlight the potential of Y2Te3 for high‐temperature thermoelectric applications and demonstrate the effectiveness of grain boundary engineering in enhancing thermoelectric performance. [ABSTRACT FROM AUTHOR]

Lattice softening is an intricate mechanism utilized to modulate lattice thermal conductivity (κlat). However, experimental observations are often complicated by numerous factors including thermal regimes, elemental matrices, and crystalline topographies, making the fundamental mechanisms complex. In this study, the temperature gradients are meticulously harnessed during phase transitions, both in heating and cooling trajectories, to ascertain that atomic configuration acts as the paramount factor modulating phonon propagation. Within CuTeI, the predilection between the tetragonal (β) and orthorhombic (α) phases is deftly manipulated via specific thermal pathways to a juncture of 273 K. A salient 44% variance in κlat is observed consequent to a singular alteration in the structural disposition of the bridging Cu atoms. Such atomic configurations delineate pronounced differential effects on the transmission dynamics of transverse and longitudinal phonons. The theoretical analysis indicates that the transverse acoustic velocity plays a more pivotal role in dictating κlat than its longitudinal counterpart due to its greater contribution to the Grüneisen parameter. The synergistic interplay of lattice softening and anharmonicity enhancement culminates in an exceptionally diminished κlat in α‐CuTeI, registering a record low κlat of 0.21 W/(m × K) among inorganic materials dominated by phonon–phonon scattering at 273 K. The revelations proffer avant‐garde perspectives for the nuanced modulation of phonon velocities and κlat. [ABSTRACT FROM AUTHOR]

Nanostructuring to reduce thermal conductivity is among the most promising strategies for designing next‐generation, high‐performance thermoelectric materials. In practice, electrical grain boundary resistance can overwhelm the thermal conductivity reduction induced by nanostructuring, which results in worse overall performance. Since a large body of work has characterized the transport of both polycrystalline ceramics and single crystals of SrTiO3, it is an ideal material system for conducting a case study of electrical grain boundary resistance. An effective mass model is used to characterize the transport signatures of electrical grain boundary resistance and evaluate thermodynamic design principles for controlling that resistance. Treating the grain boundary as a secondary phase to the bulk crystallites explains the transport phenomena. Considering that the interface can be engineered by controlling oxygen partial pressure, temperature, and the addition of extrinsic elements into the grain boundary phase, the outlook for SrTiO3 as a nanostructured thermoelectric is promising, and the zT could be greater than 0.5 at room temperature. [ABSTRACT FROM AUTHOR]

The Ag and In co‐doped PbTe, AgnPb100InnTe100+2n (LIST), exhibits n‐type behavior and features unique inherent electronic levels that induce self‐tuning carrier density. Results show that In is amphoteric in the LIST, forming both In3+ and In1+ centers. Through unique interplay of valence fluctuations in the In centers and conduction band filling, the electron carrier density can be increased from ≈3.1 × 1018 cm−3 at 323 K to ≈2.4 × 1019 cm−3 at 820 K, leading to large power factors peaking at ≈16.0 µWcm−1 K−2 at 873 K. The lone pair of electrons from In+ can be thermally continuously promoted into the conduction band forming In3+, consistent with the amphoteric character of In. Moreover, with rising temperature, the Fermi level shifts into the conduction band, which enlarges the optical band gap based on the Moss–Burstein effect, and reduces bipolar diffusion and thermal conductivity. Adding extra Ag in LIST improves the electrical transport properties and meanwhile lowers the lattice thermal conductivity to ≈0.40 Wm−1 K−1. The addition of Ag creates spindle‐shaped Ag2Te nanoprecipitates and atomic‐scale interstitials that scatter a broader set of phonons. As a result, a maximum ZT value ≈1.5 at 873 K is achieved in Ag6Pb100InTe102 (LIST). [ABSTRACT FROM AUTHOR]

Materials with high zT over a wide temperature range are essential for thermoelectric applications. n-Type Mg 3 Sb 2 -based compounds have been shown to achieve high zT at 700 K, but their performance at low temperatures (<500 K) is compromised due to their highly resistive grain boundaries. Syntheses and optimization processes to mitigate this grain-boundary effect has been limited due to loss of Mg, which hinders a sample's n-type dopability. A Mg-vapor anneal processing step that grows a sample's grain size and preserves its n-type carrier concentration during annealing is demonstrated. The electrical conductivity and mobility of the samples with large grain size follows a phonon-scattering-dominated T -3/2 trend over a large temperature range, further supporting the conclusion that the temperature-activated mobility in Mg 3 Sb 2 -based materials is caused by resistive grain boundaries. The measured Hall mobility of electrons reaches 170 cm 2 V -1 s -1 in annealed 800 °C sintered Mg 3 + δ Sb 1.49 Bi 0.5 Te 0.01 , the highest ever reported for Mg 3 Sb 2 -based thermoelectric materials. In particular, a sample with grain size >30 mm has a zT 0.8 at 300 K, which is comparable to commercial thermoelectric materials used at room temperature (n-type Bi 2 Te 3 ) while reaching zT 1.4 at 700 K, allowing applications over a wider temperature scale., (© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)