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The ternary phase, Yb14CdSb11, has been synthesized by flux and polycrystalline methods. The crystal structure is determined via single-crystal X-ray diffraction, revealing that it crystallizes in the Ca14AlSb11 structure type (I41/acd space group with unit cell parameters of a = 16.5962(2) & Aring; and c = 22.1346(5) & Aring;, 90 K, Z = 8, R1 = 2.65%, and wR2 = 4.58%). The polycrystalline form of the compound is synthesized from a stoichiometric reaction of Yb4Sb3, CdSb, Yb, and Sb. The elemental composition is confirmed using scanning electron microscopy and energy-dispersive spectroscopy, and phase purity is verified by powder X-ray diffraction. Thermoelectric measurements, including resistivity, Seebeck coefficient, thermal conductivity, Hall carrier concentration, and Hall mobility, are conducted from 300 to 1273 K. Yb14CdSb11 exhibits a peak zT = 0.90 at 1200 K. Carrier concentration and Hall mobility range from 6.99 x 1020-1.01 x 1021 cm-3 and 4.45-9.35 x 10-1 cm2 V-1 s-1, respectively. This carrier concentration is lower than that reported for the Zn or Mn analogs leading to a lower thermoelectric figure of merit at high temperatures. However, with appropriate doping, this phase should also be a promising p-type candidate for high-temperature energy conversion applications. 

The interplay of synthesis, experiments, and theory in broadening the landscape of thermoelectric materials is reported. 

The Zintl phases, Yb 14 M Sb 11 ( M = Mn, Mg, Al, Zn), are now some of the highest thermoelectric efficiency p-type materials with stability above 873 K. Yb 14 MnSb 11 gained prominence as the first p-type thermoelectric material to double the efficiency of SiGe alloy, the heritage material in radioisotope thermoelectric generators used to power NASA’s deep space exploration. This study investigates the solid solution of Yb 14 Mg 1− x Al x Sb 11 (0 ≤ x ≤ 1), which enables a full mapping of the metal-to-semiconductor transition. Using a combined theoretical and experimental approach, we show that a second, high valley degeneracy ( N v = 8) band is responsible for the groundbreaking performance of Yb 14 M Sb 11 . This multiband understanding of the properties provides insight into other thermoelectric systems (La 3− x Te 4 , SnTe, Ag 9 AlSe 6 , and Eu 9 CdSb 9 ), and the model predicts that an increase in carrier concentration can lead to zT > 1.5 in Yb 14 M Sb 11 systems. 

Accurate density functional theory calculations of the interrelated properties of thermoelectric materials entail high computational cost, especially as crystal structures increase in complexity and size. New methods involving ab initio scattering and transport (AMSET) and compressive sensing lattice dynamics are used to compute the transport properties of quaternary CaAl 2 Si 2 -type rare-earth phosphides RECuZnP 2 (RE = Pr, Nd, Er), which were identified to be promising thermoelectrics from high-throughput screening of 20 000 disordered compounds. Experimental measurements of the transport properties agree well with the computed values. Compounds with stiff bulk moduli (>80 GPa) and high speeds of sound (>3500 m s −1 ) such as RECuZnP 2 are typically dismissed as thermoelectric materials because they are expected to exhibit high lattice thermal conductivity. However, RECuZnP 2 exhibits not only low electrical resistivity, but also low lattice thermal conductivity (∼1 W m −1 K −1 ). Contrary to prior assumptions, polar-optical phonon scattering was revealed by AMSET to be the primary mechanism limiting the electronic mobility of these compounds, raising questions about existing assumptions of scattering mechanisms in this class of thermoelectric materials. The resulting thermoelectric performance ( zT of 0.5 for ErCuZnP 2 at 800 K) is among the best observed in phosphides and can likely be improved with further optimization.