Machine Learning for Predicting Ultralow Thermal Conductivity and High ZT in Complex Thermoelectric Materials.

Efficient and precise calculations of thermal transport properties and figures of merit, alongside a deep comprehension of thermal transport mechanisms, are essential for the practical utilization of advanced thermoelectric materials. In this study, we explore the microscopic processes governing thermal transport in the distinguished crystalline material Tl9SbTe6 by integrating a unified thermal transport theory with machine learning-assisted self-consistent phonon calculations. Leveraging machine learning potentials, we expedite the analysis of phonon energy shifts, higher-order scattering mechanisms, and thermal conductivity arising from various contributing factors, such as population and coherence channels. Our finding unveils an exceptionally low thermal conductivity of 0.31 W m-1 K-1 at room temperature, a result that closely correlates with experimental observations. Notably, we observe that the off-diagonal terms of heat flux operators play a significant role in shaping the overall lattice thermal conductivity of Tl9SbTe6, where the ultralow thermal conductivity resembles that of glass due to limited group velocities. Furthermore, we achieve a maximum ZT value of 3.17 in the c-axis orientation for p-type Tl9SbTe6 at 600 K and an optimal ZT value of 2.26 in the a-axis and b-axis direction for n-type Tl9SbTe6 at 500 K. The crystalline Tl9SbTe6 not only showcases remarkable thermal insulation but also demonstrates impressive electrical properties owing to the dual-degeneracy phenomenon within its valence band. These results not only elucidate the underlying reasons for the exceptional thermoelectric performance of Tl9SbTe6 but also suggest potential avenues for further experimental exploration.

Encyclopedia of emergent particles in three-dimensional crystals.

The past decade has witnessed a surge of interest in exploring emergent particles in condensed matter systems. Novel particles, emerged as excitations around exotic band degeneracy points, continue to be reported in real materials and artificially engineered systems, but so far, we do not have a complete picture on all possible types of particles that can be achieved. Here, via systematic symmetry analysis and modeling, we accomplish a complete list of all possible particles in time-reversal-invariant systems. This includes both spinful particles such as electron quasiparticles in solids, and spinless particles such as phonons or even excitations in electric-circuit and mechanical networks. We establish detailed correspondence between the particle, the symmetry condition, the effective model, and the topological character. This obtained encyclopedia concludes the search for novel emergent particles and provides concrete guidance to achieve them in physical systems.

n-Bi2-xSbxTe3: A Promising Alternative to Mainstream Thermoelectric Material n-Bi2Te3-xSex near Room Temperature.

For decades, the V2VI3 compounds, specifically p-type Bi2-xSbxTe3 and n-type Bi2Te3-xSex, have remained the cornerstone of commercial thermoelectric solid-state cooling and power generation near room temperature. However, a long-standing problem in V2VI3 thermoelectrics is that n-type Bi2Te3-xSex is inferior in performance to p-type Bi2-xSbxTe3 near room temperature, restricting the device efficiency. In this work, we developed high-performance n-type Bi2-xSbxTe3, a composition long thought to only make good p-type thermoelectrics, to replace the mainstream n-type Bi2Te3-xSex. The success arises from the synergy of the following mechanisms: (i) the donorlike effect, which produces excessive conduction electrons in Bi2Te3, is compensated by the antisite defects regulated by Sb alloying; (ii) the conduction band degeneracy increases from 2 for Bi2Te3 and Bi2Te3-xSex to 6 for Bi2-xSbxTe3, favoring high Seebeck coefficients; and (iii) the larger mass fluctuation yet smaller electronegativity difference and smaller atomic radius difference between Bi and Sb effectively suppresses the lattice thermal conductivity and retains decent carrier mobility. A state-of-the-art zT of 1.0 near room temperature was attained in hot deformed Bi1.5Sb0.5Te3, which is higher than those for most known n-type thermoelectric materials, including commercial Bi2Te3-xSex ingots and the popular Mg3Sb2. Technically, building both the n-leg and p-leg of a thermoelectric module using similar chemical compositions has key advantages in the mechanical strength and the durability of devices. These results attested to the promise of n-type Bi2-xSbxTe3 as a replacement of the mainstream n-type Bi2Te3-xSex near room temperature.

Combination of Carrier Concentration Regulation and High Band Degeneracy for Enhanced Thermoelectric Performance of Cu3SbSe4.

The effect of Al-, Ga-, and In-doping on the thermoelectric (TE) properties of Cu3SbSe4 has been comparatively studied on the basis of theoretical prediction and experimental validation. It is found that tiny Al/Ga/In substitution leads to a great enhancement of electrical conductivity with high carrier concentration and also large Seebeck coefficient due to the preserved high band degeneracy and thereby a remarkably high power factor. Ultimately, coupled with the depressed lattice thermal conductivity, all three elements (Al/Ga/In) substituted samples have obtained a highly improved thermoelectric performance with respect to undoped Cu3SbSe4. Compared to the samples at the same Al/In doping level, the slightly Ga-doped sample presents better TE performance over the wide temperature range, and the Cu3Sb0.995Ga0.005Se4 sample presents a record high ZT value of 0.9 among single-doped Cu3SbSe4 at 623 K, which is about 80% higher than that of pristine Cu3SbSe4. This work offers an alternative approach to boost the TE properties of Cu3SbSe4 by selecting efficient dopant to weaken the coupling between electrical conductivity and Seebeck coefficient.