Thomas C. Chasapis

High ZT in p-Type (PbTe)1–2x(PbSe)x(PbS)x Thermoelectric Materials

Lead chalcogenide thermoelectric systems have been shown to reach record high figure of merit values via modification of the band structure to increase the power factor or via nanostructuring to reduce the thermal conductivity. Recently, (PbTe)1-x(PbSe)x was reported to reach high power factors via a delayed onset of interband crossing. Conversely, the (PbTe)1-x(PbS)x was reported to achieve low thermal conductivities arising from extensive nanostructuring. Here we report the thermoelectric properties of the pseudoternary 2% Na-doped (PbTe)1-2x(PbSe)x(PbS)x system. The (PbTe)1-2x(PbSe)x(PbS)x system is an excellent platform to study phase competition between entropically driven atomic mixing (solid solution behavior) and enthalpy-driven phase separation. We observe that the thermoelectric properties of the PbTe-PbSe-PbS 2% Na doped are superior to those of 2% Na-doped PbTe-PbSe and PbTe-PbS, respectively, achieving a ZT ≈2.0 at 800 K. The material exhibits an increased the power factor by virtue of valence band modification combined with a very reduced lattice thermal conductivity deriving from alloy scattering and point defects. The presence of sulfide ions in the rock-salt structure alters the band structure and creates a plateau in the electrical conductivity and thermopower from 600 to 800 K giving a power factor of 27 μW/cmK(2). The very low total thermal conductivity values of 1.1 W/m·K of the x = 0.07 composition is accounted for essentially by phonon scattering from solid solution defects rather than the assistance of endotaxial nanostructures.

n-Type Bi2Te3–xSex Nanoplates with Enhanced Thermoelectric Efficiency Driven by Wide-Frequency Phonon Scatterings and Synergistic Carrier Scatterings

Driven by the prospective applications of thermoelectric materials, massive efforts have been dedicated to enhancing the conversion efficiency. The latter is governed by the figure of merit (ZT), which is proportional to the power factor (S(2)σ) and inversely proportional to the thermal conductivity (κ). Here, we demonstrate the synthesis of high-quality ternary Bi2Te3-xSex nanoplates using a microwave-assisted surfactant-free solvothermal method. The obtained n-type Bi2Te2.7Se0.3 nanostructures exhibit a high ZT of 1.23 at 480 K measured from the corresponding sintered pellets, in which a remarkably low κ and a shift of peak S(2)σ to high temperature are observed. By detailed electron microscopy investigations, coupled with theoretical analysis on phonon transports, we propose that the achieved κ reduction is attributed to the strong wide-frequency phonon scatterings. The shifting of peak S(2)σ to high temperature is due to the weakened temperature dependent transport properties governed by the synergistic carrier scatterings and the suppressed bipolar effects by enlarging the band gap.

Contrasting role of antimony and bismuth dopants on the thermoelectric performance of lead selenide

Increasing the conversion efficiency of thermoelectric materials is a key scientific driver behind a worldwide effort to enable heat to electricity power generation at competitive cost. Here we report an increased performance for antimony-doped lead selenide with a thermoelectric figure of merit of ~1.5 at 800 K. This is in sharp contrast to bismuth doped lead selenide, which reaches a figure of merit of <1. Substituting antimony or bismuth for lead achieves maximum power factors between ~23-27 μW cm(-1) K(-2) at temperatures above 400 K. The addition of small amounts (~0.25 mol%) of antimony generates extensive nanoscale precipitates, whereas comparable amounts of bismuth results in very few or no precipitates. The antimony-rich precipitates are endotaxial in lead selenide, and appear remarkably effective in reducing the lattice thermal conductivity. The corresponding bismuth-containing samples exhibit smaller reduction in lattice thermal conductivity.

NMR probe of metallic states in nanoscale topological insulators

A 125Te NMR study of bismuth telluride nanoparticles as a function of particle size revealed that the spin-lattice relaxation is enhanced below 33 nm, accompanied by a transition of NMR spectra from the single to the bimodal regime. The satellite peak features a negative Knight shift and higher relaxivity, consistent with core polarization from p-band carriers. Whereas nanocrystals follow a Korringa law in the range 140-420 K, micrometer particles do so only below 200 K. The results reveal increased metallicity of these nanoscale topological insulators in the limit of higher surface-to-volume ratios.

Understanding Bulk Defects in Topological Insulators from Nuclear‐Spin Interactions

Non-invasive local probes are needed to characterize bulk defects in binary and ternary chalcogenides. These defects contribute to the non-ideal behavior of topological insulators. We have studied bulk electronic properties via

Nanocomposites from Solution-Synthesized PbTe-BiSbTe Nanoheterostructure with Unity Figure of Merit at Low-Medium Temperatures (500–600 K)

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Evaporative thinning: A facile synthesis method for high quality ultrathin layers of 2D crystals

Te NMR in Bi

Understanding the role and interplay of heavy-hole and light-hole valence bands in the thermoelectric properties of PbSe

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Site‐Specific Contributions to the Band Inversion in a Topological Crystalline Insulator

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Self-Tuning n-Type Bi2(Te,Se)3/SiC Thermoelectric Nanocomposites to Realize High Performances up to 300 °C

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