Chan-Chieh Lin

High thermoelectric performance due to nano-inclusions and randomly distributed interface potentials in N-type (PbTe0.93−xSe0.07Clx)0.93(PbS)0.07 composites

In a composite of two dissimilar or homologous semiconductors with different energy band gaps or metal/semiconductor composites, we expect a band bending effect at the interfaces. The band bending effect induced by the different Fermi levels of two compounds can selectively scatter carriers due to energy-dependent scattering time, resulting in enhancement of the Seebeck coefficient. In addition, nano-inclusions in a matrix will effectively scatter phonons. Here, we demonstrate the effects of electron and phonon scattering by nano-inclusions in n-type (PbTe0.93−xSe0.07Clx)0.93(PbS)0.07 (x = 0.0005, 0.01, 0.1 and 0.2) composites. In the matrix, the nano-inclusions increased the Seebeck coefficient while reducing lattice thermal conductivity in (PbTe0.93−xSe0.07Clx)0.93(PbS)0.07. The chlorine doping increases the Fermi level to the bottom of the conduction band giving rise to increased electron concentration. The simultaneous emergence of the high Seebeck coefficient and low thermal conductivity resulted in the exceptional ZT value of 1.52 at 700 K for low chlorine doping (x = 0.0005), which is a very high value in n-type thermoelectric materials. The randomly distributed interface potential, induced by Fermi level tuning, with nano-inclusions is a new criterion for investigating thermoelectric properties.

Enhancement of thermoelectric properties by effective K-doping and nano precipitation in quaternary compounds of (Pb1−xKxTe)0.70(PbSe)0.25(PbS)0.05

We investigated thermoelectric properties in K-doped quaternary compounds of (Pb1−xKxTe)0.70(PbSe)0.25(PbS)0.05 (x ≤ 0.03). In terms of two valence bands model, we argue that the L-band approaches to the Σ-band with increasing the K-doping concentration resulting in the increase of carrier concentration and effective mass of carrier due to the increase of band degeneracy. The effective K-doping by x = 0.02 and PbS substitution causes high power factor and low thermal conductivity, resulting in the comparatively high ZT value of 1.72 at 800 K. The low thermal conductivity for (Pb0.98K0.02Te)0.70(PbSe)0.25(PbS)0.05 compound is attributed from the lattice distortion and line dislocation in a phase of nano precipitation. By optimizing K-doping and PbS substitution, we achieved the enhancement of practical thermoelectric performance such as average ZTavg = 1.08, engineering (ZT)eng = 0.81, maximum efficiency ηmax = 11.63%, and output power density Pd = 6.3 W cm−2, with temperature difference ΔT = 500 K, which has practical applicability in waste heat power generation technologies.

Enhancement of Thermoelectric Performance in Na-Doped Pb0.6Sn0.4Te0.95–xSexS0.05 via Breaking the Inversion Symmetry, Band Convergence, and Nanostructuring by Multiple Elements Doping

Topological insulators have attracted much interest in topological states of matter featuring unusual electrical conduction behaviors. It has been recently reported that a topological crystalline insulator could exhibit a high thermoelectric performance by breaking its crystal symmetry via chemical doping. Here, we investigate the multiple effects of Na, Se, and S alloying on thermoelectric properties of a topological crystalline insulator Pb0.6Sn0.4Te. The Na doping is known to be effective for breaking the crystalline mirror symmetry of Pb0.6Sn0.4Te. We demonstrate that simultaneous emergence of band convergence by Se alloying and nanostructuring by S doping enhance the power factor and decrease lattice thermal conductivity, respectively. Remarkably, the high power factor of 22.3 μW cm-1 K-2 at 800 K is achieved for Na 1%-doped Pb0.6Sn0.4Te0.90Se0.05S0.05 mainly due to a relatively high Seebeck coefficient via band convergence by Se alloying as well as the suppression of bipolar conduction at high temperatures by the increase of energy band gap. Furthermore, the lattice thermal conductivity is significantly suppressed by PbS nanoprecipitates without deteriorating the hole carrier mobility, ranging from 0.80 W m-1 K-1 for Pb0.6Sn0.4Te to 0.17 W m-1 K-1 at 300 K for Pb0.6Sn0.4Te0.85Se0.10S0.05. As a result, the synergistically combined effects of breaking the crystalline mirror symmetry of topological crystalline insulator, band convergence, and nanostructuring for Pb0.6Sn0.4Te0.95- xSe xS0.05 ( x = 0, 0.05, 0.1, 0.2, and 0.95) give rise to an impressively high ZT of 1.59 at 800 K for x = 0.05. We suggest that the multiple doping in topological crystalline insulators is effective for improving the thermoelectric performance.

Enhancement of thermoelectric performance via weak disordering of topological crystalline insulators and band convergence by Se alloying in Pb0.5Sn0.5Te1 − xSex

Topological crystal insulators (TCIs) that have an even number of topologically protected Dirac bands driven by crystalline mirror symmetry have attracted much attention in condensed matter physics. Here, we demonstrate that a weak disordering in the topological crystalline state can enhance thermoelectric performance significantly due to highly dispersive band dispersion and high band degeneracy which guarantee high electrical mobility and a high Seebeck coefficient, respectively. When we perturb a crystalline mirror symmetry by Se-doping in TCI Pb0.5Sn0.5Te1 − xSex, the topological state becomes weak so that it eventually evolves the normal state. We experimentally prove the topological phase transition concerning Se concentration by X-ray Absorption Spectroscopy (XAS) and extended X-ray absorption Fine Structure (EXAFS) analysis. Small crystalline perturbation by Se doping (x = 0.05) significantly enhances thermoelectric performance due to the simultaneous enhancement of electrical conductivity and the Seebeck coefficient. Therefore, we report an exceptionally high ZT value of 1.9 at 800 K for the x = 0.05 compound which is a 313% enhancement of ZT compared with the pristine compound. This research proposes a new strategy for exploring high-performance thermoelectric materials by weak disordering of topological crystalline Dirac semimetals.

Enhancement of Thermoelectric Performances in a Topological Crystal Insulator Pb0.7Sn0.3Se via Weak Perturbation of the Topological State and Chemical Potential Tuning by Chlorine Doping

Topological insulators generally share commonalities with good thermoelectric (TE) materials because of their narrow band gaps and heavy constituent elements. Here, we propose that a topological crystalline insulator (TCI) could exhibit a high TE performance by breaking its crystalline symmetry and tuning the chemical potential by elemental doping. As a candidate material, we investigate the TE properties of the Cl-doped TCI Pb0.7Sn0.3Se. The infrared absorption spectra reveal that the band gap is increased from 0.055 eV for Pb0.7Sn0.3Se to 0.075 eV for Pb0.7Sn0.3Se0.99Cl0.01, confirming that the Cl doping can break the crystalline mirror symmetry of a TCI Pb0.7Sn0.3Se and thereby enlarge its bulk electronic band gap. The topological band inversion is confirmed by the extended X-ray absorption fine structure spectroscopy, which shows that the TCI state is weakened in a chlorine x = 0.05-doped compound. The small gap opening and partial linear band dispersion with massless and massive bands may have a high power factor (PF) for high electrical conductivity with an enhancement of the Seebeck coefficient. As a result, Pb0.7Sn0.3Se0.99Cl0.01 shows a considerably enhanced ZT of 0.64 at 823 K, which is about 1200% enhancement in ZT compared with that of the undoped Pb0.7Sn0.3Se. This work demonstrates that the optimal n-type Cl doping tunes the chemical potential together with breaking the state of the TCI, suppresses the bipolar conduction at high temperatures, and thereby enables the Seebeck coefficient to increase up to 823 K, resulting in a significantly enhanced PF at high temperatures. In addition, the bipolar contribution to thermal conductivity is effectively suppressed for the Cl-doped samples of Pb0.7Sn0.3Se1- xCl x ( x ≥ 0.01). We propose that breaking the crystalline mirror symmetry in TCIs could be a new research direction for exploring high-performance TE materials.