Investigating the key role of carrier transport mechanism in SnSe nanoflakes with enhanced thermoelectric power factor.

A novel SnSe nanoflake system is explored for its thermoelectric properties from both experiments andab initiostudy. The nanoflakes of the low temperature phase of SnSe (Pnma) are synthesized employing a fast and efficient refluxing method followed by spark plasma sintering at two different temperatures. We report an enhanced power factor (12-67µW mK-2in the temperature range 300-600 K) in our p-type samples. We find that the prime reason for a high PF in our samples is a significantly improved electrical conductivity (1050-2180 S m-1in the temperature range 300-600 K). From ourab initioband structure calculations accompanied with the models of temperature and surface dependent carrier scattering mechanisms, we reveal that an enhanced electrical conductivity is due to the reduced carrier-phonon scattering in our samples. The transport calculations are performed using the Boltzmann transport equation within relaxation time approximation. With our combined experimental and theoretical study, we demonstrate that the thermoelectric properties of p-type Pnma-SnSe could be improved by tuning the carrier scattering mechanisms with a control over the spark plasma sintering temperature.

Intrinsically Patterned Two-Dimensional Transition Metal Halides.

Patterning and defect engineering are key methods for tuning the properties and enabling distinctive functionalities in two-dimensional (2D) materials. However, generating 2D periodic patterns of point defects in 2D materials, such as vacancy lattices that can serve as antidot lattices, has been elusive until now. Herein, we report on 2D transition metal dihalides epitaxially grown on metal surfaces featuring periodically assembled halogen vacancies that result in alternating coordination of the transition metal atom. Using low-temperature scanning probe microscopy and low-energy electron diffraction, we identified the structural properties of intrinsically patterned FeBr2 and CoBr2 monolayers grown epitaxially on Au(111). Density functional theory reveals that Br vacancies are facilitated by low formation energies, and the formation of a vacancy lattice results in a substantial decrease in the lattice mismatch with the underlying Au(111). We demonstrate that interfacial strain engineering presents a versatile strategy for controlled patterning in two dimensions with atomic precision over several hundred nanometers to solve a long-standing challenge of growing atomically precise antidot lattices. In particular, patterning of 2D materials containing transition metals provides a versatile method to achieve unconventional spin textures with noncollinear spin.

Synergistic Approach Toward a Reproducible High zT in n-Type and p-Type Superionic Thermoelectric Ag2Te.

Recently, superionic thermoelectrics have attracted enormous attention due to their ultralow thermal conductivity and high figure-of-merit (zT). However, their high zT is generally obtained deep inside the superionic phase, e.g., near 1000 K in Cu2X (X: chalcogen atom) family despite a relatively low superionic transition temperature of ∼400 K. At such high temperatures, the liquid-like flow of the metal ions results in material's degradation. Here, we present thermoelectric properties of superionic Ag2Te synthesized by various methods. The sintered Ag2Te samples are shown to exhibit an unpredictable behavior with respect to the sign of thermopower (S) in the superionic phase and the magnitude of electrical conductivity (σ). We overcome this issue using an all-room-temperature fabrication technique leading to an excellent reproducibility from one sample to another. To improve the zT of Ag2Te beyond the phonon-liquid electron-crystal limit (∼0.64 at 575 K in the ingot samples), we adopted a heirarchical nanostructuring technique, which effectively suppressed the thermal conductivity, leading to a significant improvement in the zT values for both n-type and p-type samples. We obtained zT of 1.2 in the n-type and 0.64 in the p-type Ag2Te at 570 K. These values supersede the zT of any Ag2Te previously reported. At 570 K, for our ball-milled/cold-pressed samples, the critical current density for metal-ion migration exceeds 15 A cm-2, which further confirms that Ag2Te is a promising thermoelectric material. Our results are supported by first-principles density functional theory calculations of the electronic and thermal properties.