Thermoelectric figure of merit, ZT, exceeding 2.6 at 850 K and copper electromigration inhibition have been demonstrated in indium modified Cu2Se.
The thermopower (S) and electrical conductivity (σ) in conventional semiconductors are coupled adversely through the carriers' density (n) making it difficult to achieve meaningful simultaneous improvements in both electronic properties through doping and/or substitutional chemistry. Here, we demonstrate the effectiveness of coherently embedded full-Heusler (FH) quantum dots (QDs) in tailoring the density, mobility, and effective mass of charge carriers in the n-type Ti(0.1)Zr(0.9)NiSn half-Heusler matrix. We propose that the embedded FH QD forms a potential barrier at the interface with the matrix due to the offset of their conduction band minima. This potential barrier discriminates existing charge carriers from the conduction band of the matrix with respect to their relative energy leading to simultaneous large enhancements of the thermopower (up to 200%) and carrier mobility (up to 43%) of the resulting Ti(0.1)Zr(0.9)Ni(1+x)Sn nanocomposites. The improvement in S with increasing mole fraction of the FH-QDs arises from a drastic reduction (up to 250%) in the effective carrier density coupled with an increase in the carrier's effective mass (m*), whereas the surprising enhancement in the mobility (μ) is attributed to an increase in the carrier's relaxation time (τ). This strategy to manipulate the transport behavior of existing ensembles of charge carriers within a bulk semiconductor using QDs is very promising and could pave the way to a new generation of high figure of merit thermoelectric materials.
Surfactant-free Co 3 O 4 nanostructures with various particle size ranges were synthesized via the solution combustion method using cobalt nitrate solution as a cobalt precursor and urea as a combustion fuel.Control over average particles size range was achieved by tuning the reaction ignition temperature between 300 C and 800 C. X-ray diffraction (XRD) and helium gas pycnometry indicated the formation of single phase Co 3 O 4 nanoparticles with a spinel structure. Transmission electron microscopy (TEM) studies revealed an increase of the size range from 5-8 nm to 200-400 nm for Co 3 O 4 nanoparticles synthesized at 300 C and 800 C, respectively. The corresponding decrease in the specific surface area from 39 m 2 g À1 to $2 m 2 g À1 was confirmed by gas adsorption analysis using BET techniques. Magnetic susceptibility measurements revealed a dominant antiferromagnetic (AFM) ordering and the Néel temperature decreases with a decreasing average particle size range from 31 K (200-400 nm) to 25 K (5-18 nm). Interestingly, effective magnetic moments (ranging from 4.12 m B to 6.16 m B ) substantially larger than the value of 3.9 m B expected for Co 2+ ions in the normal spinel structure of Co 3 O 4 were extracted from the inverse susceptibility data. This finding was rationalized by taking into account the disordered distribution of Co 2+ and Co 3+ ions in the Co 3 O 4 inverse spinel structures ([(Co 2+ ) 1Àx (Co 3+ ) x ] tet [(Co 2+ ) x (Co 3+ ) 2Àx ] oct O 4 ) where the inversion degree (x) depends on the synthesis temperature. Transport measurements using hot pressed pellets of Co 3 O 4 nanoparticles indicated p-type semiconducting behavior and drastic reductions in the thermal conductivity with decreasing average particle size.
The concept of band structure engineering near the Fermi level through atomic-scale alteration of a bulk semiconductor crystal structure using coherently embedded intrinsic semiconducting quantum dots provides a unique opportunity to manipulate the transport behavior of the existing ensembles of carriers within the semiconducting matrix. Here we show that in situ growth of coherent nanometer-scale full-Heusler quantum dots (fH-QDs) within the p-type Ti(0.5)Hf(0.5)CoSb(0.9)Sn(0.1) half-Heusler (hH) matrix induces a drastic decrease of the effective hole density within the hH/fH-QD nanocomposites at 300 K followed by a sharp increase with rising temperature. This behavior is associated with the formation of staggered heterojunctions with a valence band (VB) offset energy, ΔE at the hH/fH phase boundaries. The energy barrier (ΔE) discriminates existing holes with respect to their energy by trapping low energy (LE) holes, while promoting the transport of high energy (HE) holes through the VB of the fH-QDs. This "hole culling" results in surprisingly large increases in the mobility and the effective mass of HE holes contributing to electronic conduction. The simultaneous reduction in the density and the increase in the effective mass of holes resulted in large enhancements of the thermopower whereas; the increase in the mobility minimizes the drop in the electrical conductivity.
The discovery of n-type ferromagnetic semiconductors (n-FMSs) exhibiting high electrical conductivity and Curie temperature (Tc) above 300 K would dramatically improve semiconductor spintronics and pave the way for the fabrication of spin-based semiconducting devices. However, the realization of high-Tc n-FMSs and p-FMSs in conventional high-symmetry semiconductors has proven extremely difficult due to the strongly coupled and interacting magnetic and semiconducting sublattices. Here we show that decoupling the two functional sublattices in the low-symmetry semiconductor FeBi2Se4 enables unprecedented coexistence of high n-type electrical conduction and ferromagnetism with Tc ≈ 450 K. The structure of FeBi2Se4 consists of well-ordered magnetic sublattices built of [FenSe4n+2]∞ single-chain edge-sharing octahedra, coherently embedded within the three-dimensional Bi-rich semiconducting framework. Magnetotransport data reveal a negative magnetoresistance, indicating spin-polarization of itinerant conducting electrons. These findings demonstrate that decoupling magnetic and semiconducting sublattices allows access to high-Tc n- and p-FMSs as well as helps unveil the mechanism of carrier-mediated ferromagnetism in spintronic materials.
The thermoelectric behavior of n-type Sb-doped half-Heusler (HH)-full-Heusler (FH) nanocomposites with general composition Ti(0.1)Zr(0.9)Ni(1+x)Sn(0.975)Sb(0.025) (x = 0, 0.02, 0.04, 0.1) was investigated in the temperature range from 300 to 775 K. Samples used for structural characterization and transport measurements were obtained through the solid-state reaction of high purity elements at 950 °C and densification of the resulting polycrystalline powders using a uniaxial hot press. X-ray diffraction study of the powder samples suggested the formation of single-phase HH alloys regardless of the Ni concentration (x value). However, high resolution transmission electron microscopy investigation revealed the presence of spherical nanoprecipitates with a broad size distribution coherently embedded in the HH matrix. The size range and dispersion of the precipitates depend on the concentration of Ni in the starting mixture. Well dispersed nanoprecipitates with size ranging from 5 nm to 50 nm are observed in the nanocomposite with x = 0.04, while severe agglomeration of large precipitates (>50 nm) is observed in samples with x = 0.1. Hall effect measurements of various samples indicate that the carrier concentration within the Sb-doped HH matrix remains nearly constant (~7 × 10(20) cm(-3)) for samples with x = 0.02 and x = 0.04, whereas a significant increase of the carrier concentration to ~9 × 10(20) cm(-3) is observed for the sample with x = 0.1. Interestingly, only a marginal change in thermopower value is observed for various samples despite the large difference in the carrier density. In addition, the carrier mobility remains constant up to x = 0.04 suggesting that the small nanoprecipitates in these samples do not disrupt electronic transport within the matrix. Remarkably, a large reduction in the total thermal conductivity is observed for all nanocomposites, indicating the effectiveness of the embedded nanoprecipitates in scattering phonons while enabling efficient electron transfer across the matrix/inclusion interfaces.
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