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Structural and dielectric properties of prepared PbS and PbTe nanomaterials
摘要： In this work, PbS and PbTe nanomaterials with various morphologies were synthesized by a hydrothermal method. The structural properties were investigated by using X-ray diffraction (XRD) and corresponding scanning electron microscopy together with their EDX analysis. Both the PbS and PbTe nanomaterials possess good polycrystalline structure. The crystallite size, determined from the XRD data, of PbS is 5 nm whereas the corresponding value of PbTe is 2.69 nm. SEM micrographs reveal that the prepared PbS nanomaterial has star-shaped structures, micro-flowers, some cubes, and semi-dendrites, whereas PbTe has semi-flower structures. Additionally, the dielectric properties have been studied in a broad frequency range from 0.1 Hz up to 1 MHz at temperatures from 298–423 K. The real and imaginary parts of the complex dielectric constant ε' and ε'' of PbTe are comparatively higher than those of PbS. Moreover, the dielectric data were analyzed on the basis of the electric modulus.
关键词： electric modulus,PbS,EDX,PbTe,dielectric properties,SEM
更新于2025-09-23 15:23:52
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Sharp increase in the density of states in PbTe upon approaching a saddle point in the band structure
摘要： PbTe is a leading mid-range thermoelectric material with a zT that has been enhanced by, amongst other methods, band engineering. Here we present an experimental study of the Hall effect, quantum oscillations, specific heat, and electron microprobe analysis that explores the evolution of the electronic structure of PbTe heavily doped with the 'ideal' acceptor Na up to the solubility limit. We identify two phenomenological changes that onset as the electronic structure deviates from a Kane-type dispersion at around 180 meV; a qualitative change in the field dependence of the Hall effect indicative of an increase in the high-field limit and a change in the Fermiology, and a sharp increase in the density of states as a function of energy. Following consideration of three possible origins for the observed phenomenology we conclude that the most likely source is nonellipsoidicity of the L pocket upon approach to a saddle point in the band structure, which is evidenced directly by our quantum oscillation measurements. Comparison to density functional theory calculations imply that this evolution of the electronic structure may be a key contributor to the large thermopower in PbTe.
关键词： band structure,PbTe,Hall effect,density of states,thermoelectric,quantum oscillations
更新于2025-09-23 15:23:52
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-type PbTe from first principles
摘要： We present an ab initio study that identifies the main electron-phonon scattering channels in n-type PbTe. We develop an electronic transport model based on the Boltzmann transport equation within the transport relaxation time approximation, fully parametrized from first-principles calculations that accurately describe the dispersion of the electronic bands near the band gap. Our computed electronic mobility as a function of temperature and carrier concentration is in good agreement with experiments. We show that longitudinal optical phonon scattering dominates electronic transport in n-type PbTe, while acoustic phonon scattering is relatively weak. We find that scattering due to soft transverse optical phonons is by far the weakest scattering mechanism, due to the symmetry-forbidden scattering between the conduction band minima and the zone center soft modes. Soft phonons thus play the key role in the high thermoelectric figure of merit of n-type PbTe: they do not degrade its electronic transport properties although they strongly suppress the lattice thermal conductivity. Our results suggest that materials like PbTe with soft modes that are weakly coupled with the electronic states relevant for transport may be promising candidates for efficient thermoelectric materials.
关键词： electron-phonon scattering,transport relaxation time approximation,thermoelectric materials,Boltzmann transport equation,n-type PbTe
更新于2025-09-23 15:21:01
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Probing of Thermal Transport in 50-nm Thick PbTe Nanocrystal Film by Time-Domain Thermoreflectance
摘要： Bottom-up fabrication of thermoelectric (TE) materials from colloidal nanocrystal (NC) building blocks can substantially increase their TE efficiency, e.g., by reducing lattice thermal conductivity. In this work, 10-nm spherical phase-pure oleate-capped PbTe NCs with narrow size distribution were synthesized and employed to fabricate 50-nm thick films on insulating SiO2/Si substrates. The spin-coating, with subsequent ligand exchange procedure, was applied to enhance coupling interactions between the NCs. Using dark conductivity measurements, we confirmed the semiconducting behavior and the Schottky-type electrical field-dependent conductivity mechanism in the resultant thin films. The thermal transport in the thin-film was probed by means of a time-domain thermoreflectance (TDTR) method. For this purpose, we used a customized state-of-the-art system based on a picosecond thermoreflectance instrument, which enables area-selective analysis with spatial resolution down to 5 μm. The results show that as-fabricated PbTe NC films exhibit ultralow thermal conductivity of 0.9 W m–1 K–1 at 300 K. The transport property findings suggest potential in the proposed quick and cost-effective spin-coating strategy for bottom-up fabrication of nanostructured TE films from high-quality colloidal NC building blocks.
关键词： colloidal nanocrystals,spin-coating,thermoelectric materials,thermal conductivity,time-domain thermoreflectance,PbTe
更新于2025-09-23 15:21:01
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The mechanochemical synthesis of PbTe nanostructures: following the Ostwald ripening effect during milling
摘要： A fundamental understanding of the Ostwald ripening effect (ORE) during the mechanochemical synthesis of PbTe nanostructures is presented. The ripening process involves the coarsening of larger particles from those of smaller size; this phenomenon was systematically evaluated at different stages of milling by microscopy analyses (AFM, TEM, STEM and HRTEM). At the early stage of milling, smaller particles and quantum dots are eventually dissolved to lower the total energy associated with their surfaces. The ripening process – during milling – involves short-range mass transfer among particles. HRTEM analyses allowed us to identify that coarsening occurs by thermo-mechanically activated cooperative mechanisms. The detachment of the atoms from smaller particles to form bigger ones plays a major role in the particle coarsening. It was found that the coarsening process was not limited to crystalline nanostructures; so grain boundaries, edge dislocations and boundaries among crystalline and amorphous phases also play an important role to determine how species migration contributes to generate coarse particles. Those serve as sites for inducing coarsening in an equivalent way as surfaces do. Secondary ion mass spectrometry and elemental chemical mapping (EDX-STEM) revealed that both the purity and the chemical homogeneity of the PbTe nanostructures are prominent features of this material. Additionally, a direct band gap enhancement (780 nm) compared to bulk PbTe (3859 nm) was detected. It occurred due to the quantum confinement effect, lattice imperfections and even surface properties of the nanostructures. It is important to point out that the whole optical behaviour of the PbTe nanostructures was dependent upon the embedded nanoparticles and quantum dots in the clusters and coarse particles ranging from 15 nm to 35 nm.
关键词： PbTe nanostructures,microscopy analyses,quantum confinement effect,mechanochemical synthesis,Ostwald ripening effect,high-energy milling
更新于2025-09-19 17:15:36
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Synthesis of ultra-narrow PbTe nanorods with extremely strong quantum confinement
摘要： Monodisperse, high-quality, ultra-narrow PbTe nanorods were synthesized for the first time in a one-pot, hot-injection reaction using trans-2-decenoic acid as the agents for lead precursors and tris(diethylamino)phosphine as the telluride precursors. High monomer reactivity, rapid nucleation and fast growth rate derived from the new precursors led to the anisotropic growth of PbTe nanocrystals at low reaction temperatures (< 150 oC). In addition, the aspect ratio of PbTe nanorods could be largely adjusted from 4 to 15 by tuning the Pb to Te precursor molar ratio and reaction temperatures. Moreover, the synthesized ultra-narrow PbTe nanorods exhibited extremely strong quantum confinement and presented unique optical properties. We revealed that the diameter and length of PbTe nanorods could significantly affect their optical properties, which potentially offer them new opportunities in the application of optoelectronic and thermoelectric devices and make them desired subjects for multiple exciton generation and other fundamental physics studies.
关键词： optical properties,PbTe nanorods,Colloidal semiconductor nanocrystals
更新于2025-09-10 09:29:36