An official website of the United States government
Abstract Fe 1+ y Te 1− x Se x is characterized by its complex magnetic phase diagram and highly orbital-dependent band renormalization. Despite this, the behavior of nematicity and nematic fluctuations, especially for high tellurium concentrations, remains largely unknown. Here we present a study of both B 1 g and B 2 g nematic fluctuations in Fe 1+ y Te 1− x Se x (0 ≤ x ≤ 0.53) using the technique of elastoresistivity measurement. We discovered that the nematic fluctuations in two symmetry channels are closely linked to the corresponding spin fluctuations, confirming the intertwined nature of these two degrees of freedom. We also revealed an unusual temperature dependence of the nematic susceptibility, which we attributed to a loss of coherence of the d x y orbital. Our results highlight the importance of orbital differentiation on the nematic properties of iron-based materials.
more »
« less
Temperature Dependent n‐Type Self Doping in Nominally 19‐Electron Half‐Heusler Thermoelectric Materials
Abstract The discovery of a semiconducting ground stateXyYZ(y= 0.8 or 0.75) in nominally 19‐electron half‐Heusler materials warrants a closer look at their apparently metallic properties that often make them good thermoelectric (TE) materials. By systematically investigating the temperature dependence of off‐stoichiometry (x) in V0.8+xCoSb, Nb0.8+xCoSb, and Ti0.75+xNiSb it is found thatxinvariably increases with increasing temperature, leading to an n‐type self‐doping behavior. In addition, there is also a large phase width (range ofx) associated with each phase that is temperature dependent. Thus, unlike in typical 18‐electron half‐Heuslers (e,g, TiNiSn), the temperature dependence of vacancy and carrier concentration (n) in nominally 19‐electron half‐Heuslers links its transport properties to synthesis conditions. The temperature dependence ofxandnare understood using density functional theory based defect energies (Ed) and phase diagrams.Edare calculated for 21 systems which can be used in predicting solubility in this family of compounds. Using this simple strategy, suitable composition and temperature synthesis conditions are devised for obtaining an optimizednto engineer TE properties in phase‐pure V0.8+xCoSb, and the previously unexplored Ta0.8+xCoSb.
more »
« less
- PAR ID:
- 10075772
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Energy Materials
- Volume:
- 8
- Issue:
- 30
- ISSN:
- 1614-6832
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
More Like this
-
-
Abstract Next‐generation electronics and energy technologies can now be developed as a result of the design, discovery, and development of novel, environmental friendly lead (Pb)‐free ferroelectric materials with improved characteristics and performance. However, there have only been a few reports of such complex materials’ design with multi‐phase interfacial chemistry, which can facilitate enhanced properties and performance. In this context, herein, novel lead‐free piezoelectric materials (1‐x)Ba0.95Ca0.05Ti0.95Zr0.05O3‐(x)Ba0.95Ca0.05Ti0.95Sn0.05O3, are reported, which are represented as (1‐x)BCZT‐(x)BCST, with demonstrated excellent properties and energy harvesting performance. The (1‐x)BCZT‐(x)BCST materials are synthesized by high‐temperature solid‐state ceramic reaction method by varyingxin the full range (x= 0.00–1.00). In‐depth exploration research is performed on the structural, dielectric, ferroelectric, and electro‐mechanical properties of (1‐x)BCZT‐(x)BCST ceramics. The formation of perovskite structure for all ceramics without the presence of any impurity phases is confirmed by X‐ray diffraction (XRD) analyses, which also reveals that the Ca2+, Zr4+, and Sn4+are well dispersed within the BaTiO3lattice. For all (1‐x)BCZT‐(x)BCST ceramics, thorough investigation of phase formation and phase‐stability using XRD, Rietveld refinement, Raman spectroscopy, high‐resolution transmission electron microscopy (HRTEM), and temperature‐dependent dielectric measurements provide conclusive evidence for the coexistence of orthorhombic + tetragonal (Amm2+P4mm) phases at room temperature. The steady transition ofAmm2crystal symmetry toP4mmcrystal symmetry with increasingxcontent is also demonstrated by Rietveld refinement data and related analyses. The phase transition temperatures, rhombohedral‐orthorhombic (TR‐O), orthorhombic‐ tetragonal (TO‐T), and tetragonal‐cubic (TC), gradually shift toward lower temperature with increasingxcontent. For (1‐x)BCZT‐(x)BCST ceramics, significantly improved dielectric and ferroelectric properties are observed, including relatively high dielectric constantεr≈ 1900–3300 (near room temperature),εr≈ 8800–12 900 (near Curie temperature), dielectric loss, tanδ≈ 0.01–0.02, remanent polarizationPr≈ 9.4–14 µC cm−2, coercive electric fieldEc≈ 2.5–3.6 kV cm−1. Further, high electric field‐induced strainS≈ 0.12–0.175%, piezoelectric charge coefficientd33≈ 296–360 pC N−1, converse piezoelectric coefficient ≈ 240–340 pm V−1, planar electromechanical coupling coefficientkp≈ 0.34–0.45, and electrostrictive coefficient (Q33)avg≈ 0.026–0.038 m4C−2are attained. Output performance with respect to mechanical energy demonstrates that the (0.6)BCZT‐(0.4)BCST composition (x= 0.4) displays better efficiency for generating electrical energy and, thus, the synthesized lead‐free piezoelectric (1‐x)BCZT‐(x)BCST samples are suitable for energy harvesting applications. The results and analyses point to the outcome that the (1‐x)BCZT‐(x)BCST ceramics as a potentially strong contender within the family of Pb‐free piezoelectric materials for future electronics and energy harvesting device technologies.more » « less
-
Abstract Transport equations for electron thermal energy in the high- β e intracluster medium (ICM) are developed that include scattering from both classical collisions and self-generated whistler waves. The calculation employs an expansion of the kinetic electron equation along the ambient magnetic field in the limit of strong scattering and assumes whistler waves with low phase speeds V w ∼ v te / β e ≪ v te dominate the turbulent spectrum, with v te the electron thermal speed and β e ≫ 1 the ratio of electron thermal to magnetic pressure. We find: (1) temperature-gradient-driven whistlers dominate classical scattering when L c > L / β e , with L c the classical electron mean free path and L the electron temperature scale length, and (2) in the whistler-dominated regime the electron thermal flux is controlled by both advection at V w and a comparable diffusive term. The findings suggest whistlers limit electron heat flux over large regions of the ICM, including locations unstable to isobaric condensation. Consequences include: (1) the Field length decreases, extending the domain of thermal instability to smaller length scales, (2) the heat flux temperature dependence changes from T e 7 / 2 / L to V w nT e ∼ T e 1 / 2 , (3) the magneto-thermal- and heat-flux-driven buoyancy instabilities are impaired or completely inhibited, and (4) sound waves in the ICM propagate greater distances, as inferred from observations. This description of thermal transport can be used in macroscale ICM models.more » « less
-
Realization of ferromagnetic (FM) interlayer coupling in magnetic topological insulators (TIs) of the MnBi 2 Te 4 family of materials (MBTs) may pave the way for realizing the high-temperature quantum anomalous Hall effect (high- T QAHE). Here we propose a generic dual d-band (DDB) model to elucidate the energy difference (Δ E = E AFM − E FM ) between the AFM and FM coupling in transition-metal (TM)-doped MBTs, where the valence of TMs splits into d-t 2g and d-e g sub-bands. Remarkably, the DDB shows that Δ E is universally determined by the relative position of the dopant (X) and Mn d-e g / t 2g bands, . If Δ E d > 0, then Δ E > 0 and the desired FM coupling is favored. This surprisingly simple rule is confirmed by first-principles calculations of hole-type 3d and 4d TM dopants. Significantly, by applying the DDB model, we predict the high- T QAHE in the V-doped Mn 2 Bi 2 Te 5 , where the Curie temperature is enhanced by doubling of the MnTe layer, while the topological order mitigated by doping can be restored by strain.more » « less
-
Grading of bandgap by alloying CdTe with selenium to form a CdSexTe1–x/CdTe‐graded bilayer device has led to a device efficiency over 19%. A CdSexTe1–xabsorber would increase the short‐circuit current due to its lower bandgap but at the expense of open‐circuit voltage. It has been demonstrated that adding a CdTe layer at the back of such a CdSexTe1–xfilm reduces the voltage deficit caused by the lower bandgap of absorber from selenium alloying while maintaining the higher short‐circuit current. This leads to a photovoltaic device that draws advantage from both materials with an efficiency greater than either of them. Herein, a detailed account using device data, ultraviolet photoelectron spectroscopy, electron microscopy, and first‐principles density functional theory modeling is provided, which shows that CdTe acts as an electron reflector for CdSexTe1–x.more » « less
