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  1. Synergizing a Large Ordinary Nernst Effect and Axis‐Dependent Conduction Polarity in Flat Band KMgBi Crystals

    Abstract The exploration of quantum materials in which an applied thermo/electrical/magnetic field along one crystallographic direction produces an anisotropic response has led to unique functionalities. Along these lines, KMgBi is a layered, narrow gap semiconductor near a critical state between multiple Dirac phases due to the presence of a flat band near the Fermi level. The valence band is highly anisotropic with minimal cross‐plane dispersion, which, in combination with an isotropic conduction band, enables axis‐dependent conduction polarity. Thermopower and Hall measurements indicate dominant p‐type conduction along the cross‐plane direction, and n‐type conduction along the in‐plane direction, leading to a significantmore » zero‐field transverse thermoelectric response when the heat flux is at an angle to the principal crystallographic directions. Additionally, a large Ordinary Nernst effect (ONE) is observed with an applied field.  It arises from the ambipolar term in the Nernst effect, whereby the Lorentz force on electrons and holes makes them drift in opposite directions so that the resulting Nernst voltage becomes a function of the difference between their partial thermopowers, greatly enhancing the ONE. It is proven that axis‐dependent polarity can synergistically enhance the ONE, in addition to leading to a zero‐field transverse thermoelectric performance.« less
  2. Axis dependent conduction polarity in the air-stable semiconductor, PdSe 2

    We establish PdSe 2 as a robust, dopable, technologically viable semiconductor model system that simultaneously exhibits dominant p-type conduction cross-plane and n-type conduction in-plane.
  3. Adiabatic and isothermal configurations for Re4Si7 transverse thermoelectric power generators

    We report that transverse thermoelectric generators (TTEGs) have the potential to overcome two challenging problems that limit the commercial application of classical thermoelectric generators (TEGs): the significant irreversible efficiency losses in the contacts and the thermal degradation of the contacts at the hot end. TTEGs are built from a single material that can generate a thermoelectric current in a direction that is orthogonal to a temperature gradient. They only require a single set of contacts that are displaced away from the hot end. Here, we experimentally explore the device design considerations for optimizing the performance of this far less exploredmore » class of thermal-to-electric generation devices. We fabricate Re4Si7 TTEGs and show that there is no measurable loss in efficiency with a single set of contacts that are midway between the hot and cold ends. We show that a new effect must be considered: the appearance of transverse thermal gradients that lead to significant differences between the performance of TTEGs implemented in isothermal and adiabatic geometries. The isothermal TTEG configuration leads to much higher device efficiencies. Overall, this work highlights how different the design of TTEGs is from that of conventional TEGs and the importance of controlling the device geometry for optimum waste heat recovery.« less
  4. Giant anomalous Nernst signal in the antiferromagnet YbMnBi2

    A large anomalous Nernst effect (ANE) is crucial for thermoelectric energy conversion applications because the associated unique transverse geometry facilitates module fabrication. Topological ferromagnets with large Berry curvatures show large ANEs; however, they face drawbacks such as strong magnetic disturbances and low mobility due to high magnetization. Herein, we demonstrate that YbMnBi2, a canted antiferromagnet, has a large ANE conductivity of ~10 A m–1 K–1 that surpasses large values observed in other ferromagnets (3–5 A m–1 K–1). The canted spin structure of Mn guarantees a non-zero Berry curvature, but generates only a weak magnetization three orders of magnitude lower thanmore » that of general ferromagnets. The heavy Bi with a large spin–orbit coupling enables a large ANE and low thermal conductivity, whereas its highly dispersive px/y orbitals ensure low resistivity. The high anomalous transverse thermoelectric performance and extremely small magnetization make YbMnBi2 an excellent candidate for transverse thermoelectrics.« less
  5. Combining Spin-Seebeck and Nernst Effects in Aligned MnBi/Bi Composites

    The spin-Seebeck effect (SSE) is an advective transport process traditionally studied in bilayers composed of a ferromagnet (FM) and a non-magnetic metal (NM) with strong spin-orbit coupling. In a temperature gradient, the flux of magnons in the FM transfers spin-angular momentum to electrons in the NM, which by the inverse spin-Hall effect generates an SSE voltage. In contrast, the Nernst effect is a bulk transport phenomenon in homogeneous NMs or FMs. These effects share the same geometry, and we show here that they can be added to each other in a new combination of FM/NM composites where synthesis via in-fieldmore » annealing results in the FM material (MnBi) forming aligned needles inside an NM matrix with strong spin-orbit coupling (SOC) (Bi). Through examination of the materials’ microstructural, magnetic, and transport properties, we searched for signs of enhanced transverse thermopower facilitated by an SSE contribution from MnBi adding to the Nernst effect in Bi. Our results indicate that these two signals are additive in samples with lower MnBi concentrations, suggesting a new way forward in the study of SSE composite materials.« less
  6. Highly efficient transverse thermoelectric devices with Re 4 Si 7 crystals

    The viability and advantages of transverse thermoelectric generators over longitudinal generators have been established using single crystal Re 4 Si 7 -based devices, showing efficiencies comparable to the best commercially-available modules.
  7. Computationally Guided Discovery of Axis-Dependent Conduction Polarity in NaSnAs Crystals

    Most electronic materials exhibit a single dominant charge carrier type, either holes or electrons, along all crystallographic directions. However, there are a small number of compounds, mostly metals, that exhibit simultaneous p-type and n-type conduction behavior along different crystallographic directions. We demonstrate that the experimental discovery of semiconductors with this axis-dependent conduction polarity can be facilitated by identifying a large anisotropy of either the electron or hole effective masses (m*) or both, providing the electron and hole masses dominate along different crystallographic directions. We calculated the layered semiconductor NaSnAs to have a lower electron m* in-plane than the cross-plane andmore » a very large hole m* in-plane and small hole m* cross-plane. We established the growth of >3 mm-sized NaSnAs crystals via Sn flux and confirmed the band gap to be 0.65 eV, in agreement with theory. NaSnAs exhibits p-type thermopowers cross-plane and n-type thermopowers in-plane, confirming that the large anisotropy in the effective mass at the band edges is an excellent indicator for axis-dependent conduction polarity. Altogether, this work shows that the discovery of semiconductors with such a phenomenon can be accelerated by computationally evaluating the anisotropic curvatures of the band edges, paving the way for their future discovery and application.« less
  8. Highly efficient transverse thermoelectric devices with Re 4 Si 7 crystals

    The viability and advantages of transverse thermoelectric generators over longitudinal generators have been established using single crystal Re4Si7-based devices, showing efficiencies comparable to the best commercially-available modules.
  9. Paramagnon drag in high thermoelectric figure of merit Li-doped MnTe

    Local thermal magnetization fluctuations in Li-doped MnTe are found to increase its thermopower α strongly at temperatures up to 900 K. Below the Néel temperature (TN~ 307 K), MnTe is antiferromagnetic, and magnon drag contributes αmdto the thermopower, which scales as ~T3. Magnon drag persists into the paramagnetic state up to >3 ×TN because of long-lived, short-range antiferromagnet-like fluctuations (paramagnons) shown by neutron spectroscopy to exist in the paramagnetic state. The paramagnon lifetime is longer than the charge carrier–magnon interaction time; its spin-spin spatial correlation length is larger than the free-carrier effective Bohr radius and de Broglie wavelength. Thus, tomore » itinerant carriers, paramagnons look like magnons and give a paramagnon-drag thermopower. This contribution results in an optimally doped material having a thermoelectric figure of merit ZT> 1 at T> ~900 K, the first material with a technologically meaningful thermoelectric energy conversion efficiency from a spin-caloritronic effect.« less
  10. Off-stoichiometric silver antimony telluride: An experimental study of transport properties with intrinsic and extrinsic doping

    AgSbTe2 is a thermoelectric semiconductor with an intrinsically low thermal conductivity and a valence band structure that is favorable to obtaining a high thermoelectric figure of merit zT. It also has a very small energy gap Eg ~ 7.6 ± 3 meV. As this gap is less than the thermal excitation energy at room temperature, near-intrinsic AgSbTe2 is a two carrier system having both holes (concentration p) and electrons (n). Good thermoelectric performance requires heavy p-type doping (p > > n). This can be achieved with native defects or with extrinsic doping, e.g. with transition metal element. The use ofmore » defect doping is complicated by the fact that many of the ternary Ag-Sb-Te and pseudo-binary Sb2Te3-Ag2Te phase diagrams are contradictory. This paper determines the compositional region most favorable to creating a single phase material. Through a combination of intrinsic and extrinsic doping, values of zT > 1 are achieved, though not on single-phased material. In addition, we show that thermal conductivity is not affected by defects, further demonstrating that the low lattice thermal conductivity of I-V-VI2 materials is due to an intrinsic mechanism, insensitive to changes in defect structure.« less
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