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  1. Abstract

    Dirac and Weyl semimetals are a central topic of contemporary condensed matter physics, and the discovery of new compounds with Dirac/Weyl electronic states is crucial to the advancement of topological materials and quantum technologies. Here we show a widely applicable strategy that uses high configuration entropy to engineer relativistic electronic states. We take theAMnSb2(A= Ba, Sr, Ca, Eu, and Yb) Dirac material family as an example and demonstrate that mixing of Ba, Sr, Ca, Eu and Yb at theAsite generates the compound (Ba0.38Sr0.14Ca0.16Eu0.16Yb0.16)MnSb2(denoted asA5MnSb2), giving access to a polar structure with a space group that is not present in any of the parent compounds.A5MnSb2is an entropy-stabilized phase that preserves its linear band dispersion despite considerable lattice disorder. Although bothA5MnSb2andAMnSb2have quasi-two-dimensional crystal structures, the two-dimensional Dirac states in the pristineAMnSb2evolve into a highly anisotropic quasi-three-dimensional Dirac state triggered by local structure distortions in the high-entropy phase, which is revealed by Shubnikov–de Haas oscillations measurements.

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  2. Abstract

    There is tremendous interest in employing collective excitations of the lattice, spin, charge, and orbitals to tune strongly correlated electronic phenomena. We report such an effect in a ruthenate, Ca3Ru2O7, where two phonons with strong electron-phonon coupling modulate the electronic pseudogap as well as mediate charge and spin density wave fluctuations. Combining temperature-dependent Raman spectroscopy with density functional theory reveals two phonons,B2PandB2M, that are strongly coupled to electrons and whose scattering intensities respectively dominate in the pseudogap versus the metallic phases. TheB2Psqueezes the octahedra along the out of planec-axis, while theB2Melongates it, thus modulating the Ru 4d orbital splitting and the bandwidth of the in-plane electron hopping; Thus,B2Popens the pseudogap, whileB2Mcloses it. Moreover, theB2phonons mediate incoherent charge and spin density wave fluctuations, as evidenced by changes in the background electronic Raman scattering that exhibit unique symmetry signatures. The polar order breaks inversion symmetry, enabling infrared activity of these phonons, paving the way for coherent light-driven control of electronic transport.

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    Free, publicly-accessible full text available December 1, 2024
  3. Thermal rectification is an asymmetric heat transfer process where directionally dependent transport occurs along a given axis. In this work, geometric parameters that govern thermal rectification in solids composed of various semiconducting materials were investigated utilizing metalattice data for seven materials with pore sizes ranging between 2 and 30 nm. Using numerical simulation, thermal rectification was calculated at different thermal biases in single material systems, including silicon, cubic boron nitride, and diamond, among others. The largest thermal rectification for each material was exhibited in bilayer sample stacks that were thermally matched (i.e., the thermal resistance of each layer in the stack is equal in either forward or reverse direction). Of the materials tested, diamond provided the highest thermal rectification for all cases, with its best case achieving a thermal rectification of 57.2%. This novel thermal functionality will find application in advanced applications for temperature regulation, including resonator systems where thermal effects may significantly alter and/or degrade performance. 
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  4. Oxides of p-block metals (e.g., indium oxide) and semimetals (e.g., antimony oxide) are of broad practical interest as transparent conductors and light absorbers for solar photoconversion due to the tunability of their electronic conductivity and optical absorption. Comparatively, these oxides have found limited applications in solar-to-hydrogen photocatalysis primarily due to their high electronegativity, which impedes electron transfer for converting protons into molecular hydrogen. We have shown recently that inserting s-block metal cations into p-block oxides is effective at lowering electronegativities while affording further control of band gaps. Here, we explain the origins of this dual tunability by demonstrating the mediator role of s-block metal cations in modulating orbital hybridization while not contributing to frontier electronic states. From this result, we carry out a comprehensive computational study of 109 ternary oxides of s- and p-block metal elements as candidate photocatalysts for solar hydrogen generation. We downselect the most desirable materials using band gaps and band edges obtained from Hubbard-corrected density-functional theory with Hubbard parameters computed entirely from first principles, evaluate the stability of these oxides in aqueous conditions, and characterize experimentally four of the remaining materials, synthesized with high phase uniformity, to assess the accuracy of computational predictions. We thus propose seven oxide semiconductors, including CsIn3O5, Sr2In2O5, and KSbO2 which, to the extent of our literature review, have not been previously considered as water-splitting photocatalysts. 
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