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The previously unreported layered compounds IrTe 2 I and RhTe 2 I were prepared by a high-pressure synthesis method. Single crystal X-ray and powder X-ray diffraction studies find that the compounds are isostructural, crystallizing in a layered orthorhombic structure in the non-centrosymmetric, non-symmorphic space group Pca 2 1 (#29). Characterization reveals diamagnetic, high resistivity, semiconducting behavior for both compounds, consistent with the +3 chemical valence and d 6 electronic configurations for both iridium and rhodium and the Te–Te dimers seen in the structural study. Electronic band structures are calculated for both compounds, showing good agreement with the experimental results. 

Abstract 1D charge transport offers great insight into strongly correlated physics, such as Luttinger liquids, electronic instabilities, and superconductivity. Although 1D charge transport is observed in nanomaterials and quantum wires, examples in bulk crystalline solids remain elusive. In this work, it is demonstrated that spin‐orbit coupling (SOC) can act as a mechanism to induce quasi‐1D charge transport in the Ln₃MPn₅(Ln = lanthanide; M = transition metal; Pn = Pnictide) family. From three example compounds, La₃ZrSb₅, La₃ZrBi₅, and Sm₃ZrBi₅, density functional theory calculations with SOC included show a quasi‐1D Fermi surface in the bismuthide compounds, but an anisotropic 3D Fermi surface in the antimonide structure. By performing anisotropic charge transport measurements on La₃ZrSb₅, La₃ZrBi₅, and Sm₃ZrBi₅, it is demonstrated that SOC starkly affects their anisotropic resistivity ratios (ARR) at low temperatures, with an ARR of ≈4 in the antimonide compared to ≈9.5 and ≈22 (≈32 after magnetic ordering) in La₃ZrBi₅and Sm₃ZrBi₅, respectively. This report demonstrates the utility of spin‐orbit coupling to induce quasi‐low‐dimensional Fermi surfaces in anisotropic crystal structures, and provides a template for examining other systems.