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Abstract While ∼30% of materials are reported to be topological, topological insulators are rare. Magnetic topological insulators (MTI) are even harder to find. Identifying crystallographic features that can host the coexistence of a topological insulating phase with magnetic order is vital for finding intrinsic MTI materials. Thus far, most materials that are investigated for the determination of an MTI are some combination of known topological insulators with a magnetic ion such as MnBi₂Te₄. Motivated by the recent success of EuIn₂As₂, the role of chemical pressure on topologically trivial insulator is investigated, Eu₅In₂Sb₆via Ga substitution. Eu₅Ga₂Sb₆is predicted to be topological but is synthetically difficult to stabilize. The intermediate compositions between Eu₅In₂Sb₆and Eu₅Ga₂Sb₆are observed through theoretical works to explore a topological phase transition and band inversion mechanism. The band inversion mechanism is attributed to changes in Eu–Sb hybridization as Ga is substituted for In due to chemical pressure. Eu₅In_4/3Ga_2/3Sb₆is also synthesized, the highest Ga concentration in Eu₅In_2‐xGa_xSb₆, and report the thermodynamic, magnetic, transport, and Hall properties. Overall, the work paints a picture of a possible MTI via band engineering and explains why Eu‐based Zintl compounds are suitable for the co‐existence of magnetism and topology. 

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. 

Abstract Advancements in low‐dimensional functional device technology heavily rely on the discovery of suitable materials which have interesting physical properties as well as can be exfoliated down to the 2D limit. Exfoliable high‐mobility magnets are one such class of materials that, not due to lack of effort, has been limited to only a handful of options. So far, most of the attention has been focused on the van der Waals (vdW) systems. However, even within the non‐vdW, layered materials, it is possible to find all these desirable features. Using chemical reasoning, it is found that NdSb₂is an ideal example. Even with a relatively small interlayer distance, this material can be exfoliated down to few layers. NdSb₂has an antiferromagnetic ground state with a quasi 2D spin arrangement. The bulk crystals show a very large, non‐saturating magnetoresistance along with highly anisotropic electronic transport properties. It is confirmed that this anisotropy originates from the 2D Fermi pockets which also imply a rather quasi 2D confinement of the charge carrier density. Both electron and hole‐type carriers show very high mobilities. The possible non‐collinear spin arrangement also results in an anomalous Hall effect.