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Creators/Authors contains: "Schoop, Leslie_M"

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  1. Abstract GdTe3is a layered antiferromagnet which has attracted attention due to its exceptionally high mobility, distinctive unidirectional incommensurate charge density wave (CDW), superconductivity under pressure, and a cascade of magnetic transitions between 7 and 12 K, with as yet unknown order parameters. Here, we use spin-polarized scanning tunneling microscopy to directly image the charge and magnetic orders in GdTe3. Below 7 K, we find a striped antiferromagnetic phase with twice the periodicity of the Gd lattice and perpendicular to the CDW. As we heat the sample, we discover a spin density wave with the same periodicity as the CDW between 7 and 12 K; the viability of this phase is supported by our Landau free energy model. Our work reveals the order parameters of the magnetic phases in GdTe3and shows how the interplay between charge and spin can generate a cascade of magnetic orders. 
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  2. 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. Eu5In4/3Ga2/3Sb6is also synthesized, the highest Ga concentration in Eu5In2‐xGaxSb6, 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. 
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  3. 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. 
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  4. 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. 
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  5. Abstract This study presents a new material, “HxCrS2” (denotes approximate composition) formed by proton‐exchange of NaCrS2which has a measured capacity of 728 mAh g−1with significant improvements to capacity retention, sustaining over 700 mAh g−1during cycling experiments. This is the highest reported capacity for a transition metal sulfide electrode and outperforms the most promising proposed sodium anodes to date. HxCrS2exhibits a biphasic structure featuring alternating crystalline and amorphous lamella on the scale of a few nanometers. This unique structural motif enables reversible access to Cr redox in the material resulting in higher capacities than seen in the parent structure which features only S redox. Pretreatment by proton‐exchange offers a route to materials such as HxCrS2which provide fast diffusion and high capacities for sodium‐ion batteries. 
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  6. Abstract While several magnetic topological semimetals have been discovered in recent years, their band structures are far from ideal, often obscured by trivial bands at the Fermi energy. Square‐net materials with clean, linearly dispersing bands show potential to circumvent this issue. CeSbTe, a square‐net material, features multiple magnetic‐field‐controllable topological phases. Here, it is shown that in this material, even higher degrees of tunability can be achieved by changing the electron count at the square‐net motif. Increased electron filling results in structural distortion and formation of charge density waves (CDWs). The modulation wave‐vector evolves continuously leading to a region of multiple discrete CDWs and a corresponding complex “Devil's staircase” magnetic ground state. A series of fractionally quantized magnetization plateaus is observed, which implies direct coupling between CDW and a collective spin‐excitation. It is further shown that the CDW creates a robust idealized nonsymmorphic Dirac semimetal, thus providing access to topological systems with rich magnetism. 
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  7. Abstract Van der Waals (vdW) materials are an indispensable part of functional device technology due to their versatile physical properties and ease of exfoliating to the low‐dimensional limit. Among all the compounds investigated so far, the search for magnetic vdW materials has intensified in recent years, fueled by the realization of magnetism in 2D. However, metallic magnetic vdW systems are still uncommon. In addition, they rarely host high‐mobility charge carriers, which is an essential requirement for high‐speed electronic applications. Another shortcoming of 2D magnets is that they are highly air sensitive. Using chemical reasoning, TaCo2Te2is introduced as an air‐stable, high‐mobility, magnetic vdW material. It has a layered structure, which consists of Peierls distorted Co chains and a large vdW gap between the layers. It is found that the bulk crystals can be easily exfoliated and the obtained thin flakes are robust to ambient conditions after 4 months of monitoring using an optical microscope. Signatures of canted antiferromagntic behavior are also observed at low‐temperature. TaCo2Te2shows a metallic character and a large, nonsaturating, anisotropic magnetoresistance. Furthermore, the Hall data and quantum oscillation measurements reveal the presence of both electron‐ and hole‐type carriers and their high mobility. 
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