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Superlattice formation dictates the physical properties of many materials, including the nature of the ground state in magnetic materials. Chemical composition is commonly considered to be the primary determinant of superlattice identity, especially in intercalation compounds. Here, we find that, contrary to this conventional wisdom, kinetic control of superlattice growth leads to the coexistence of disparate domains within a compositionally "perfect" single crystal. We demonstrate that Cr$_{1/4}$TaS$_2$ is a bulk noncollinear antiferromagnet in which scattering between bulk and minority superlattice domains engenders complex magnetotransport below the N\'{e}el temperature, including an anomalous Hall effect. We characterize the magnetic phases in different domains, image their nanoscale morphology, and propose a mechanism for nucleation and growth. These results provide a blueprint for the deliberate engineering of macroscopic transport responses via microscopic patterning of magnetic exchange interactions in superlattice domains., Comment: 50 pages, 19 figures, 6 tables

The construction of thin film heterostructures has been a widely successful archetype for fabricating materials with emergent physical properties. This strategy is of particular importance for the design of multilayer magnetic architectures in which direct interfacial spin--spin interactions between magnetic phases in dissimilar layers lead to emergent and controllable magnetic behavior. However, crystallographic incommensurability and atomic-scale interfacial disorder can severely limit the types of materials amenable to this strategy, as well as the performance of these systems. Here, we demonstrate a method for synthesizing heterostructures comprising magnetic intercalation compounds of transition metal dichalcogenides (TMDs), through directed topotactic reaction of the TMD with a metal oxide. The mechanism of the intercalation reaction enables thermally initiated intercalation of the TMD from lithographically patterned oxide films, giving access to a new family of multi-component magnetic architectures through the combination of deterministic van der Waals assembly and directed intercalation chemistry.

Some magnetic systems display a shift in the center of their magnetic hysteresis loop away from zero field, a phenomenon termed exchange bias. Despite the extensive use of the exchange bias effect, particularly in magnetic multilayers, for the design of spin-based memory/electronics devices, a comprehensive mechanistic understanding of this effect remains a longstanding problem. Recent work has shown that disorder-induced spin frustration might play a key role in exchange bias, suggesting new materials design approaches for spin-based electronic devices that harness this effect. Here, we design a spin glass with strong spin frustration induced by magnetic disorder by exploiting the distinctive structure of Fe intercalated ZrSe2, where Fe(II) centers are shown to occupy both octahedral and tetrahedral interstitial sites and to distribute between ZrSe2 layers without long-range structural order. Notably, we observe behavior consistent with a magnetically frustrated, and multi-degenerate ground state in these Fe0.17ZrSe2 single crystals, which persists above room temperature. Moreover, this magnetic frustration leads to a robust and tunable exchange bias up to 250 K. These results not only offer important insights into the effects of magnetic disorder and frustration in magnetic materials generally, but also highlight as design strategy the idea that a large exchange bias can arise from an inhomogeneous microscopic environment without discernible long-range magnetic order. In addition, these results show that intercalated TMDs like Fe0.17ZrSe2 hold potential for spintronics technologies that can achieve room temperature applications., Comment: Manuscript, 22 pages, 6 figures; Supporting information, 41 pages, 19 figures

Magnetic materials with noncollinear spin textures are promising for spintronic applications. To realize practical devices, control over the length and energy scales of such spin textures is imperative. The chiral helimagnets Cr1/3NbS2 and Cr1/3TaS2 exhibit analogous magnetic phase diagrams with different real-space periodicities and field dependence, positioning them as model systems for studying the relative strengths of the microscopic mechanisms giving rise to exotic spin textures. Here, we carry out a comparative study of the electronic structures of Cr1/3NbS2 and Cr1/3TaS2 using angle-resolved photoemission spectroscopy and density functional theory. We show that bands in Cr1/3TaS2 are more dispersive than their counterparts in Cr1/3NbS2 and connect this result to bonding and orbital overlap in these materials. We also unambiguously distinguish exchange splitting from surface termination effects by studying the dependence of their photoemission spectra on polarization, temperature, and beam size. We find strong evidence that hybridization between intercalant and host lattice electronic states mediates the magnetic exchange interactions in these materials, suggesting that band engineering is a route toward tuning their spin textures. Overall, these results underscore how the modular nature of intercalated transition metal dichalcogenides translates variation in composition and electronic structure to complex magnetism., Comment: 46 pages, 18 figures, 5 tables

Two-dimensional (2D) magnetic crystals hold promise for miniaturized and ultralow power electronic devices that exploit spin manipulation. In these materials, large, controllable magnetocrystalline anisotropy is a prerequisite for the stabilization and manipulation of long-range magnetic order. In known 2D magnetic crystals, relatively weak magnetocrystalline anisotropy results in typically soft ferromagnetism. Here, we demonstrate that ferromagnetic order persists down to the thinnest limit of Fe$_x$TaS$_2$ (Fe-intercalated bilayer 2H-TaS$_2$) with giant coercivities up to 3 tesla. We prepare Fe-intercalated TaS$_2$ by chemical intercalation of van der Waals layered 2H-TaS$_2$ crystals and perform variable-temperature quantum transport, transmission electron microscopy, and confocal Raman spectroscopy measurements to shed new light on the coupled effects of dimensionality, degree of intercalation, and intercalant order/disorder on the hard ferromagnetic behavior of Fe$_x$TaS$_2$. More generally, we show that chemical intercalation gives access to a rich synthetic parameter space for low-dimensional magnets, in which magnetic properties can be tailored by the choice of the host material and intercalant identity/amount, in addition to the manifold distinctive degrees of freedom available in atomically thin, van der Waals crystals.

We report on the evolution of the thermal metal-insulator transition in polycrystalline samples of Nd$_2$Ir$_2$O$_7$ upon hole-doping via substitution of Ca$^{2+}$ for Nd$^{3+}$. Ca substitution mediates a filling-controlled Mott-like transition with minimal resolvable structural changes and without altering site symmetry. Local structure confirms that Ca substitution does not result in local chemical phase separation, and absorption spectroscopy establishes that Ir cations maintain a spin-orbit entangled electronic configuration. The metal-insulator transition coincides with antiferromagnetic ordering on the Ir sublattice for all measured samples, and both decrease in onset temperature with Ca content. Weak low-temperature upturns in susceptibility and resistivity for samples with high Ca content suggest that Nd sublattice antiferromagnetism continues to couple to carriers in the metallic regime., Comment: 10 pages, 7 figures