Correlated quantum phenomena in one-dimensional (1D) systems that exhibit competing electronic and magnetic order are of strong interest for the study of fundamental interactions and excitations, such as Tomonaga–Luttinger liquids and topological orders and defects with properties completely different from the quasiparticles expected in their higher-dimensional counterparts. However, clean 1D electronic systems are difficult to realize experimentally, particularly for magnetically ordered systems. Here, we show that the van der Waals layered magnetic semiconductor CrSBr behaves like a quasi-1D material embedded in a magnetically ordered environment. The strong 1D electronic character originates from the Cr–S chains and the combination of weak interlayer hybridization and anisotropy in effective mass and dielectric screening, with an effective electron mass ratio of m X e/m Y e ∼ 50. This extreme anisotropy experimentally manifests in strong electron–phonon and exciton–phonon interactions, a Peierls-like structural instability, and a Fano resonance from a van Hove singularity of similar strength to that of metallic carbon nanotubes. Moreover, because of the reduced dimensionality and interlayer coupling, CrSBr hosts spectrally narrow (1 meV) excitons of high binding energy and oscillator strength that inherit the 1D character. Overall, CrSBr is best understood as a stack of weakly hybridized monolayers and appears to be an experimentally attractive candidate for the study of exotic exciton and 1D-correlated many-body physics in the presence of magnetic order.
Understanding the stability limitations and defect formation mechanisms in 2D magnets is essential for their utilization in spintronic and memory technologies. Here, defects in mono‐ to multilayer CrSBr are correlated with structural, vibrational, and magnetic properties. Resonant Raman scattering is used to reveal distinct vibrational defect signatures. In pristine CrSBr, it is shown that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. Environmental exposure is shown to cause drastic degradation in monolayers, with the formation of intralayer defects. This is in contrast to multilayers that predominantly show bromine surface defects. Through deliberate ion irradiation, the formation of defect modes is tuned: these are strongly polarized and resonantly enhanced, reflecting the quasi‐‐1D electronic character of CrSBr. Strikingly, pronounced signatures of spin‐phonon coupling of the intrinsic phonon modes and the ion beam‐induced defect modes are observed throughout the magnetic transition temperature. Overall, defect engineering of magnetic properties is possible, with resonant Raman spectroscopy serving as a direct fingerprint of magnetic phases and defects in CrSBr.
Low‐temperature ceramic proton conductors such as ceria are important for applications ranging from sensors and resistive switches to new devices like implantable solid‐oxide glucose fuel cells. Spray pyrolysis offers a promising fabrication route for proton‐conducting ceria, with direct liquid‐to‐solid synthesis and control over crystallinity and grain size. To date, there are conflicting reports on ceria's proton conduction mechanism, particularly whether the interior contributes to proton conduction or transport occurs exclusively along a surface water layer. In this work, proton conductivity is observed in sprayed ceria thin films at 125 °C and below. Post‐annealed films exhibit higher conductivity than as‐deposited films of 3.3 × 10−5 S cm−1 at 25 °C, which is comparable to previous reports and ascribed to the increase in crystallinity and grain size by post‐annealing. This indicates that the interior of ceria in fact contributes to proton conduction. Remarkably slow hydration kinetics of ceria are observed, with time‐dependent conductivity equilibrating to 9.53 × 10−6 S cm−1 after up to 76 h. This implies kinetics may have suppressed proton conduction in previous studies, explaining the strong fluctuations in reports to date. Slow protonation kinetics must be considered when designing functional ceria ceramics, for example, in electrochemical bio‐energy conversion, sensing or neuromorphic computing.
Ceria thin films deposited by spray pyrolysis show a strong preferential 〈200〉 orientation after annealing corresponding to the {100} facet of high catalytic activity. This texture correlates with an unusually strong blue shift of the Raman F2g peak.
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