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The layered, air-stable van der Waals antiferromagnetic compound CrSBr exhibits pronounced coupling between its optical, electronic, and magnetic properties. As an example, exciton dynamics can be significantly influenced by lattice vibrations through exciton-phonon coupling. Using low-temperature photoluminescence spectroscopy, we demonstrate the effective coupling between excitons and phonons in nanometer-thick CrSBr. By careful analysis, we identify that the satellite peaks predominantly arise from the interaction between the exciton and an optical phonon with a frequency of 118 cm-1 (~14.6 meV) due to the out-of-plane vibration of Br atoms. Power-dependent and temperature-dependent photoluminescence measurements support exciton-phonon coupling and indicate a coupling between magnetic and optical properties, suggesting the possibility of carrier localization in the material. The presence of strong coupling between the exciton and the lattice may have important implications for the design of light-matter interactions in magnetic semiconductors and provide insights into the exciton dynamics in CrSBr. This highlights the potential for exploiting exciton-phonon coupling to control the optical properties of layered antiferromagnetic materials.

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Photodetectors and sensors have a prominent role in our lives and cover a wide range of applications, including intelligent systems and the detection of harmful and toxic elements. Although there have been several studies in this direction, their practical applications have been hindered by slow response and low responsiveness. To overcome these problems, we have presented here a self-powered (photoelectrochemical, PEC), ultrasensitive, and ultrafast photodetector platform. For this purpose, a novel few-layered palladium–phosphorus–sulfur (PdPS) was fabricated by shear exfoliation for effective photodetection as a practical assessment. The characterization of this self-powered broadband photodetector demonstrated superior responsivity and specific detectivity in the order of 33 mA W–1 and 9.87 × 1010 cm Hz1/2 W–1, respectively. The PEC photodetector also exhibits a broadband photodetection capability ranging from UV to IR spectrum, with the ultrafast response (∼40 ms) and recovery time (∼50 ms). In addition, the novel few-layered PdPS showed superior sensing ability to organic vapors with ultrafast response and a recovery time of less than 1 s. Finally, the photocatalytic activity in the form of hydrogen evolution reaction was explored due to the suitable band alignment and pronounced light absorption capability. The self-powered sensing platforms and superior catalytic activity will pave the way for practical applications in efficient future devices.

van der Waals magnetic materials are an ideal platform to study low-dimensional magnetism. Opposed to other members of this family, the magnetic semiconductor CrSBr is highly resistant to degradation in air, which, in addition to its exceptional optical, electronic, and magnetic properties, is the reason the compound is receiving considerable attention at the moment. For many years, its magnetic phase diagram seemed to be well-understood. Recently, however, several groups observed a magnetic transition in magnetometry measurements at temperatures of around 40 K that is not expected from theoretical considerations, causing a debate about the intrinsic magnetic properties of the material. In this Letter, we report the absence of this particular transition in magnetization measurements conducted on high-quality CrSBr crystals, attesting to the extrinsic nature of the low-temperature magnetic phase observed in other works. Our magnetometry results obtained from large bulk crystals are in very good agreement with the magnetic phase diagram of CrSBr previously predicted by the mean-field theory; A-type antiferromagnetic order is the only phase observed below the Néel temperature at TN = 131 K. Moreover, numerical fits based on the Curie–Weiss law confirm that strong ferromagnetic correlations are present within individual layers even at temperatures much larger than TN.

Understanding the stability limitations and defect formation mechanisms in 2D magnets is essen- tial for their utilization in spintronic and memory technologies. Here, we correlate defects in mono- to multilayer CrSBr with their structural and vibrational properties. We use resonant Raman scattering to reveal distinct vibrational defect signatures. In pristine CrSBr, we show that bromine atoms mediate vibrational interlayer coupling, allowing for distinguishing between surface and bulk defect modes. We show that environmental exposure causes drastic degradation in monolayers, with intralayer defects forming more readily in monolayers. Through deliberate ion irradiation, we tune the formation of defect modes, which we show are strongly polarized and resonantly enhanced, reflecting the quasi-1D electronic character of CrSBr. Overall, we present a structural and vibrational study of defective CrSBr, demonstrate the air stability above the monolayer threshold, and provide further insight into the quasi-1D physics present, creating crucial understanding for defect engineering of magnetic textures.

Layered magnetic materials are becoming a major platform for future spin-based applications. Particularly the air-stable van der Waals compound CrSBr is attracting considerable interest due to its prominent magneto-transport and magneto-optical properties. In this work, we observe a transition from antiferromagnetic to ferromagnetic behavior in CrSBr crystals exposed to high-energy, non-magnetic ions. Already at moderate fluences, ion irradiation induces a remanent magnetization with hysteresis adapting to the easy-axis anisotropy of the pristine magnetic order up to a critical temperature of 110 K. Structure analysis of the irradiated crystals in conjunction with density functional theory calculations suggest that the displacement of constituent atoms due to collisions with ions and the formation of interstitials favors ferromagnetic order between the layers.

Nanopillars of ZnO were implanted with Au-400 keV ions at various ion fluences from 1 × 10¹⁵ cm⁻² to 1 × 10¹⁶ cm⁻² and subsequently annealed at 750 °C for 15 min in order to reduce the implantation damage and to support Au nanoparticle (NP) aggregation. It was found that implantation-induced effects and thermal effects influence the Au NP coalescence as well as the quality of the ZnO nanopillars. Rutherford Back-Scattering spectrometry (RBS) showed the broader Au-depth profiles than it was theoretically predicted, but the Au-concentration maximum agrees well with prediction taking into account the effective ZnO layer density. The implantation at the higher fluences induced the morphology modification of the nanopillar layer evidenced by RBS and scanning electron microscopy (SEM). An indirect evidence of this effect was given by optical ellipsometry due to gradual refractive index changes in the ZnO nanopillars with the increased Au-ion fluence. Optical characterization of the Au-implanted and annealed nanopillars performed by means of photoluminescence (PL) and diffuse-reflectance spectroscopy (DRS) evidenced the surface plasmon resonance (SPR) activity of the embedded Au NPs. The SPR-enhanced scattering and PL emission observed in the spectral range 500–650 nm are ascribed to Au NPs or more complex Au-clusters. In addition, the ellipsometry measurements of extinction coefficient are found to corroborate well results from DRS, both indicating increase of SPR effect with the increase of Au-ion fluence and after the post-annealing.

2D transition metal carbides and/or nitrides, so-called MXenes, are noted as ideal fast-charging cation-intercalation electrode materials, which nev-ertheless suffer from limited specific capacities. Herein, it is reported that constructing redox-active phosphorus−oxygen terminals can be an attractive strategy for Nb4C3 MXenes to remarkably boost their specific capacities for ultrafast Na+ storage. As revealed, redox-active terminals with a stoichio-metric formula of PO2- display a metaphosphate-like configuration with each P atom sustaining three PO bonds and one PO dangling bond. Compared with conventional O-terminals, metaphosphate-like terminals empower Nb4C3 (denoted PO2-Nb4C3) with considerably enriched carrier density (four-fold), improved conductivity (12.3-fold at 300 K), additional redox-active sites, boosted Nb redox depth, nondeclined Na+-diffusion capability, and buffered internal stress during Na+ intercalation/de-intercalation. Consequently, com-pared with O-terminated Nb4C3, PO2-Nb4C3 exhibits a doubled Na+-storage capacity (221.0 mAh g-1), well-retained fast-charging capability (4.9 min at 80% capacity retention), significantly promoted cycle life (nondegraded capacity over 2000 cycles), and justified feasibility for assembling energy−power-balanced Na-ion capacitors. This study unveils that the molecular-level design of MXene terminals provides opportunities for developing simulta-neously high-capacity and fast-charging electrodes, alleviating the energy−power tradeoff typical for energy-storage devices.

2D magnets represent material systems in which magnetic order and topological phase transitions can be observed. Based on these phenomena, novel types of computing architectures and magnetoelectronic devices can be envisaged. Unlike conventional magnetic films, their magnetism is independent of the substrate and interface qualities, and 2D magnetic properties manifest even in formally bulk single crystals. However, 2D magnetism in layered materials is rarely reported often due to weak exchange interactions and magnetic anisotropy, and low magnetic transition temperatures. Here, the electron spin resonance (ESR) properties of a layered antiferromagnetic CrSBr single crystal are reported. The W-like shape angular dependence of the ESR linewidth provides a signature for room temperature spin–spin correlations and for the XY spin model. By approaching the Néel temperature the arising of competing intralayer ferromagnetic and interlayer antiferromagnetic interactions might lead to the formation of vortex and antivortex pairs. This argument is inferred by modeling the temperature dependence of the ESR linewidth with the topological Berezinskii-Kosterlitz-Thouless phase transition. These findings together with the chemical stability and semiconducting properties, make CrSBr a promising layered magnet for future magneto- and topological-electronics.

Liquid phase exfoliation is a commonly used method to produce 2D nanosheets from a range of layered crystals. However, such nanosheets display broad size and thickness distributions and correlations between area and thickness, issues that limit nanosheet application potential. To understand the factors controlling the exfoliation process, we have liquid-exfoliated 11 different layered materials, size-selecting each into fractions before using AFM to measure the nanosheet length, width, and thickness distributions for each fraction. The resultant data show a clear power-law scaling of nanosheet area with thickness for each material. We have developed a simple nonequilibrium thermodynamics-based model predicting that the power-law prefactor is proportional to both the ratios of in-plane-tearing/out-of-plane-peeling energies and in-plane/out-of-plane moduli. By comparing the experimental data with the modulus ratio calculated from first-principles, we find close agreement between experiment and theory. This supports our hypothesis that energy equipartition holds between nanosheet tearing and peeling during sonication-assisted exfoliation.