Spin–vibration coupling has been proven to be crucial for spin dynamics; theoretical studies are now addressing this experimental challenge.

Herein, we present two geometrical models based on an effective point-charge approach to provide a full description of the lowest sublevels in lanthanoid single ion magnets (SIMs). The first one, named as the Radial Effective Charge (REC) model, evaluates the crystal field effect of spherical ligands, e.g. F⁻, Cl⁻ or Br⁻, by placing the effective charge along the Ln–ligand axes. In this case the REC parameters are obtained fitting high-resolution spectroscopic data for lanthanoid halides. The second model, named as the Lone Pair Effective Charge (LPEC) model, has been developed in order to provide a realistic description of systems in which the lone pairs are not pointing directly towards the magnetic ion. A relevant example of this kind is provided by the bis(phthalocyaninato)lanthanoids [Ln(Pc)₂]⁻. We show that a fit of the magnetic properties of the [Ln(Pc)₂]⁻ (Ln = Tb, Dy, Ho, Er, Tm and Yb) allows us to extract the LPEC parameters for the lanthanoid complexes coordinated to sp²-nitrogens. Finally, we show that these effective corrections may be extrapolated to a large variety of lanthanoid and actinoid compounds, having either extended or molecular structures.

2D magnetic materials offer unprecedented opportunities for fundamental and applied research in spintronics and magnonics. Beyond the pioneering studies on 2D CrI₃ and Cr₂Ge₂Te₆, the field has expanded to 2D antiferromagnets exhibiting different spin anisotropies and textures. Of particular interest is the layered metamagnet CrSBr, a relatively air‐stable semiconductor formed by antiferromagnetically‐coupled ferromagnetic layers (T_c∼150 K) that can be exfoliated down to the single‐layer. It presents a complex magnetic behavior with a dynamic magnetic crossover, exhibiting a low‐temperature hidden‐order below T*∼40 K. Here, the magneto‐transport properties of CrSBr vertical heterostructures in the 2D limit are inspected. The results demonstrate the marked low‐dimensional character of the ferromagnetic monolayer, with short‐range correlations above T_c and an Ising‐type in‐plane anisotropy, being the spins spontaneously aligned along the easy axis b below T_c. By applying moderate magnetic fields along a and c axes, a spin‐reorientation occurs, leading to a magnetoresistance enhancement below T*. In multilayers, a spin‐valve behavior is observed, with negative magnetoresistance strongly enhanced along the three directions below T*. These results show that CrSBr monolayer/bilayer provides an ideal platform for studying and controlling field‐induced phenomena in two‐dimensions, offering new insights regarding 2D magnets and their integration into vertical spintronic devices.

The alkaline oxygen evolution reaction is a key step in producing green hydrogen through water electrolysis, but its large-scale industrial application remains limited due to challenges with current electrocatalysts—particularly in terms of scalability, efficiency, and long-term stability. Here we show an industrially scalable synthesis of an active NiFe layered double hydroxide (NiFe-LDH) catalyst using a room-temperature, atmospheric-pressure route. The process involves homogeneous alkalinization, where chloride ions nucleophilically attack an epoxide ring, producing a low-dimensional, defect-rich NiFe-LDH with pronounced iron clustering. In-situ spectroscopy and ab-initio calculations reveal that these structural features maximize the conversion of the NiFe-LDH to the catalytic active phase and minimize the energy barrier, improving catalytic efficiency. When used as the anode in an anion exchange membrane water electrolyzer operating at 70 °C, our material delivers 1 A cm⁻² at 1.69 V in a 5 cm² full-cell setup, with notable durability compared to conventional NiFe-LDHs. This scalable approach could considerably lower the cost of green hydrogen production by enabling more efficient alkaline electrolyzers.