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Abstract: Practical electrochemical energy conversion requires electrocatalysts that coordinate multiple elementary steps at spatially distinct active sites, yet atomic-level control of such site-specific reactivity within a single heterogeneous particle remains challenging. Here we propose and realize atomic-scale gradient strain as a design concept for heterogeneous electrocatalysis. Using Pd@Pt core-shell tetrahedra as a model system, we construct a continuous lattice-strain gradient across individual 3–4 atomic-layer Pt {111} epitaxial shells, where lattice-mismatch-driven compression relaxes from edges to center regions. This single-particle strain gradient, spanning approximately −8% to −2%, spatially links *O2 activation at highly compressed sites with *OH weakening at moderately compressed sites through kinetically accessible intermediate redistribution. The catalysts exhibit competitive oxygen reduction reaction performance, with mass and specific activities of 2.19 A mgPt⁻1 and 3.01 mA cm⁻2 at 0.9 V vs reversible hydrogen electrode, while retaining 91% activity after 20 k cycles. In membrane electrode assemblies, they achieve 0.57 A mgPt⁻1, and peak power densities of 2.10 W cm⁻2 in H2 − O2 and 1.16 W cm⁻2 in H2−air, with over 90% performance retention after 20 k cycles.

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Abstract: Epitaxial films of the ferromagnetic manganite La0.7⁢Sr0.3⁢MnO3 on substrates of the ferroelectric perovskite BaTiO3 are known to display sharp magnetic changes and large magnetoelectric effects when the film is strained by the substrate undergoing thermally driven structural transitions and ferroelectric domain switching, respectively. However, only a single component of the in-plane magnetization has been hitherto imaged. Here we present magnetic vector maps—obtained from photoemission electron microscopy images with magnetic contrast from x-ray magnetic circular dichroism—to show that the electrically and thermally driven changes of local and global magnetization are deterministically influenced by the state of the substrate while also being complex and sample dependent. Our findings, supported by ferromagnetic resonance data and vibrating sample magnetometry, reveal that the behavior of La0.7⁢Sr0.3⁢MnO3 films on BaTiO3 substrates is not well predicted from knowledge of each system, probably due to long-range strain between BaTiO3 domains. In the future, it would be interesting to reduce complexity by patterning the film into regions between which magnetic communication is negligible.

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Abstract: Rare-earth iron garnet (RE3Fe5O12) films are promising insulating ferrimagnets. They can show low magnetic damping, perpendicular magnetic anisotropy, and ultrafast spin dynamics, which makes them ideal for spin transport applications. In this work, we investigate the interaction between the magnetic sublattices in Er3Fe5O12 thin films grown by pulsed laser deposition on a Gd3Ga5O12 substrate. Structural and magnetic characterization reveals high-quality single-crystal growth, with a compensation temperature close to the reported bulk value (∼80 K). Magnetic phase diagrams based on element-specific measurements map out the regions where ferrimagnetic, canted, and aligned phases are stable across the compensation temperature. The micromagnetic dynamics resulting from perpendicular magnetic pulse perturbation of an in-plane magnetized layer was investigated at room temperature and revealed complex configurations. These results are key features for modulating magnetization dynamics through the compensation phenomenon, which is essential for spin-based devices operating in a low-temperature regime.

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Abstract: Superfluid helium droplets represent a unique state of matter, which are large clusters of helium typically containing approximately 103-1011 helium atoms and exhibit remarkable properties such as superfluidity, a very low temperature (0.37 K) and high thermal conductivity. This PhD project investigates two novel aspects of superfluid helium droplets: the use of superfluid helium nanodroplets as the nanoreactors to grow magnetic nanoparticles and the generation and exploration of quantum vortices in a controlled manner. In the first part, we exploit the very low temperature and rapid cooling to develop a new approach for fabricating magnetic nanoparticles. For the very low temperature and the ultrahigh thermal conductivity, superfluid helium can suppress thermal effects during the atom-by-atom growth of magnetic nanoparticles, making the relatively weak exchange interactions (compared with metallic bonding) the driving force. As a result, the atomic spins align for ferromagnetic elements and thus the magnetic moments of nanoparticles are maximized. In particular, we focus on iron nanoparticles coated by a gold shell and investigate their properties by electron microscopy (for structural investigation) and x-ray circular dichroism (XMCD), for magnetic property measurement) at the Diamond Light Source. We first study mass spectrometry of small iron clusters and observed abnormal behaviours. Unlike other molecular clusters formed in helium droplets such as water, gold and silver, which typically follow a Poisson distribution, Fe+ channel was found to be far greater than that of FeN+ (N = 2-8) clusters. We postulate this as an indicator for the formation of high-spin iron clusters inside superfluid helium and attempt to provide an interpretation based on DFT calculations. However, XMCD showed an expected low magnetisation for Fe/Au core-shell nanoparticles which is even lower than iron oxide nanoparticles, indicating that the neutral Fe atoms are oxidized into Fe2+ within the nanoparticles which is magnetically inert. This is accounted by the very high electron negativity of Au atoms and the alloying effect during the growth of nanoparticles, which dismisses the magnetic properties. Our work shows that the choice of protective shell is important to maintain the magnetic properties of iron nanoparticles and points the direction for the next-step research. The second part presents a breakthrough in quantum vortex research. We demonstrate a novel method for generating controlled vortex arrays in superfluid helium droplets through collisions with cesium ions. Subsequential addition of metal atoms (Ag and Au) to helium droplets and the formation of nanodroplets allow the vortex lattices to be imaged after the nanoparticles are deposited onto a solid surface. By this approach we have revealed a record-high vortex density of 5.6×10¹⁴ m⁻², exceeding previous observations in bulk superfluid helium by more than six orders of magnitude. This unprecedented vortex density opens new possibilities for studying quantum hydrodynamics at extreme angular momenta and investigating quantum turbulence in previously inaccessible regimes. Through detailed theoretical analysis and experimental characterization, this work establishes superfluid helium droplets as a versatile platform for both materials synthesis and fundamental research. Our findings not only advance the understanding of superfluidity but also provide a new pathway for developing high-performance magnetic nanomaterials that can potentially revolutionize biomedical science and technologies.

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Abstract: Layered oxide materials, with their two-dimensional crystalline architectures and tunable interlayer interaction, serve as a fertile field for harnessing emergent quantum phenomena. Among these materials, metallic delafossites (e.g., PdCoO2) have emerged as a prominent system with extraordinary two-dimensional electronic properties, though their intrinsic lack of ferromagnetism has remained a fundamental constraint. Here, we report the creation of robust, bulk high-temperature ferromagnetism (𝑇𝑐>420  K) in inherently nonmagnetic PdCoO2 through controlled hydrogenation while preserving the delafossite structure. This process induces layer-selective electron doping into CoO2 layers, stabilizing Ising-type ferromagnetism with pronounced perpendicular magnetic anisotropy while preserving the material’s exceptional metallicity. Remarkably, the system self-assembles into a superlattice of alternating metallic Pd and insulating ferromagnetic hydrogenated CoO2 layers, enabling an unconventional anomalous Hall effect mediated by interlayer spin-charge coupling. These findings demonstrate that bulk ferromagnetism can be achieved in delafossite oxides while preserving their structural integrity, positioning hydrogenated delafossites as a versatile platform for exploring correlated quantum effects and designing multifunctional devices.