Magnetic materials with strong spin-orbit coupling (SOC) are essential for the advancement of spin-orbitronic devices, as they enable efficient spin-charge conversion, complex magnetic structures, spin-valley physics, topological phases and other exotic phenomena. 5d transition-metal oxides such as SrIrO3 feature large SOC, but usually show paramagnetic behavior due to broad bands and a low density of states at the Fermi level, accompanied by a relatively low Coulomb repulsion. Here, we unveil ferromagnetism in 5d SrIrO3 thin films grown on SrTiO3 (111). Through substrate-induced structural engineering, a zigzag stacking of three-unit-cell thick layers along the [111] direction is achieved, stabilizing a ferromagnetic state at the interfaces. Magnetotransport measurements reveal an anomalous Hall effect below similar to 30 K and hysteresis in the Hall conductivity below 7 K, indicating ferromagnetic ordering. X-ray magnetic circular dichroism further supports these results. Theoretical analysis suggests that the structural engineering of the IrO6 octahedral network enhances the density of states at the Fermi level and thus stabilizes Stoner ferromagnetism. This work highlights the potential of structurally engineered 5d oxides for spin-orbitronic devices, where efficient control of SOC-induced magnetic phases by electric currents can lead to lower energy consumption and improved performance in next-generation device technologies.

We measure the electron beam-induced current to analyze the electron-induced secondary electron (SE) emission from micron-sized gold particles illuminated by 80 and 300 keV electrons in a transmission electron microscope. A direct comparison of the experimental and simulated SE emission (SEE) employing Monte Carlo scattering simulations based on the GEANT4 toolkit yields overall good agreement with a noticeable discrepancy arising from the shortcoming of the GEANT4 scattering cross sections in the low-loss regime. Thus, the electron beam-induced current analysis allows to quantify the inelastic scattering including SEE in the transmission electron microscope and provides further insight into the charging mechanisms.

Near-infrared (NIR) controlled drug delivery systems have drawn a lot of attention throughout the past few decades due to the deep penetration depth and comparatively minor side effects of the stimulus. In this study, we introduce an innovative approach for gastric cancer treatment by combining photothermal infrared-sensitive gold nanorods (AuNRs) with a conjugated microporous polymer (CMP) to create a drug delivery system tailored for transporting the cytostatic drug 5-fluorouracil (5-FU). CMPs are fully conjugated networks with high internal surface areas that can be precisely tailored to the adsorption and transport of active compounds through the right choice of chemical functionalities. By incorporation of surfactant-stabilized AuNRs into the CMP synthesis in dimethylformamide (DMF) the surfactant shell is destabilized and subsequently replaced by the CMP. Particularly, low initial surfactant concentrations led to uniform distribution of the AuNRs in the polymer matrix. Importantly, the integrated AuNRs maintain their plasmonic properties, as was confirmed via electron energy loss spectroscopy. Therefore, the significant photothermal properties are translated to the hybrid material as shown in a proof-of-principle experiment. Further, in an approximated gastric environment, 5-FU release studies were conducted with and without NIR stimulus. Thereby it was observed that increased Brownian motion due to the NIR irradiation not only accelerates the release but also increases the total released amount by influencing the adsorption-desorption equilibrium. This remarkable level of control of the release process underlines the immense potential of this hybrid material for precise and targeted drug delivery.

Assemblies of plasmonic nanoparticles (NPs) support hybridized modes of localized surface plasmons (LSPs), which delocalize in geometrically well-ordered arrangements. Here, the hybridization behavior of LSPs in geometrically completely disordered two-dimensional arrangements of Au NPs fabricated by an e-beam synthesis method is studied. Employing electron energy loss spectroscopy in a scanning transmission electron microscope and numerical simulations, the disorder-driven spatial and spectral localization of the coupled LSP modes that depends on the NP thickness is revealed. Below a NP thickness of 0.4 nm, localization increases toward higher hybridized LSP mode energies. In comparison, above 10 nm thickness, a decrease of localization toward higher mode energies is observed. In the intermediate thickness regime, a transition of the energy dependence of the localization between the two limiting cases, exhibiting a mode energy with minimal localization, is observed. It is shown that this behavior is mainly driven by the energy and thickness dependence of the polarizability of the individual NPs.

The perfect linear temperature dependence of the electrical resistivity in a variety of “strange” metals is a real puzzle in condensed matter physics. For these materials also other non-Fermi liquid properties are predicted or detected. In particular we mention the results derived from holographic theories which conclude that plasmons should be overdamped due to a low energy continuum in the electronic susceptibility. These predictions were supported by electron energy-loss spectroscopy in reflection on cuprates and ruthenates. Here we use electron energy-loss spectroscopy in transmission to study collective charge excitations in the layer metal Sr 2 RuO 4 . This metal has a transition from a perfect Fermi liquid below T ≈ 30 K into a “strange” metal phase above T ≈ 800 K. In this compound we cover a complete range between in-phase and out-of-phase oscillations. Outside the classical range of electron-hole excitations, leading to a Landau damping, we observe well-defined plasmons. The optical (acoustic) plasmon due to an in-phase (out-of-phase) charge oscillation of neighbouring layers exhibits a quadratic (linear) positive dispersion. Using a model for the Coulomb interaction of the charges in a layered system, it is possible to describe the range of optical plasmon excitations at high energies in a mean-field random phase approximation without taking correlation effects into account. In contrast, resonant inelastic X-ray scattering data show at low energies an enhancement of the acoustic plasmon velocity due to correlation effects. This difference can be explained by an energy dependent effective mass which changes from ≈ 3.5 at low energy to 1 at high energy near the optical plasmon energy. There are no signs of over-damped plasmons predicted by holographic theories.

Sodium is known as a soft metal that can easily change its particle morphology. It can form outstretched and rolled fibers with plastic or brittle behavior, and cubes. In Na-batteries, metallic Na anodes demonstrate a high reactivity towards the majority of electrolyte solutions, volume change and a random deposition process from the electrolyte, accompanied by dendrite formation. In order to smooth the electrochemical Na deposition, we propose NaOH as a simple artificial protective layer for sodium, formed by its exposure to ambient conditions for a certain period of time. The formed NaOH layer on top of the metallic sodium suppresses the volume change and dendrite growth on the sodium surface. Additionally, the protected sodium does not change its morphology after a prolonged contact with carbonate-based electrolytes. In symmetric Na-batteries, the NaOH layer increases the lifetime of the electrochemical cell by eight times in comparison to non-protected Na. In the full-cell with a layered sodium oxide cathode, the NaOH-protected sodium anode also leads to a high cycling stability, providing 81 % of the initial cell capacity after 500 cycles with a 1C current rate. In contrast, batteries with a non-protected Na-anode reach only 20 % of their initial capacity under the same conditions. Therefore, the main benefits of the NaOH artificial layer are the chemical compatibility with the carbonate-based electrolytes, the protection of Na metal against reaction with the electrolyte solution, the rapid Na-ion diffusion through the layer and the formation of a mechanical barrier, mitigating Na-dendrite growth. This work presents an easily scalable method to protect sodium without any additional chemicals or a special environment for this reaction.

The so-called Transport of Intensity Equation (TIE) phase retrieval technique is widely applied in light, x-ray and electron optics to reconstruct, e.g., refractive indices, electric and magnetic fields in solids. Here, we present a largely improved TIE reconstruction algorithm, which properly considers intensity variations as well as unknown boundary conditions in a finite difference implementation of the Transport of Intensity partial differential equation. That largely removes reconstruction artifacts encountered in state-of-the-art Poisson solvers of the TIE, and hence significantly increases the applicability of the technique.

Two-dimensional random metal networks possess unique electrical and optical properties, such as almost total optical transparency and low sheet resistance, which are closely related to their disordered structure. Here we present a detailed experimental and theoretical investigation of their plasmonic properties, revealing Anderson (disorder-driven) localized surface plasmon (LSP) resonances of very large quality factors and spatial localization close to the theoretical maximum, which couple to electromagnetic waves. Moreover, they disappear above a geometry-dependent threshold at ca. 1.7 eV in the investigated Au networks, explaining their large transparencies in the optical spectrum.

The combination of plasmonic nanoparticles and optical microcavities has attracted broad interest for both fundamental and applied studies. However, the conventional scheme of plasmonic nanoparticles being located at microcavity outer surfaces suffers from serious problems such as significant radiative/scattering losses and chemical/mechanical instabilities. Here, silver nanoparticles (NPs) and dispersed ions embedded in nanomembrane‐formed whispering‐gallery‐mode (WGM) microtube cavities are prepared by ion implantations as compact and stable optoplasmonic microcavities. Upon low ion fluence implantation, dispersed silver ions are generated in the tube cavity wall, leading to a redshift of the WGM resonant cavity modes due to the increased refractive index. The silver ions start to aggregate into plasmonic NPs in the cavity wall when increasing implantation ion fluences. The competition and transition between redshift induced by the refractive index increase and blueshift induced by the formation of plasmonic NPs are investigated. Moreover, quality factor enhancement of the WGM modes is observed owing to the improved light confinement caused by the presence of NPs. This work demonstrates a convenient approach for the fabrication of stable optoplasmonic microcavities and fine tuning of resonant modes, indicating wide applications such as wavelength selective tuning and enhanced light–matter interactions.

Hybrid metallic nanoparticles (NPs) encapsulated in oxide shells are currently intensely studied for plasmonic applications in sensing, medicine, catalysis, and photovoltaics. Here, a method for the synthesis of Au@Ag@SiO 2 cubes with a uniform silica shell of variable and adjustable thickness in the nanometer range is introduced and their excellent, highly reproducible, and tunable optical response is demonstrated. Varying the silica shell thickness, the excitation energies of the single NP plasmon modes can be tuned in a broad spectral range between 2.55 and 3.25 eV. Most importantly, a strong coherent coupling of the surface plasmons is revealed at the silver–silica interface with Mie resonances at the silica–vacuum interface leading to a significant field enhancement at the encapsulated NP surface in the range of 100% at shell thicknesses t ≃ 20 nm. Consequently, the synthesis method and the field enhancement open pathways to a widespread use of silver NPs in plasmonic applications including photonic crystals and may be transferred to other non‐precious metals.

Chains of coupled metallic nanoparticles are of special interest for plasmonic applications because they can sustain highly dispersive plasmon bands, allowing strong ballistic plasmon wave transport. Whereas early studies focused on homogeneous particle chains exhibiting only one dominant band, heterogeneous assemblies consisting of different nanoparticle species came into the spotlight recently. Their increased configuration space principally allows engineering multiple bands, bandgaps, or topological states. Simultaneously, the challenge of the precise arrangement of nanoparticles, including their distances and geometric patterns, as well as the precise characterization of the plasmonics in these systems, persists. Here, the surface plasmon resonances in heterogeneous AgAu nanoparticle chains are reported. Wrinkled templates are used for directed self‐assembly of monodisperse gold and silver nanospheres as chains, which allows assembling statistical combinations of more than 10 9 particles. To reveal the spatial and spectral distribution of the plasmonic response, state‐of‐the‐art scanning transmission electron microscopy coupled with electron energy loss spectroscopy accompanied by boundary element simulations is used. A variety of modes in the heterogeneous chains are found, ranging from localized surface plasmon modes occurring in single gold or silver spheres, respectively, to modes that result from the hybridization of the single particles. This approach opens a novel avenue toward combinatorial studies of plasmonic properties in heterosystems.

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Electronic topological states of matter exhibit novel types of responses to electromagnetic fields. The response of strong topological insulators, for instance, is characterized by a so-called axion term in the electromagnetic Lagrangian which is ultimately due to the presence of topological surface states. Here we develop the axion Mie theory for the electromagnetic response of spherical particles including arbitrary sources of fields, i.e., charge and current distributions. We derive an axion induced mixing of transverse magnetic and transverse electric modes which are experimentally detectable through small induced rotations of the field vectors. Our results extend upon previous analyses of the problem. Our main focus is on the experimentally relevant problem of electron energy loss spectroscopy in topological insulators, a technique that has so far not yet been used to detect the axion electromagnetic response in these materials.

Imprint lithography has emerged as a reliable, reproducible, and rapid method for patterning colloidal nanostructures. As a promising alternative to top-down lithographic approaches, the fabrication of nanodevices has thus become effective and straightforward. In this study, a fusion of interference lithography (IL) and nanosphere imprint lithography on various target substrates ranging from carbon film on transmission electron microscope grid to inorganic and dopable polymer semiconductor is reported. 1D plasmonic photonic crystals are printed with 75% yield on the centimeter scale using colloidal ink and an IL-produced polydimethylsiloxane stamp. Atomically smooth facet, single-crystalline, and monodisperse colloidal building blocks of gold (Au) nanoparticles are used to print 1D plasmonic grating on top of a titanium dioxide (TiO2) slab waveguide, producing waveguide-plasmon polariton modes with superior 10 nm spectral line-width. Plasmon-induced hot electrons are confirmed via two-terminal current measurements with increased photoresponsivity under guiding conditions. The fabricated hybrid structure with Au/TiO2 heterojunction enhances photocatalytic processes like degradation of methyl orange (MO) dye molecules using the generated hot electrons. This simple colloidal printing technique demonstrated on silicon, glass, Au film, and naphthalenediimide polymer thus marks an important milestone for large-scale implementation in optoelectronic devices.

Electronic topological states of matter exhibit novel types of responses to electromagnetic fields. The response of strong topological insulators, for instance, is characterized by a so-called axion term in the electromagnetic Lagrangian which is ultimately due to the presence of topological surface states. Here we develop the axion Mie theory describing the electromagnetic response of spherical particles including an axion electromagnetic coupling at the surface of a particle. The approach includes arbitrary sources of fields, i.e., charge and current distributions. We derive an axion induced mixing of transverse magnetic and transverse electric modes which are experimentally detectable through small induced rotations of the field vectors.

Electronic topological states of matter exhibit novel types of responses to electromagnetic fields.The response of strong topological insulators, for instance, is characterized by a so-called axion term in the electromagnetic Lagrangian which is ultimately due to the presence of topological surface states.Here we develop the axion Mie theory describing the electromagnetic response of spherical particles including an axion electromagnetic coupling at the surface of a particle.The approach includes arbitrary sources of fields, i.e., charge and current distributions.We derive an axion induced mixing of transverse magnetic and transverse electric modes which are experimentally detectable through small induced rotations of the field vectors.

The developed three-step synthesis of plasmonic gold nanoparticles allows outstanding control over their growth kinetic, size and habit.

Surface plasmons are self-sustaining resonances occurring at interfaces of dielectric media where the permittivity changes sign. They often exhibit strongly enhanced, localized electrical fields, so they couple strongly to electromagnetic, in particular optical, excitations. Accordingly, surface plasmons are able to be used for sub-wavelength control of electromagnetic fields. Based on this, novel electronic devices can be realized, for instance on-chip light spectrometers and linear accelerators, plasmonic rectennas for the harvesting of light or LEDs and photovoltaics with a higher efficiency. For a thorough understanding of the properties of plasmonic resonances in different materials and structures the spatial distribution of transient electromagnetic fields is of particular interest. To map the evanescent electrical field with high spatial and spectral resolution, electron energy-loss spectroscopy (EELS) in the scanning transmission electron microscope (STEM) can be utilized. Here, on the one hand, the Cartesian z-component of the induced electric field parallel to the beam direction causes an energy loss of the beam electrons, on the other hand, the lateral components of the induced electric and magnetic field lead to a deflection of the electron beam. z-component by at positions microscopy technique