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We thank the German Science Foundation (DFG) for financial support within the grants SFB 765 and SFB 658. M.F.G. and J.P.R. also acknowledge the support of the Cluster of Excellence “Matters of Activity. Image Space Material” funded by the DFG under Germany’s Excellence Strategy EXC 2025-390648296. Furthermore, A.T. acknowledges the DFG for funding within the project TH 1463/12-1. We thank Dr. Andreas Schäfer and Maiko Schulze for solid NMR experiments and we appreciate the effort of Vahid Ahmadi Soureshjani in MALDI-TOF experiments. We acknowledge M. Eng. Jörg M. Stockmann for operating the XPS instrument at the BAM and Prof. Stephanie Reich and Dr. Antonio Setaro for fruitful discussions. 2DTs-HRTEM and -EELS studies were conducted at the Laboratorio de Microscopias Avanzadas, Instituto de Nanociencia de Aragon, Universidad de Zaragoza, Spain. R.A. gratefully acknowledges the support from the Spanish Ministry of Economy and Competitiveness (MINECO) through project grant MAT2016-79776-P (AEI/FEDER, UE) and from the European Union H2020 programs ETN projects “Graphene Flagship” (785219 and 881603), FLAG-ERA - Graphene (MICINN) GATES (PCI2018-093137) and “ESTEEM3” (823717).

While GeSn alloys with high Sn content constitute direct group-IV semiconductors, their growth on Si remains challenging. The deposition of a few monolayers of pure Sn on Ge and their overgrowth with Ge using molecular beam epitaxy can be a means of obtaining Sn-rich quantum wells with very high Sn content while maintaining high crystal quality. Here, we provide structural and compositional information on such structures with very high accuracy. Based on our characterization results we theoretically predict transition energies and compare them with experimental results from photoluminescence measurements. Our results constitute the groundwork for tuning the molecular beam epitaxy based growth of Sn-rich quantum wells and dots for applications in electronic and optoelectronic devices.

Improved multiphoton¿excited imaging and microspectroscopy require nanoprobes that can give different nonlinear optical signals. Here, composite nanostructures with a barium titanate core and a plasmonic moiety at their surface are synthesized and characterized. It is found that the core provides a high second¿order nonlinear susceptibility for sensitive second harmonic generation (SHG) imaging in living cells. As a second function in the two¿photon regime, the plasmonic part yields high local fields for resonant and nonresonant surface enhanced hyper Raman scattering (SEHRS). SEHRS complements the one¿photon surface enhanced Raman scattering (SERS) spectra that are also enhanced by the plasmonic shells. Barium titanate silver core¿shell (Ag@BaTiO3) composites are specifically suited for SEHRS and SHG excited at 1064 nm, while gold at barium titanate (Au@BaTiO3) nanoparticles can be useful in a combination of SHG and SERS at lower wavelengths, here at 785 nm and 850 nm. The theoretical models show that the optical properties of the BaTiO3 dielectric core depend on probing frequency, shape, size, and plasmonic properties of the surrounding gold nanoparticles so that they can be optimized for a particular type of experiment. These versatile, tunable probes give new opportunities for combined multiphoton probing of morphological structure and chemical properties of biosystems., Funding by ERC Starting Grant No. 259432 MULTIBIOPHOT to J.K., a Chemiefonds Fellowship (FCI) to F.M., and DFG GSC 1013 SALSA to V.Z. are gratefully acknowledged. A.N., R.E., and J.A. acknowledge the National Project FIS2016‐80174‐P from the MICINN, Grant No. IT1164‐19, for research groups of the Basque University system from the Department of Education of the Basque Government and Elkartek project KK‐2018/00001 from the Department of Economical Development and Infrastructures of the Basque Government.

Electron energy-loss spectroscopy and energy-dispersive X-ray spectroscopy are two of the most common means for chemical analysis in the scanning transmission electron microscope. The marked progress of the instrumentation hardware has made chemical analysis at atomic resolution readily possible nowadays. However, the acquisition and interpretation of atomically resolved spectra can still be problematic due to image distortions and poor signal-to-noise ratio of the spectra, especially for investigation of energy-loss near-edge fine structures. By combining multi-frame spectrum imaging and automatic energy-offset correction, we developed a spectrum imaging technique implemented into customized DigitalMicrograph scripts for suppressing image distortions and improving the signal-to-noise ratio. With practical examples, i.e. SrTiO 3 bulk material and Sr-doped La 2 CuO 4 superlattices, we demonstrate the improvement of elemental mapping and the EELS spectrum quality, which opens up new possibilities for atomically resolved EELS fine structure mapping.

We propose a simple system to investigate the influence of microstructure on the resistive switching behavior via bi-crystal CuO nanowires. CuO nanowires are prepared by thermally oxidizing transmission electron microscopy copper grids in air. Single-crystal and bi-crystal CuO nanowires can be selectively obtained by adjusting the temperature. The devices made of single-crystal nanowires follow Ohm’s law, with a high resistance, within the sweeping voltage range of 0–4 V, whereas those made of bi-crystal nanowires exhibit threshold and memory resistive switching behaviors, which are due to the enrichment of copper ions in the grain boundaries of bi-crystal CuO nanowires providing sources for the formation of conductive filaments. Moreover, the bi-crystal nanowires with higher defect densities in grain boundaries result in lower threshold voltages of switching from high to low resistance states. The threshold resistive switching behavior can be turned into memory resistive switching behavior by increasing the thickness of the device electrodes or reducing the compliance current. The endurance of memory resistive switching through the pre-defined conduction paths in the single grain boundaries of bi-crystal CuO nanowires is at least 1000 cycles without any performance deterioration. This high reliability is ascribed to the single conductive filaments.

The transport of intensity equation (TIE) relates the variation of intensity of a wave-front along its mean direction of propagation with its phase. In experimental application, characteristic artefacts may affect the retrieved phase. These originate from inadequacies in estimating the axial derivative and the amplification of noise in the inversion of the TIE. To tackle these issues, images recorded at multiple planes of focus can be integrated into a multi-focus TIE (MFTIE) solution. This methodology relies on the efficient sampling of phase information in the spatial-frequency domain, typically by the definition of band pass filters implemented as a progression of sharp spatial frequency cut-offs. We present a convenient MFTIE implementation which avoids the need for recording images at very specific planes of focus and applies overlapping cut-offs, greatly simplifying the experimental application. This new approach additionally also accounts for partial spatial coherence in a flux-preserving framework. Using simulated data as well as experimental data from optical microscopy and electron microscopy we show that the frequency response of this MFTIE algorithm recovers efficiently a wide range of spatial frequencies of the phase that can be further extended by simple iterative refinement.

The influence of surface oxidation on the low-loss spectrum of aluminum nitride (AlN) is investigated in electron energy-loss spectroscopy with scanning transmission electron microscopy. Contrary to intrinsic bulk AlN, oxidized AlN exhibits considerable spectral broadening both in the full width at half maximum of bulk plasmon and the subsidiary features. The modification in the low-loss lineshapes due to oxidation significantly complicates the determination of the dielectric function intrinsic to AlN. Simulations based on dielectric theory qualitatively consist with the experimental results while incorporating thick overlayers, further suggesting that the surface oxide of AlN can be rough and porous in nature.