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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).

Inline electron holography, the recovery of amplitude and phase of an electron wave function having passed through a thin specimen from a focal series recorded in a transmission electron microscope is being applied in many labs worldwide. At medium range magnification (i.e. typically ≥ 0 . 8 nm where the lattice of small unit cell crystals such as silicon is not resolved), where the defocus needs to be varied over a rather large range of several hundred nm or even μ m, the retrieval of low spatial frequency information is severely affected by the choice of experimental parameters as well as the way of data normalization. Methods to quantitatively analyze the reliability of phase maps obtained by inline electron holography are presented, and data recorded and processed in different ways are compared. While, even under optimized conditions, the phase reconstructed from an experimental focal series still lacks very low spatial frequency components, regularization schemes exist and are demonstrated to effectively hide artifacts associated with this lack of information.

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.

Semipolar {101¯1} InGaN quantum wells are grown on (001) Si substrates with an Al-free buffer and wafer-scale uniformity. The novel structure is achieved by a bottom-up nano-heteroepitaxy employing self-organized ZnO nanorods as the strain-relieving layer. This ZnO nanostructure unlocks the problems encountered by the conventional AlN-based buffer, which grows slowly and contaminates the growth chamber.

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 surface effect on the photodetection of metal oxide nanostructures acting as a double-edged sword achieves ultrahigh photogain but unavoidably prolongs the response time due to slow oxygen adsorption/desorption processes. In this study, we break the compromise to enhance the UV photogain by 3 orders of magnitude as well as increase the photoresponse speed by 5 times via incorporating open-circuit p–n nanoscale heterojunctions (NHJs) by forming single-crystalline p-NiO nanoparticles on n-ZnO nanowires. This is because the formation of NHJs enhances surface band bending of ZnO nanowires, improving the spatial separation efficiency of photogenerated electrons and holes, and passivates the ZnO surfaces by minimizing the interaction of photocarriers with chemisorbed oxygen molecules. The concept using NHJs explores a new pathway toward ultrafast and supersensitive photodetection.

The microstructure evolution of sputtered gadolinium oxide nanocrystal (NC) memory devices upon annealing has been characterized in detail by transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). TEM results indicate that the as-deposited film is composed of metallic Gd clusters embedded in an amorphous Gd x O y matrix. The Gd clusters undergo phase transformation to oxide NCs upon annealing, reaching a maximum density of 7.9–9.1 × 10 11 cm − 2 at 850 °C, which is consistent with the largest memory window width. Upon annealing at even higher temperature, TEM diffraction patterns and XPS composition profiles indicate apparent Si diffusion into the NC layer, probably from the SiO 2 tunneling oxide or the Si substrate, leading to the formation of gadolinium silicate NCs. The presence of silicate NCs gradually deteriorates the device performance due to the reduction of barrier confinement for stored charges, although the dot density is only marginally decreased. The results suggest that the optimum memory device performance is dominated by not only the most considered size and density of NCs, but also the composition and phase inside.

In this study, the formation of Cu oxide on Cu film is studied during Cu electropolishing in a phosphoric acid-based electrolyte with various Cu ion concentrations, from 2.28% to 10.08%. In cyclic voltammetry measurement, the maximum current density of the anodic peak (Imax) decreases from 38.87 to 28.13 mA/cm2 with increasing Cu ion concentration, indicating that an oxide film forms on the Cu film surface and the thickness increases with Cu ion concentration. Microstructures and crystallography of the oxide film are examined by transmission electron microscopy, which confirms the increase of the oxide film thickness due to the high Cu ion concentration in a H3PO4 electrolyte. Three types of Cu oxide are detected using X-ray photoelectron spectroscopy, namely Cu2O, Cu(OH)2, and CuO. With a Cu-ion electrolyte concentration of less than 6.99%, Cu(OH)2 is dominant, while at higher Cu-ion concentrations, CuO predominates. The formation of CuO protects Cu from corrosion in the electrolyte with the Cu-ion concentration of over 6.99%.

The microstructure, growth mechanism, and ferromagnetic (FM)/antiferromagnetic (AFM) coupling have been discussed in Ni:ZnO nanorod/Zn:NiO nanowall composite structures. The composite structures were synthesized by a hydrothermal method at 90 °C. A systematic investigation of high-resolution transmission electron microscopy, X-ray absorption spectroscopy, and magnetization studies reveals that the as-synthesized product shows FM behavior at room temperature, whereas the annealed sample shows mixed (FM/AFM) magnetic behavior. A detectable magnetic exchange coupling between FM/AFM has been demonstrated by magnetization measurements in the annealed products. The observed room-temperature FM behavior in these nanostructures was interpreted in terms of bound magnetic polarons.

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.

ZnO seed layers and well-aligned ZnO single-crystalline micro/nanorods were synthesized on bare Si in one step without the assistance of catalysts by chemical bath deposition. Scanning electron microscopy (SEM) images and X-ray diffraction patterns show that the alignment of ZnO rods on Si(100) could be adjusted by varying the substrates’ angles of incline, the reaction temperature, and the precursor concentration. Transmission electron microscopy cross-sectional images demonstrate that a polycrystalline seed layer with (0002) preferred orientation was formed between the well-aligned rods and Si substrate placed vertically while a randomly oriented layer was formed between the randomly aligned rods and Si substrate placed horizontally. The formation of seed layers and alignment of as-synthesized ZnO rods were attributed to the assistance of boundary layers in a chemical bath deposition system.

Well-controlled growth of Ag nanoparticles (NPs) on Si substrates is important for next generation Si-based optoelectronic devices, but only randomly oriented Ag NPs have been previously reported. In this work, well-oriented Ag NPs with regular shapes are pseudomorphically grown on Si(100) and Si(111) substrates with crystallographic relationships of {100} mathematical left angle bracket 010 mathematical right angle bracket Ag ∥ {100} mathematical left angle bracket 010 mathematical right angle bracket Si and {111} mathematical left angle bracket 110 mathematical right angle bracket Ag ∥ {111} mathematical left angle bracket 110 mathematical right angle bracket Si, respectively. From a cross-sectional image, the Ag NPs on Si(100) substrates penetrate into Si and generate an inverted pyramid-like structure terminated by {111} planes embedded in Si substrates. In contrast, the Ag NPs on Si(111) substrates show flat morphology with the top plane terminated by Ag {111}. The Si underneath Ag NPs was not penetrated by Ag and a SiO(2) layer was formed between Ag and Si. Photoluminescence spectra of the Ag NPs show ultraviolet emissions centered in the 340-343 nm range. The mathematical left angle bracket 111 mathematical right angle bracket-oriented Ag particles show stronger emissions with an extra peak at 343 nm compared with mathematical left angle bracket 100 mathematical right angle bracket-oriented Ag NPs. Raman spectra show that the mathematical left angle bracket 100 mathematical right angle bracket - and mathematical left angle bracket 111 mathematical right angle bracket-oriented Ag NPs can enhance the peak intensity of Si(100) and Si(111) by 45.3% and 32.5%, respectively. The orientation-controlled Ag NPs with anisotropic optical properties are promising materials for Si-based optoelectronics.

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.

Gadolinium oxide nanocrystal (Gd 2 O 3 -NC) memories treated by postdeposition rapid thermal annealing were investigated. Bandgap offset performed by a crystallized Gd 2 O 3 -NC dot surrounded by amorphous Gd 2 O 3 dielectrics is successfully demonstrated and proven by the transmission electron microscopy images and electron diffraction pattern. The Gd 2 O 3 -NC memory exhibits a hysteresis memory window of 4 V and NC dot density of more than 8.5 X 10 11 cm -2 . In addition, the formation of Gd 2 O 3 -NC and charge loss characteristics on annealing temperature were analyzed and optimized at 850°C. The data endurance of 10 4 program and erase cycling for a sufficient memory window (>2 V) was also observed for the Gd 2 O 3 nanocrystal memory.