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Wöste, Andreas; Hergert, Germann; Quenzel, Thomas; Silies, Martin; Wang, Dong; Groß, Petra; Lienau, Christoph
Ultrafast coupling of optical near fields to low-energy electrons probed in a point-projection microscope. - In: Nano letters, ISSN 1530-6992, Bd. 23 (2023), 12, S. 5528-5534

We report the first observation of the coupling of strong optical near fields to wavepackets of free, 100 eV electrons with <50 fs temporal resolution in an ultrafast point-projection microscope. Optical near fields are created by excitation of a thin, nanometer-sized Yagi-Uda antenna, with 20 fs near-infrared laser pulses. Phase matching between electrons and near fields is achieved due to strong spatial confinement of the antenna near field. Energy-resolved projection images of the antenna are recorded in an optical pump-electron probe scheme. We show that the phase modulation of the electron by transverse-field components results in a transient electron deflection while longitudinal near-field components broaden the kinetic energy distribution. This low-energy electron near-field coupling is used here to characterize the chirp of the ultrafast electron wavepackets, acquired upon propagation from the electron emitter to the sample. Our results bring direct mapping of different vectorial components of highly localized optical near fields into reach.



https://doi.org/10.1021/acs.nanolett.3c00738
Matthes, Sebastian; Glaser, Marcus; Vardo, Emina; Sauni Camposano, Yesenia Haydee; Jaekel, Konrad; Bergmann, Jean Pierre; Schaaf, Peter
Influence of extrinsic induced tensile stress on the self-propagating high-temperature synthesis of nanosized Al/Ni multilayers. - In: Journal of materials science, ISSN 1573-4803, Bd. 58 (2023), 24, S. 10085-10095

Reactive multilayer systems consisting of alternating nanoscale Al and Ni layers are applicable in joining, various pyrotechnic applications and thermal batteries. Since diffusion based high-temperature synthesis occurs without the presence of air, efforts have focused on investigating the understanding of the fundamental reaction processes and characteristics. The aim of this study is to expose the reactive multilayers to extrinsic induced tensile stress so that the self-propagating synthesis can proceed under these conditions. Further, the properties during and after the reaction will be investigated. Multilayers deposited by sputtering on Kapton® substrates with different bilayer- and total thicknesses as well as commercial Nanofoils® with thicknesses of 40 µm and 60 µm were used as samples. The investigations focused on the propagation velocity measured with a high-speed camera, the temperature regime determined with a high-speed pyrometer, and the formed phases after the synthesis examined via X-ray diffraction. The gained results of this study reveal important insights for the application of the reactive Al/Ni multilayer system in terms of stability or reliability related to propagation front velocity, maximum temperature and formed phases under induced external tensile stresses.



https://doi.org/10.1007/s10853-023-08618-w
Isaac, Nishchay Angel; Schlag, Leslie; Ispas, Adriana; Reiprich, Johannes; Soydan, Alper K.; Moreira, Pedro H. O.; Thiele, Sebastian; Aliabadian, Bardia; Flock, Dominik; Knauer, Andrea; Jiménez, Juan J.; Bund, Andreas; Morales Sánchez, Francisco Miguel; Pezoldt, Jörg; Jacobs, Heiko O.
Novel gas phase route toward patterned deposition of sputter-free Pt/Al nanofoils. - In: Advanced Materials Technologies, ISSN 2365-709X, Bd. 8 (2023), 18, 2300448, S. 1-8

This article reports a new approach toward fabrication and directed assembly of nanoparticulate reactive system (Nanofoils) on patterned substrates. Different from current state-of-the-art, gas phase electrodeposition uses nanoparticles instead of atoms to form densely packed multilayered thin films at room temperature-pressure. On ignition, the multilayer system undergoes an exothermic self-propagating reaction. The numerous contact points between two metallic nanoparticulate layers aid in high heat release. Sub-10-nm Platinum (Pt) and Aluminum (Al) particles are synthesized through cathode erosion of metal electrodes in a flow of pure nitrogen gas (spark ablation). Pt/Al bilayer stacks with total thickness of 3–8 µm undergo self-propagating reaction with a 10.3 mm s−1 wavefront velocity on local ignition. The reaction wavefront is captured using high speed videography. Calorimetry studies reveal two exothermic peaks suggesting Pt/Al alloy formation. The peak at 135 &ring;C has a higher calorific value of 150 mW g−1 while the peak at 400 &ring;C has a 12 mW g−1 exothermic peak. X-ray diffraction study shows reaction-products are cubic Al2Pt with small quantities of orthorhombic Al6Pt and orthorhombic AlPt2. Electron microscopy studies help draw a correlation between film morphology, bimetallic interface, nanoparticle oxidation, and self-propagating reaction kinetics that is significant in broadening our understanding towards nanoparticulate reactive systems.



https://doi.org/10.1002/admt.202300448
Heiniger-Schell, Juliana; Bharuth-Ram, Krish; Naicker, Kimara; Masondo, Vusumuzi; Dang, Thien Thanh; Escobar Castillo, Marianela; Díaz-Guerra, Carlos; Marschick, Georg; Masenda, Hilary; Gunnlaugsson, Haraldur P.; Qi, Bingcui; Unzueta, Iraultza; Ólafsson, Sveinn; Adhikari, Rajdeep; Peters, Gerrard; Naidoo, Deena; Schaaf, Peter; Zyabkin, Dmitry; Johnston, Karl; Becker, Sven; Jakob, Gerhard
Temperature dependence of the hyperfine magnetic field at Fe sites in Ba-doped BiFeO3 thin films studied by emission Mössbauer spectroscopy. - In: Crystals, ISSN 2073-4352, Bd. 13 (2023), 5, 724, S. 1-13

Emission 57Fe Mössbauer spectroscopy (eMS), following the implantation of radioactive 57Mn+ ions, has been used to study the temperature dependence of the hyperfine magnetic field at Fe sites in Ba-doped BiFeO3 (BFO) thin films. 57Mn β decays (t1/2 = 90 s) to the 14.4 keV Mössbauer state of 57Fe, thus allowing online eMS measurements at a selection of sample temperatures during Mn implantation. The eMS measurements were performed on two thin film BFO samples, 88 nm and 300 nm thick, and doped to 15% with Ba ions. The samples were prepared by pulsed laser deposition on SrTiO3 substrates. X-ray diffraction analyses of the samples showed that the films grew in a tetragonal distorted structure. The Mössbauer spectra of the two films, measured at absorber temperatures in the range 301 K-700 K, comprised a central pair of paramagnetic doublets and a magnetic sextet feature in the wings. The magnetic component was resolved into (i) a component attributed to hyperfine interactions at Fe3+ ions located in octahedral sites (Bhf); and (ii) to Fe3+ ions in implantation induced lattice defects, which were characterized by a distribution of the magnetic field BDistr. The hyperfine magnetic field at the Fe probes in the octahedral site has a room temperature value of Bhf = 44.5(9) T. At higher sample temperatures, the Bhf becomes much weaker, with the Fe3+ hyperfine magnetic contribution disappearing above 700 K. Simultaneous analysis of the Ba-BFO eMS spectra shows that the variation of the hyperfine field with temperature follows the Brillouin curve for S = 5/2.



https://doi.org/10.3390/cryst13050724
Li, Feitao; Flock, Dominik; Wang, Dong; Schaaf, Peter
Solid-state dewetting of Ag/Ni bi-layers: accelerated void formation by the stress gradient in the bottom Ni layer. - In: Journal of alloys and compounds, ISSN 1873-4669, Bd. 960 (2023), 170735

Solid-state dewetting (SSD) of the immiscible Ag/Ni bi-layers was studied. After annealing at 400 &ring;C for 1 min, the Ag film was dewetted on the Ni film, and this is the first observation about the SSD of one metal film on another metal film. The easier dewetting of Ag than Ni was attributed to its lower melting point, faster grain boundary self-diffusion and poor wettability between them. At 500 &ring;C, the void formation in the bottom Ni layer was highlighted and compared to Ni single layer: many voids in the former while no visible voids in the latter, indicating that the presence of Ag accelerated the SSD of Ni. It was attributed to the vertical stress gradient in the bottom Ni film of Ag/Ni bi-layers, which accelerated the Ni diffusion and formation of the voids in the underlying Ni film around and below the Ag particles. Besides, voids were more easily formed below the Ag particles than between them due to the large lattice mismatch at the Ag/Ni interface and the possible formation of Ag-Ni alloys. The destabilization of the Ag on the Ni film contributes to the understanding of dewetting kinetics, which is beneficial to realize the controllable nanofabrication.



https://doi.org/10.1016/j.jallcom.2023.170735
Brokmann, Ulrike; Weigel, Christoph; Altendorf, Luisa-Marie; Strehle, Steffen; Rädlein, Edda
Wet chemical and plasma etching of photosensitive glass. - In: Solids, ISSN 2673-6497, Bd. 4 (2023), 3, S. 213-234

Photosensitive glasses for radiation-induced 3D microstructuring, due to their optical transparency and thermal, mechanical, and chemical resistance, enable the use of new strategies for numerous microscale applications, ranging from optics to biomedical systems. In this context, we investigated the plasma etching of photosensitive glasses after their exposure and compared it to the established wet chemical etching method, which offers new degrees of freedom in microstructuring control and microsystem fabrication. A CF4/H2 etching gas mixture with a constant volumetric flow of 30 sccm and a variable H2 concentration from 0% to 40% was utilized for plasma-based etching, while for wet chemical etching, diluted hydrofluoric acid (1% ≤ cHF ≤ 20%) was used. Therefore, both etching processes are based on a chemical etching attack involving fluorine ions. A key result is the observed reversion of the etch selectivity between the initial glassy and partially crystallized parts that evolve after UV exposure and thermal treatment. The crystallized parts were found to be 27 times more soluble than the unexposed glass parts during wet chemical etching. During the plasma etching process, the glassy components dissolve approximately 2.5 times faster than the partially crystalline components. Unlike wet chemical etching, the surfaces of plasma etched photostructured samples showed cone- and truncated-cone-shaped topographies, which supposedly resulted from self-masking effects during plasma etching, as well as a distinct physical contribution from the plasma etching process. The influences of various water species on the etching behaviors of the homogeneous glass and partially crystallized material are discussed based on FTIR-ATR and in relation to the respective etch rates and SNMS measurements.



https://doi.org/10.3390/solids4030014
Stauffenberg, Jaqueline; Reibe, Michael; Krötschl, Anja; Reuter, Christoph; Ortlepp, Ingo; Dontsov, Denis; Hesse, Steffen; Rangelow, Ivo W.; Strehle, Steffen; Manske, Eberhard
Tip-based nanofabrication below 40 nm combined with a nanopositioning machine with a movement range of Ø100 mm. - In: Micro and nano engineering, ISSN 2590-0072, Bd. 19 (2023), 100201, S. 1-5

In this paper, the combination of an advanced nanopositioning technique and a tip-based system, which can be used as an atomic force microscope (AFM) and especially for field emission scanning probe lithography (FESPL) is presented. This is possible through the use of active microcantilevers that allow easy switching between measurement and write modes. The combination of nanopositioning and nanomeasuring machines and tip-based systems overcomes the usual limitations of AFM technology and makes it possible to perform high-precision surface scanning and nanofabrication on wafer sizes up to 4 in. We specifically discuss the potential of nanofabrication via FESPL in combination with the nanofabrication machine (NFM-100). Results are presented, where nanofabrication is demonstrated in form of a spiral path over a total length of 1 mm and the potential of this technique in terms of accuracy is discussed. Furthermore, ten lines were written with a pitch of 100 nm and a linewidth below 40 nm was achieved, which is in principle possible over the entire range of motion.



https://doi.org/10.1016/j.mne.2023.100201
Mathew, Sobin; Reiprich, Johannes; Narasimha, Shilpashree; Abedin, Saadman; Kurtash, Vladislav; Thiele, Sebastian; Hähnlein, Bernd; Scheler, Theresa; Flock, Dominik; Jacobs, Heiko O.; Pezoldt, Jörg
Three-dimensional MoS2 nanosheet structures: CVD synthesis, characterization, and electrical properties. - In: Crystals, ISSN 2073-4352, Bd. 13 (2023), 3, 448, S. 1-14

The proposed study demonstrates a single-step CVD method for synthesizing three-dimensional vertical MoS2 nanosheets. The postulated synthesizing approach employs a temperature ramp with a continuous N2 gas flow during the deposition process. The distinctive signals of MoS2 were revealed via Raman spectroscopy study, and the substantial frequency difference in the characteristic signals supported the bulk nature of the synthesized material. Additionally, XRD measurements sustained the material’s crystallinity and its 2H-MoS2 nature. The FIB cross-sectional analysis provided information on the origin and evolution of the vertical MoS2 structures and their growth mechanisms. The strain energy produced by the compression between MoS2 islands is assumed to primarily drive the formation of vertical MoS2 nanosheets. In addition, vertical MoS2 structures that emerge from micro fissures (cracks) on individual MoS2 islands were observed and examined. For the evaluation of electrical properties, field-effect transistor structures were fabricated on the synthesized material employing standard semiconductor technology. The lateral back-gated field-effect transistors fabricated on the synthesized material showed an n-type behavior with field-effect mobility of 1.46 cm2 V^-1 s^-1 and an estimated carrier concentration of 4.5 × 10^12 cm^-2. Furthermore, the effects of a back-gate voltage bias and channel dimensions on the hysteresis effect of FET devices were investigated and quantified.



https://doi.org/10.3390/cryst13030448
Moritz, Dominik Christian; Calvet, Wolfram; Zare Pour, Mohammad Amin; Paszuk, Agnieszka; Mayer, Thomas; Hannappel, Thomas; Hofmann, Jan Philipp; Jaegermann, Wolfram
Dangling bond defects on Si surfaces and their consequences on energy band diagrams: from a photoelectrochemical perspective. - In: Solar RRL, ISSN 2367-198X, Bd. 7 (2023), 9, 2201063, S. 1-10

Using silicon in multijunction photocells leads to promising device structures for direct photoelectrochemical water splitting. In this regard, photoelectron spectra of silicon surfaces are used to investigate the energetic condition of contact formation. It is shown that the Fermi-level position at the surface differs from the values expected from their bulk doping concentrations, indicating significant surface band bending which may limit the overall device efficiency. In this study, the influence of different surface preparation procedures for p- and n-doped Si wafers on surface band bending is investigated. With the help of photoemission and X-ray absorption spectroscopy, Si dangling bonds are identified as dominating defect centers at Si surfaces. These defects lead to an occupied defect band in the lower half and an unoccupied defect band in the upper half of the Si bandgap. However, partial oxidation of the defect centers causes a shift of defect bands, with only donor states remaining in the Si bandgap. Source-induced photovoltages at cryogenic temperatures indicate that partial surface oxidation also decreases the recombination activity of these defect centers. It is shown that defect distribution, defect concentration, and source-induced photovoltages need to be considered when analyzing Fermi-level pinning at Si surfaces.



https://doi.org/10.1002/solr.202201063
Shekhawat, Deepshikha; Sudhahar, Dwarakesh; Döll, Joachim; Grieseler, Rolf; Pezoldt, Jörg
Phase formation of cubic silicon carbide from reactive silicon-carbon multilayers. - In: MRS advances, ISSN 2059-8521, Bd. 8 (2023), 9, S. 494-498

Silicon carbide layers were fabricated using self-propagating high-temperature synthesis of binary silicon-carbon based reactive multilayers. The silicon and carbon bilayers were fabricated with two different bilayer thicknesses. They are deposited by magnetron sputtering in an alternating layer system with a total thickness of 1 μm. The entire system is annealed by rapid thermal annealing at different temperatures ranging from 500 to 1100 &ring;C. From XRD analysis we could find that the formation of the silicon carbide phase was initiated from 700 &ring;C. With increasing bilayer thickness the silicon carbide phase formation was partially suppressed by the silicon recrystallization due to resulting lower carbon diffusion into silicon. The transformation process proceeds in a four-step process: densification/recrystallization, interdiffusion, nucleation and transformation. From this, it was noted that when compared to low bilayer thickness samples, the formation of the silicon carbide phase is delayed with increasing bilayer thickness and needs higher reaction initiation temperatures.



https://doi.org/10.1557/s43580-023-00531-3