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In the search for novel organic charge transfer salts with variable degrees of charge transfer we have studied the effects of two modifications of the recently synthesized donor–acceptor system [tetramethoxypyrene (TMP)]–[tetracyanoquinodimethane (TCNQ)]. One is of chemical nature by substituting the acceptor TCNQ molecules by F4TCNQ molecules. The second consists in simulating the application of uniaxial pressure along the stacking axis of the system. In order to test the chemical substitution, we have grown single crystals of the TMP–F4TCNQ complex and analyzed its electronic structure via electronic transport measurements, ab initio density functional theory (DFT) calculations and UV/VIS/IR absorption spectroscopy. This system shows an almost ideal geometrical overlap of nearly planar molecules stacked alternately (mixed stack) and this arrangement is echoed by a semiconductor-like transport behavior with an increased conductivity along the stacking direction. This is in contrast to TMP–TCNQ which shows a less pronounced anisotropy and a smaller conductivity response. Our band structure calculations confirm the one-dimensional behavior of TMP–F4TCNQ with pronounced dispersion only along the stacking axis. Infrared measurements illustrating the C[triple bond, length as m-dash]N vibration frequency shift in F4TCNQ suggest however no improvement in the degree of charge transfer in TMP–F4TCNQ with respect to TMP–TCNQ. In both complexes about 0.1e is transferred from TMP to the acceptor. Concerning the pressure effect, our DFT calculations on the designed TMP–TCNQ and TMP–F4TCNQ structures under different pressure conditions show that application of uniaxial pressure along the stacking axis of TMP–TCNQ may be the route to follow in order to obtain a much more pronounced charge transfer.
In this paper we present first-order reversal curve (FORC) diagrams of ensembles of three-dimensional Co3Fe nanostructures as 2 × 2 arrays of nano-cubes and nano-trees. The structures are fabricated and investigated by an advanced platform of focused electron beam induced deposition combined with high-resolution detection of magnetic stray fields using a home-built micro-Hall magnetometer based on an AlGaAs/GaAs heterostructure. The experimental FORC diagrams are compared to macrospin simulations for both geometries at different angles of the externally applied magnetic field. The measured FORC diagrams are in good agreement with the simulated ones and reflect non-uniform magnetization reversal dominated by multi-vortex states within, and strong magnetic coupling between, the building blocks of our nanostructures. Thus, a FORC analysis of small arrays of 3D magnetic nanostructures provides more detailed insights into the mechanisms of magnetization reversal beyond standard major hysteresis loop measurements.
Bei den im Rahmen des Forschungsverbundes erfolgten faunistischen Untersuchungen stand die Charakterisierung der unterschiedlichen, vor allem aber der wertvollen Biotoptypen der Braunkohlenfolgelandschaft mit Hilfe der dort lebenden Tierarten bzw. Artengemeinschaften im Vordergrund. Es wurden Tiergruppen bearbeitet, die zum einen ein hohes indikatorisches Potential besitzen, zum anderen unterschiedliche ökologische Hierachieebenen repräsentieren. Eine Auswertung der Ergebnisse erfolgte zumeist auf der Ebene der Biotoptypengruppen (siehe Heyde; Jakob; Köck; Reuter im gleichen Heft).
By the fabrication of periodically arranged nanomagnetic systems it is possible to engineer novel physical properties by realizing artificial lattice geometries that are not accessible via natural crystallization or chemical synthesis. This has been accomplished with great success in two dimensions in the fields of artificial spin ice and magnetic logic devices, to name just two. Although first proposals have been made to advance into three dimensions (3D), established nanofabrication pathways based on electron beam lithography have not been adapted to obtain free-form 3D nanostructures. Here we demonstrate the direct-write fabrication of freestanding ferromagnetic 3D nano-architectures. By employing micro-Hall sensing, we have determined the magnetic stray field generated by our free-form structures in an externally applied magnetic field and we have performed micromagnetic and macro-spin simulations to deduce the spatial magnetization profiles in the structures and analyze their switching behavior. Furthermore we show that the magnetic 3D elements can be combined with other 3D elements of different chemical composition and intrinsic material properties.
A careful analysis of the magneto-transport properties of epitaxial nanostructured Nb thin films in the normal and the mixed state is performed. The nanopatterns were prepared by focused ion beam (FIB) milling. They provide a washboard-like pinning potential landscape for vortices in the mixed state and simultaneously cause a resistivity anisotropy in the normal state. Two matching magnetic fields for the vortex lattice with the underlying nanostructures have been observed. By applying these fields, the most likely pinning sites along which the flux lines move through the samples have been selected. By this, either the background isotropic pinning of the pristine film or the enhanced isotropic pinning originating from the nanoprocessing have been probed. Via an Arrhenius analysis of the resistivity data the pinning activation energies for three vortex lattice parameters have been quantified. The changes in the electrical transport and the pinning properties have been correlated with the results of the microstructural and topographical characterization of the FIB-patterned samples. Accordingly, along with the surface processing, FIB milling has been found to alter the material composition and the degree of disorder in as-grown films. The obtained results provide further insight into the pinning mechanisms at work in FIB-nanopatterned superconductors, e.g. for fluxonic applications.
Focused electron beam induced deposition (FEBID) is a direct-write nanofabrication technique able to pattern three-dimensional magnetic nanostructures at resolutions comparable to the characteristic magnetic length scales. FEBID is thus a powerful tool for 3D nanomagnetism which enables unique fundamental studies involving complex 3D geometries, as well as nano-prototyping and specialized applications compatible with low throughputs. In this focused review, we discuss recent developments of this technique for applications in 3D nanomagnetism, namely the substantial progress on FEBID computational methods, and new routes followed to tune the magnetic properties of ferromagnetic FEBID materials. We also review a selection of recent works involving FEBID 3D nanostructures in areas such as scanning probe microscopy sensing, magnetic frustration phenomena, curvilinear magnetism, magnonics and fluxonics, offering a wide perspective of the important role FEBID is likely to have in the coming years in the study of new phenomena involving 3D magnetic nanostructures.
Fabrication of three-dimensional (3D) nanoarchitectures by focused electron beam induced deposition (FEBID) has matured to a level that highly complex and functional deposits are becoming available for nanomagnetics and plasmonics. However, the generation of suitable pattern files that control the electron beam’s movement, and thereby reliably map the desired target 3D structure from a purely geometrical description to a shape-conforming 3D deposit, is nontrivial. To address this issue we developed several writing strategies and associated algorithms implemented in C++. Our pattern file generator handles different proximity effects and corrects for height-dependent precursor coverage. Several examples of successful 3D nanoarchitectures using different precursors are presented that validate the effectiveness of the implementation.
Three-dimensional (3D) nanomagnetism, where spin configurations extend into the vertical direction of a substrate plane allow for more complex, hierarchical systems and the design of novel magnetic effects. As an important step towards this goal, we have recently demonstrated the direct-write fabrication of freestanding ferromagnetic 3D nano-architectures of ferromagnetic CoFe in shapes of nano-tree and nano-cube structures by means of focused electron beam induced deposition. Here, we present a comprehensive characterization of the magnetic properties of these structures by local stray-field measurements using a high-resolution micro-Hall magnetometer. Measurements in a wide range of temperatures and different angles of the externally applied magnetic field with respect to the surface plane of the sensor are supported by corresponding micromagnetic simulations, which explain the overall switching behavior of in part rather complex magnetization configurations remarkably well. In particular, the simulations yield coercive and switching fields that are in good quantitative correspondence with the measured coercive and switching fields assuming a bulk metal content of 100 at % consisting of bcc Co 3 Fe. We show that thermally-unstable magnetization states can be repetitively prepared and their lifetime controlled at will, a prerequisite to realizing dynamic and thermally-active magnetic configurations if the building blocks are to be used in lattice structures.
Focused electron and ion beam-induced deposition (FEBID/FIBID) are direct-write techniques with particular advantages in three-dimensional (3D) fabrication of ferromagnetic or superconducting nanostructures. Recently, two novel precursors, HCo 3 Fe(CO) 12 and Nb(NMe 3 ) 2 (N-t-Bu), were introduced, resulting in fully metallic CoFe ferromagnetic alloys by FEBID and superconducting NbC by FIBID, respectively. In order to properly define the writing strategy for the fabrication of 3D structures using these precursors, their temperature-dependent average residence time on the substrate and growing deposit needs to be known. This is a prerequisite for employing the simulation-guided 3D computer aided design (CAD) approach to FEBID/FIBID, which was introduced recently. We fabricated a series of rectangular-shaped deposits by FEBID at different substrate temperatures between 5 ∘ C and 24 ∘ C using the precursors and extracted the activation energy for precursor desorption and the pre-exponential factor from the measured heights of the deposits using the continuum growth model of FEBID based on the reaction-diffusion equation for the adsorbed precursor.
Directed deposition of silicon nanowires using neopentasilane as precursor and gold as catalyst
(2012)
In this work the applicability of neopentasilane (Si(SiH3)4) as a precursor for the formation of silicon nanowires by using gold nanoparticles as a catalyst has been explored. The growth proceeds via the formation of liquid gold/silicon alloy droplets, which excrete the silicon nanowires upon continued decomposition of the precursor. This mechanism determines the diameter of the Si nanowires. Different sources for the gold nanoparticles have been tested: the spontaneous dewetting of gold films, thermally annealed gold films, deposition of preformed gold nanoparticles, and the use of “liquid bright gold”, a material historically used for the gilding of porcelain and glass. The latter does not only form gold nanoparticles when deposited as a thin film and thermally annealed, but can also be patterned by using UV irradiation, providing access to laterally structured layers of silicon nanowires.
Nano-granular metals are materials that fall into the general class of granular electronic systems in which the interplay of electronic correlations, disorder and finite size effects can be studied. The charge transport in nano-granular metals is dominated by thermally-assisted, sequential and correlated tunneling over a temperature-dependent number of metallic grains. Here we study the frequency-dependent conductivity (AC conductivity) of nano-granular Platinum with Pt nano-grains embedded into amorphous carbon (C). We focus on the transport regime on the insulating side of the insulator metal transition reflected by a set of samples covering a range of tunnel-coupling strengths. In this transport regime polarization contributions to the AC conductivity are small and correlation effects in the transport of free charges are expected to be particularly pronounced. We find a universal behavior in the frequency dependence that can be traced back to the temperature-dependent zero-frequency conductivity (DC conductivity) of Pt/C within a simple lumped-circuit analysis. Our results are in contradistinction to previous work on nano-granular Pd/ZrO2ZrO2 in the very weak coupling regime where polarization contributions to the AC conductivity dominated. We describe possible future applications of nano-granular metals in proximity impedance spectroscopy of dielectric materials.
Controlling magnetic properties on the nanometer-scale is essential for basic research in micro-magnetism and spin-dependent transport, as well as for various applications such as magnetic recording, imaging and sensing. This has been accomplished to a very high degree by means of layered heterostructures in the vertical dimension. Here we present a complementary approach that allows for a controlled tuning of the magnetic properties of Co/Pt heterostructures on the lateral mesoscale. By means of in situ post-processing of Pt- and Co-based nano-stripes prepared by focused electron beam induced deposition (FEBID) we are able to locally tune their coercive field and remanent magnetization. Whereas single Co-FEBID nano-stripes show no hysteresis, we find hard-magnetic behavior for post-processed Co/Pt nano-stripes with coercive fields up to 850 Oe. We attribute the observed effects to the locally controlled formation of the CoPt L10 phase, whose presence has been revealed by transmission electron microscopy.
Vanadium and Manganese Carbonyls as Precursors in Electron-Induced and Thermal Deposition Processes
(2022)
The material composition and electrical properties of nanostructures obtained from focused electron beam-induced deposition (FEBID) using manganese and vanadium carbonyl precursors have been investigated. The composition of the FEBID deposits has been compared with thin films derived by the thermal decomposition of the same precursors in chemical vapor deposition (CVD). FEBID of V(CO)6 gives access to a material with a V/C ratio of 0.63–0.86, while in CVD a lower carbon content with V/C ratios of 1.1–1.3 is obtained. Microstructural characterization reveals for V-based materials derived from both deposition techniques crystallites of a cubic phase that can be associated with VC1−xOx. In addition, the electrical transport measurements of direct-write VC1−xOx show moderate resistivity values of 0.8–1.2 × 103 µΩ·cm, a negligible influence of contact resistances and signatures of a granular metal in the temperature-dependent conductivity. Mn-based deposits obtained from Mn2(CO)10 contain ~40 at% Mn for FEBID and a slightly higher metal percentage for CVD. Exclusively insulating material has been observed in FEBID deposits as deduced from electrical conductivity measurements. In addition, strong tendencies for postgrowth oxidation have to be considered.
Biological exploration of early biomarkers for chronic kidney disease (CKD) in (pre)diabetic individuals is crucial for personalized management of diabetes. Here, we evaluated two candidate biomarkers of incident CKD (sphingomyelin (SM) C18:1 and phosphatidylcholine diacyl (PC aa) C38:0) concerning kidney function in hyperglycemic participants of the Cooperative Health Research in the Region of Augsburg (KORA) cohort, and in two biofluids and six organs of leptin receptor-deficient (db/db) mice and wild type controls. Higher serum concentrations of SM C18:1 and PC aa C38:0 in hyperglycemic individuals were found to be associated with lower estimated glomerular filtration rate (eGFR) and higher odds of CKD. In db/db mice, both metabolites had a significantly lower concentration in urine and adipose tissue, but higher in the lungs. Additionally, db/db mice had significantly higher SM C18:1 levels in plasma and liver, and PC aa C38:0 in adrenal glands. This cross-sectional human study confirms that SM C18:1 and PC aa C38:0 associate with kidney dysfunction in pre(diabetic) individuals, and the animal study suggests a potential implication of liver, lungs, adrenal glands, and visceral fat in their systemic regulation. Our results support further validation of the two phospholipids as early biomarkers of renal disease in patients with (pre)diabetes.
Most of superconductors in a magnetic field are penetrated by a lattice of quantized flux vortices. In the presence of a transport current causing the vortices to cross sample edges, emission of electromagnetic waves is expected due to the continuity of tangential components of the fields at the surface. Yet, such a radiation has not been observed so far due to low radiated power levels and lacking coherence in the vortex motion. Here, we clearly evidence the emission of electromagnetic waves from vortices crossing the layers of a superconductor/insulator Mo/Si superlattice. The emission spectra consist of narrow harmonically related peaks which can be finely tuned in the GHz range by the dc bias current and, coarsely, by the in-plane magnetic field value. Our findings show that superconductor/insulator superlattices can act as dc-tunable microwave generators bridging the frequency gap between conventional radiofrequency oscillators and (sub-)terahertz generators relying upon the Josephson effect.
The interaction of (quasi)particles with a periodic potential arises in various domains of science and engineering, such as solid-state physics, chemical physics, and communication theory. An attractive test ground to investigate this interaction is represented by superconductors with artificial pinning sites, where magnetic flux quanta (Abrikosov vortices) interact with the pinning potential U(r) = U(r + R) induced by a nanostructure. At a combination of microwave and dc currents, fluxons act as mobile probes of U(r): The ac component shakes the fluxons in the vicinity of their equilibrium points which are unequivocally determined by the local pinning force counterbalanced by the Lorentz force induced by the dc current, linked to the curvature of U(r) which can then be used for a successful fitting of the voltage responses. A good correlation of the deduced dependences U(r) with the cross sections of the nanostructures points to that pinning is primarily caused by vortex length reduction. Our findings pave a new route to a non-destructive evaluation of periodic pinning in superconductor thin films. The approach should also apply to a broad class of systems whose evolution in time can be described by the coherent motion of (quasi)particles in a periodic potential.
Der 3D‐Druck von geometrisch komplexen Nanostrukturen ist auf dem Weg zu ersten Anwendungen. Die Auswahl an geeigneten Materialien ermöglicht metallische, halbleitende, isolierende, supraleitende und exotische magnetische Eigenschaften. Das 3D‐FEBID‐Verfahren schreibt mit dem Elektronenstrahl eines Raster‐Elektronenmikroskops wie mit einem Nanostift. Das Material wird als Gasstrom von Precursor‐Molekülen über eine Hohlnadel zugeführt. Der Elektronenstrahl ermöglicht die hochlokale Fragmentierung dieser Moleküle, die meist metallische Zielatome enthalten. Die lokale Verweildauer des Strahls steuert den Strukturaufbau in der Vertikalen, während seine seitliche Bewegung zu geneigten, freistehenden Strukturen führt. Eine Herausforderung ist die definierte Strahlsteuerung, um ein CAD‐Modell möglichst präzise in ein reales 3D‐Nanoobjekt zu überführen. Für die Zukunft soll eine simulationsgestützte Software zur Steuerung des Elektronenstrahls auch Laien die Anwendung erleichtern. 3D‐FEBID ist bereits heute ein zuverlässiges und in vielerlei Hinsicht einzigartiges Verfahren zur Direktabscheidung funktionaler Nanostrukturen.
The influence of an ac current of arbitrary amplitude and frequency on the mixed-state dc-voltage-ac-drive tiltingratchet response of a superconducting film with uniaxial cosine pinning potential at finite temperature is theoretically investigated. The results are obtained in the single-vortex approximation, within the frame of an exact solution of the Langevin equation for non-interacting vortices. Both experimentally achievable, the dc ratchet response and absorbed ac power are predicted to demonstrate a pronounced filter-like behavior at microwave frequencies. Based on our findings, we propose a cut-off filter and discuss its operating curves as functions of the driving parameters, i.e, ac amplitude, frequency, and dc bias. The predicted results can be examined, e.g, on superconducting films with a washboard pinning potential landscape.