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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.
We present the application of an evolutionary genetic algorithm for the in situ optimization of nanostructures that are prepared by focused electron-beam-induced deposition (FEBID). It allows us to tune the properties of the deposits towards the highest conductivity by using the time gradient of the measured in situ rate of change of conductance as the fitness parameter for the algorithm. The effectiveness of the procedure is presented for the precursor W(CO)6 as well as for post-treatment of Pt–C deposits, which were obtained by the dissociation of MeCpPt(Me)3. For W(CO)6-based structures an increase of conductivity by one order of magnitude can be achieved, whereas the effect for MeCpPt(Me)3 is largely suppressed. The presented technique can be applied to all beam-induced deposition processes and has great potential for a further optimization or tuning of parameters for nanostructures that are prepared by FEBID or related techniques.
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.
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.
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.
We present experimental results and theoretical simulations of the adsorption behavior of the metal–organic precursor Co2(CO)8 on SiO2 surfaces after application of two different pretreatment steps, namely by air plasma cleaning or a focused electron beam pre-irradiation. We observe a spontaneous dissociation of the precursor molecules as well as autodeposition of cobalt on the pretreated SiO2 surfaces. We also find that the differences in metal content and relative stability of these deposits depend on the pretreatment conditions of the substrate. Transport measurements of these deposits are also presented. We are led to assume that the degree of passivation of the SiO2 surface by hydroxyl groups is an important controlling factor in the dissociation process. Our calculations of various slab settings, using dispersion-corrected density functional theory, support this assumption. We observe physisorption of the precursor molecule on a fully hydroxylated SiO2 surface (untreated surface) and chemisorption on a partially hydroxylated SiO2 surface (pretreated surface) with a spontaneous dissociation of the precursor molecule. In view of these calculations, we discuss the origin of this dissociation and the subsequent autocatalysis.
Background: Focused electron beam induced deposition (FEBID) is a direct-writing technique with nanometer resolution, which has received strongly increasing attention within the last decade. In FEBID a precursor previously adsorbed on a substrate surface is dissociated in the focus of an electron beam. After 20 years of continuous development FEBID has reached a stage at which this technique is now particularly attractive for several areas in both, basic and applied research. The present topical review addresses selected examples that highlight this development in the areas of charge-transport regimes in nanogranular metals close to an insulator-to-metal transition, the use of these materials for strain- and magnetic-field sensing, and the prospect of extending FEBID to multicomponent systems, such as binary alloys and intermetallic compounds with cooperative ground states.
Results: After a brief introduction to the technique, recent work concerning FEBID of Pt–Si alloys and (hard-magnetic) Co–Pt intermetallic compounds on the nanometer scale is reviewed. The growth process in the presence of two precursors, whose flux is independently controlled, is analyzed within a continuum model of FEBID that employs rate equations. Predictions are made for the tunability of the composition of the Co–Pt system by simply changing the dwell time of the electron beam during the writing process. The charge-transport regimes of nanogranular metals are reviewed next with a focus on recent theoretical advancements in the field. As a case study the transport properties of Pt–C nanogranular FEBID structures are discussed. It is shown that by means of a post-growth electron-irradiation treatment the electronic intergrain-coupling strength can be continuously tuned over a wide range. This provides unique access to the transport properties of this material close to the insulator-to-metal transition. In the last part of the review, recent developments in mechanical strain-sensing and the detection of small, inhomogeneous magnetic fields by employing nanogranular FEBID structures are highlighted.
Conclusion: FEBID has now reached a state of maturity that allows a shift of the focus towards the development of new application fields, be it in basic research or applied. This is shown for selected examples in the present review. At the same time, when seen from a broader perspective, FEBID still has to live up to the original idea of providing a tool for electron-controlled chemistry on the nanometer scale. This has to be understood in the sense that, by providing a suitable environment during the FEBID process, the outcome of the electron-induced reactions can be steered in a controlled way towards yielding the desired composition of the products. The development of a FEBID-specialized surface chemistry is mostly still in its infancy. Next to application development, it is this aspect that will likely be a guiding light for the future development of the field of focused electron beam induced deposition.
This paper introduces a new methodology for the fabrication of strain-sensor elements for MEMS and NEMS applications based on the tunneling effect in nano-granular metals. The strain-sensor elements are prepared by the maskless lithography technique of focused electron-beam-induced deposition (FEBID) employing the precursor trimethylmethylcyclopentadienyl platinum [MeCpPt(Me)3]. We use a cantilever-based deflection technique to determine the sensitivity (gauge factor) of the sensor element. We find that its sensitivity depends on the electrical conductivity and can be continuously tuned, either by the thickness of the deposit or by electron-beam irradiation leading to a distinct maximum in the sensitivity. This maximum finds a theoretical rationale in recent advances in the understanding of electronic charge transport in nano-granular metals.
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).