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Electron-assisted oxidation of Co-Si-based focused electron beam induced deposition (FEBID) materials is shown to form a 2-4 nm metal oxide surface layer on top of an electrically insulating silicon oxide layer less than 10 nm thick. Differences between thermal and electron-induced oxidation on the resulting microstructure are illustrated.

Additive nanotechnology enable curvilinear and three-dimensional (3D) magnetic architectures with tunable topology and functionalities surpassing their planar counterparts. Here, we experimentally reveal that 3D soft magnetic wireframe structures resemble compact manifolds and accommodate magnetic textures of high order vorticity determined by the Euler characteristic, χ. We demonstrate that self-standing magnetic tetrapods (homeomorphic to a sphere; χ = + 2) support six surface topological solitons, namely four vortices and two antivortices, with a total vorticity of + 2 equal to its Euler characteristic. Alternatively, wireframe structures with one loop (homeomorphic to a torus; χ = 0) possess equal number of vortices and antivortices, which is relevant for spin-wave splitters and 3D magnonics. Subsequent introduction of n holes into the wireframe geometry (homeomorphic to an n-torus; χ < 0) enables the accommodation of a virtually unlimited number of antivortices, which suggests their usefulness for non-conventional (e.g., reservoir) computation. Furthermore, complex stray-field topologies around these objects are of interest for superconducting electronics, particle trapping and biomedical applications., (© 2024. The Author(s).)

The investigation of precursor classes for the fabrication of nanostructures is of specific interest for maskless fabrication and direct nanoprinting. In this study, the differences in material composition depending on the employed process are illustrated for focused-ion-beam- and focused-electron-beam-induced deposition (FIBID/FEBID) and compared to the thermal decomposition in chemical vapor deposition (CVD). This article reports on specific differences in the deposit composition and microstructure when the (H 3 Si) 2 Fe(CO) 4 precursor is converted into an inorganic material. Maximum metal/metalloid contents of up to 90 at. % are obtained in FIBID deposits and higher than 90 at. % in CVD films, while FEBID with the same precursor provides material containing less than 45 at. % total metal/metalloid content. Moreover, the Fe:Si ratio is retained well in FEBID and CVD processes, but FIBID using Ga + ions liberates more than 50% of the initial Si provided by the precursor. This suggests that precursors for FIBID processes targeting binary materials should include multiple bonding such as bridging positions for nonmetals. In addition, an in situ method for investigations of supporting thermal effects of precursor fragmentation during the direct-writing processes is presented, and the applicability of the precursor for nanoscale 3D FEBID writing is demonstrated., Competing Interests: The authors declare no competing financial interest., (© 2024 American Chemical Society.)

Electron-induced fragmentation of the HFeCo 3 (CO) 12 precursor allows direct-write fabrication of 3D nanostructures with metallic contents of up to >95 at %. While microstructure and composition determine the physical and functional properties of focused electron beam-induced deposits, they also provide fundamental insights into the decomposition process of precursors, as elaborated in this study based on EDX and TEM. The results provide solid information suggesting that different dominant fragmentation channels are active in single-spot growth processes for pillar formation. The use of the single source precursor provides a unique insight into high- and low-energy fragmentation channels being active in the same deposit formation process.

Magnonics is a rapidly developing domain of nanomagnetism, with application potential in information processing systems. Realisation of this potential and miniaturisation of magnonic circuits requires their extension into the third dimension. However, so far, magnonic conduits are largely limited to thin films and 2D structures. Here, we introduce 3D magnonic nanoconduits fabricated by the direct write technique of focused-electron-beam induced deposition (FEBID). We use Brillouin light scattering (BLS) spectroscopy to demonstrate significant qualitative differences in spatially resolved spin-wave resonances of 2D and 3D nanostructures, which originates from the geometrically induced non-uniformity of the internal magnetic field. This work demonstrates the capability of FEBID as an additive manufacturing technique to produce magnetic 3D nanoarchitectures and presents the first report of BLS spectroscopy characterisation of FEBID conduits.

The Sencell sensor uses glucose-induced changes in an osmotic pressure chamber for continuous glucose measurement. A final device shall have the size of a grain of rice. The size limiting factor is the piezo-resistive pressure transducers inside the core sensor technology (resulting chamber volume: 70 µL. To achieve the necessary miniaturization, these pressure transducers were replaced by small (4000 × 400 × 150 nm³) nano-granular tunneling resistive (NTR) pressure sensors (chamber volume: 750 nL). For benchmark testing, we filled the miniaturized chamber with bovine serum albumin (BSA, 1 mM) and exposed it repeatedly to distilled water followed by 1 mM BSA solution. Thereafter, we manufactured sensors with glucose testing chemistry (ConcanavalinA/dextran) and investigated sensor performance with dynamic glucose changes between 0 and 300 mg/dL. Evaluation of the miniaturized sensors resulted in reliable pressure changes, both in the BSA benchmark experiment (30-35 mBar) and in the dynamic in vitro continuous glucose test (40-50 mBar). These pressure results were comparable to similar experiments with the previous larger in vitro sensors (30-50 mBar). In conclusion, the NTR pressure sensor technology was successfully employed to reduce the size of the core osmotic pressure chamber by more than 95% without loss in the osmotic pressure signal.

Recent advancements in additive manufacturing have enabled the preparation of free-shaped 3D objects with feature sizes down to and below the micrometer scale. Among the fabrication methods, focused electron beam- and focused ion beam-induced deposition (FEBID and FIBID, respectively) associate a high flexibility and unmatched accuracy in 3D writing with a wide material portfolio, thereby allowing for the growth of metallic to insulating materials. The combination of the free-shaped 3D nanowriting with established chemical vapor deposition (CVD) techniques provides attractive opportunities to synthesize complex 3D core-shell heterostructures. Hence, this hybrid approach enables the fabrication of morphologically tunable layer-based nanostructures with the great potential of unlocking further functionalities. Here, the fundamentals of such a hybrid approach are demonstrated by preparing core-shell heterostructures using 3D FEBID scaffolds for site-selective CVD. In particular, 3D microbridges are printed by FEBID with the (CH 3 ) 3 CH 3 C 5 H 4 Pt precursor and coated by thermal CVD using the Nb(NMe 2 ) 3 (N- t -Bu) and HFeCo 3 (CO) 12 precursors. Two model systems on the basis of CVD layers consisting of a superconducting NbC-based layer and a ferromagnetic Co 3 Fe layer are prepared and characterized with regard to their composition, microstructure, and magneto-transport properties.

Focused electron-beam-induced deposition (FEBID) is a highly versatile direct-write approach with particular strengths in the 3D nanofabrication of functional materials. Despite its apparent similarity to other 3D printing approaches, non-local effects related to precursor depletion, electron scattering and sample heating during the 3D growth process complicate the shape-true transfer from a target 3D model to the actual deposit. Here, we describe an efficient and fast numerical approach to simulate the growth process, which allows for a systematic study of the influence of the most important growth parameters on the resulting shape of the 3D structures. The precursor parameter set derived in this work for the precursor Me 3 PtCpMe enables a detailed replication of the experimentally fabricated nanostructure, taking beam-induced heating into account. The modular character of the simulation approach allows for additional future performance increases using parallelization or drawing on the use of graphics cards. Ultimately, beam-control pattern generation for 3D FEBID will profit from being routinely combined with this fast simulation approach for optimized shape transfer.

We fabricated memristive devices using focused electron beam-induced deposition (FEBID) as a direct-writing technique employing a Pt/TiO 2 /Pt sandwich layer device configuration. Pinching in the measured current-voltage characteristics ( i-v ), the characteristic fingerprint of memristive behavior was clearly observed. The temperature dependence was measured for both high and low resistive states in the range from 290 K down to about 2 K, showing a stretched exponential behavior characteristic of Mott-type variable-range hopping. From this observation, a valence change mechanism of the charge transport inside the TiO 2 layer can be deduced.

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 VC 1-x O x . In addition, the electrical transport measurements of direct-write VC 1-x O x show moderate resistivity values of 0.8-1.2 × 10 3 µΩ·cm, a negligible influence of contact resistances and signatures of a granular metal in the temperature-dependent conductivity. Mn-based deposits obtained from Mn 2 (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.

Two new precursors for focused electron beam-induced deposition (FEBID) of cobalt silicides have been synthesized and evaluated. The H 3 SiCo(CO) 4 and H 2 Si(Co(CO) 4 ) 2 single-source precursors retain the initial metal ratios and show low sensitivity to changes in the FEBID parameters such as acceleration voltage, beam current, and precursor pressure. The precursors allow the direct writing of material containing ∼55 to 60 at % total metal/metalloid content combined with high growth rates. During the deposition process an average of ∼80% of the carbonyl ligands are cleaved off in these planar deposits. Postgrowth electron curing does not change the deposits' composition, but resistivities decrease after the curing procedure. Temperature-dependent electrical properties indicate the presence of a granular metal for both cured samples and the as-grown Co 2 Si deposit, while the as-grown CoSi material is on the insulating side of the metal-insulator transition. The observed magnetoresistance behavior is indicative of tunneling magnetoresistance and is substantially reduced upon postgrowth irradiation treatment.

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/[Formula: see text] 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., (© 2021. The Author(s).)

Scanning Hall probe microscopy is attractive for minimally invasive characterization of magnetic thin films and nanostructures by measurement of the emanating magnetic stray field. Established sensor probes operating at room temperature employ highly miniaturized spin-valve elements or semimetals, such as Bi. As the sensor layer structures are fabricated by patterning of planar thin films, their adaption to custom-made sensor probe geometries is highly challenging or impossible. Here we show how nanogranular ferromagnetic Hall devices fabricated by the direct-write method of focused electron beam induced deposition (FEBID) can be tailor-made for any given probe geometry. Furthermore, we demonstrate how the magnetic stray field sensitivity can be optimized in situ directly after direct-write nanofabrication of the sensor element. First proof-of-principle results on the use of this novel scanning Hall sensor are shown.

The increasing demand for nanoscale magnetic devices requires development of 3D magnetic nanostructures. In this regard, focused electron beam induced deposition (FEBID) is a technique of choice for direct-writing of complex nano-architectures with applications in nanomagnetism, magnon spintronics, and superconducting electronics. However, intrinsic properties of nanomagnets are often poorly known and can hardly be assessed by local optical probe techniques. Here, an original spatially resolved approach is demonstrated for spin-wave spectroscopy of individual circular magnetic elements with sample volumes down to about 10-3 μm3. The key component of the setup is a coplanar waveguide whose microsized central part is placed over a movable substrate with well-separated CoFe-FEBID nanodisks which exhibit standing spin-wave resonances. The circular symmetry of the disks allows for the deduction of the saturation magnetization and the exchange stiffness of the material using an analytical theory. A good correspondence between the results of analytical calculations and micromagnetic simulations is revealed, indicating a validity of the used analytical model going beyond the initial thin-disk approximation used in the theoretical derivation. The presented approach is especially valuable for the characterization of direct-write magnetic elements opening new horizons for 3D nanomagnetism and magnonics.

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.

Scanning probe microscopy (SPM) has become an essential surface characterization technique in research and development. By concept, SPM performance crucially depends on the quality of the nano-probe element, in particular, the apex radius. Now, with the development of advanced SPM modes beyond morphology mapping, new challenges have emerged regarding the design, morphology, function, and reliability of nano-probes. To tackle these challenges, versatile fabrication methods for precise nano-fabrication are needed. Aside from well-established technologies for SPM nano-probe fabrication, focused electron beam-induced deposition (FEBID) has become increasingly relevant in recent years, with the demonstration of controlled 3D nanoscale deposition and tailored deposit chemistry. Moreover, FEBID is compatible with practically any given surface morphology. In this review article, we introduce the technology, with a focus on the most relevant demands (shapes, feature size, materials and functionalities, substrate demands, and scalability), discuss the opportunities and challenges, and rationalize how those can be useful for advanced SPM applications. As will be shown, FEBID is an ideal tool for fabrication / modification and rapid prototyping of SPM-tipswith the potential to scale up industrially relevant manufacturing., Competing Interests: The authors declare no conflict of interest.

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.

Superconducting planar nanostructures are widely used in applications, e.g., for highly sensitive magnetometers and in basic research, e.g., to study finite size effects or vortex dynamics. In contrast, 3D superconducting nanostructures, despite their potential in quantum information processing and nanoelectronics, have been addressed only in a few pioneering experiments. This is due to the complexity of fabricating 3D nanostructures by conventional techniques such as electron-beam lithography and to the scarce number of superconducting materials available for direct-writing techniques, which enable the growth of 3D free-standing nanostructures. Here, we present a comparative study of planar nanowires and free-standing 3D nanowires fabricated by focused electron- and ion (Ga+)-beam induced deposition (FEBID and FIBID) using the precursor Nb(NMe 2 ) 3 (N- t-Bu). FEBID nanowires contain about 67 atomic percent C, 22 atomic percent N, and 11 atomic percent Nb, while FIBID samples are composed of 43 atomic percent C, 13 atomic percent N, 15.5 atomic percent Ga, and 28.5 atomic percent Nb. Transmission electron microscopy shows that FEBID samples are amorphous, while FIBID samples exhibit a fcc NbC polycrystalline structure, with grains about 15-20 nm in diameter. Electrical transport measurements show that FEBID nanowires are highly resistive following a variable-range-hopping behavior. In contradistinction, FIBID planar nanowires become superconducting at T c ≈ 5 K. In addition, the critical temperature of free-standing 3D nanowires is as high as T c ≈ 11 K, which is close to the value of bulk NbC. In conclusion, FIBID-NbC is a promising material for the fabrication of superconducting nanowire single-photon detectors (SNSPD) and for the development of 3D superconductivity with applications in quantum information processing and nanoelectronics.

Local modification of magnetic properties of nanoelements is a key to design future-generation magnonic devices in which information is carried and processed via spin waves. One of the biggest challenges here is to fabricate simple and miniature phase-controlling elements with broad tunability. Here, we successfully realize such spin-wave phase shifters upon a single nanogroove milled by a focused ion beam in a Co-Fe microsized magnonic waveguide. By varying the groove depth and the in-plane bias magnetic field, we continuously tune the spin-wave phase and experimentally evidence a complete phase inversion. The microscopic mechanism of the phase shift is based on the combined action of the nanogroove as a geometrical defect and the lower spin-wave group velocity in the waveguide under the groove where the magnetization is reduced due to the incorporation of Ga ions during the ion-beam milling. The proposed phase shifter can easily be on-chip integrated with spin-wave logic gates and other magnonic devices. Our findings are crucial for designing nanomagnonic circuits and for the development of spin-wave nano-optics.

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.

We adjust the Proof of Work (PoW) consensus mechanism used in Bitcoin and Ethereum so that we can build on its strength while also addressing, in part, some of its perceived weaknesses. Notably, our work is motivated by the high energy consumption for mining PoW, and we want to restrict the use of PoW to a configurable, expected size of nodes, as a function of the local blockchain state. The approach we develop for this rests on three pillars: (i) Proof of Kernel Work (PoKW), a means of dynamically reducing the set of nodes that can participate in the solving of PoW puzzles such that an adversary cannot increase his attack surface because of such a reduction; (ii) Practical Adaptation of Existing Technology , a realization of this PoW reduction through an adaptation of existing blockchain and enterprise technology stacks; and (iii) Machine Learning for Adaptive System Resiliency , the use of techniques from artificial intelligence to make our approach adaptive to system, network and attack dynamics. We develop here, in detail, the first pillar and illustrate the second pillar through a real use case, a pilot project done with Porsche on controlling permissions to vehicle and data log accesses. We also discuss pertinent attack vectors for PoKW consensus and their mitigation. Moreover, we sketch how our approach may lead to more democratic PoKW-based blockchain systems for public networks that may inherit the resilience of blockchains based on PoW., Competing Interests: We declare we have no competing interests.

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 low-temperature chemical vapor growth of Ge nanowires using Ga as seed material is demonstrated. The structural and chemical analysis reveals the homogeneous incorporation of ∼3.5 at. % Ga in the Ge nanowires. The Ga-containing Ge nanowires behave like metallic conductors with a resistivity of about ∼300 μΩcm due to Ga hyperdoping with electronic contributions of one-third of the incorporated Ga atoms. This is the highest conduction value observed by in situ doping of group IV nanowires reported to date. This work demonstrates that Ga is both an efficient seed material at low temperatures for Ge nanowire growth and an effective dopant changing the semiconductor into a metal-like conductor.

In the current contribution we present a comprehensive study on the heteronuclear carbonyl complex H 2 FeRu 3 (CO) 13 covering its low energy electron induced fragmentation in the gas phase through dissociative electron attachment (DEA) and dissociative ionization (DI), its decomposition when adsorbed on a surface under controlled ultrahigh vacuum (UHV) conditions and exposed to irradiation with 500 eV electrons, and its performance in focused electron beam induced deposition (FEBID) at room temperature under HV conditions. The performance of this precursor in FEBID is poor, resulting in maximum metal content of 26 atom % under optimized conditions. Furthermore, the Ru/Fe ratio in the FEBID deposit (≈3.5) is higher than the 3:1 ratio predicted. This is somewhat surprising as in recent FEBID studies on a structurally similar bimetallic precursor, HFeCo 3 (CO) 12 , metal contents of about 80 atom % is achievable on a routine basis and the deposits are found to maintain the initial Co/Fe ratio. Low temperature (≈213 K) surface science studies on thin films of H 2 FeRu 3 (CO) 13 demonstrate that electron stimulated decomposition leads to significant CO desorption (average of 8-9 CO groups per molecule) to form partially decarbonylated intermediates. However, once formed these intermediates are largely unaffected by either further electron irradiation or annealing to room temperature, with a predicted metal content similar to what is observed in FEBID. Furthermore, gas phase experiments indicate formation of Fe(CO) 4 from H 2 FeRu 3 (CO) 13 upon low energy electron interaction. This fragment could desorb at room temperature under high vacuum conditions, which may explain the slight increase in the Ru/Fe ratio of deposits in FEBID. With the combination of gas phase experiments, surface science studies and actual FEBID experiments, we can offer new insights into the low energy electron induced decomposition of this precursor and how this is reflected in the relatively poor performance of H 2 FeRu 3 (CO) 13 as compared to the structurally similar HFeCo 3 (CO) 12 .

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., Competing Interests: The authors declare no conflict of interest.

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.

Correlated valence electrons in Ag and Cu are investigated using double photoemission spectroscopy driven by a high-order harmonic light source. Electron pairs consisting of two d electrons as well as pairs with one sp and one d electron are resolved in the two-dimensional energy spectrum. Surprisingly, the intensity ratio of sp-d to d-d pairs from Ag is 3 times higher than in the self-convoluted density of states. Our results directly show the band-resolved configurations of electron pairs in solids and emphasize a band-dependent picture for electron correlation even in these paradigmatic metals.

Alongside the development of artificially created magnetic nanostructures, micro-Hall magnetometry has proven to be a versatile tool to obtain high-resolution hysteresis loop data and access dynamical properties. Here we explore the application of First Order Reversal Curves (FORC)-a technique well-established in the field of paleomagnetism for studying grain-size and interaction effects in magnetic rocks-to individual and dipolar-coupled arrays of magnetic nanostructures using micro-Hall sensors. A proof-of-principle experiment performed on a macroscopic piece of a floppy disk as a reference sample well known in the literature demonstrates that the FORC diagrams obtained by magnetic stray field measurements using home-built magnetometers are in good agreement with magnetization data obtained by a commercial vibrating sample magnetometer. We discuss in detail the FORC diagrams and their interpretation of three different representative magnetic systems, prepared by the direct-write Focused Electron Beam Induced Deposition (FEBID) technique: (1) an isolated Co-nanoisland showing a simple square-shaped hysteresis loop, (2) a more complex CoFe-alloy nanoisland exhibiting a wasp-waist-type hysteresis, and (3) a cluster of interacting Co-nanoislands. Our findings reveal that the combination of FORC and micro-Hall magnetometry is a promising tool to investigate complex magnetization reversal processes within individual or small ensembles of nanomagnets grown by FEBID or other fabrication methods. The method provides sub-μm spatial resolution and bridges the gap of FORC analysis, commonly used for studying macroscopic samples and rather large arrays, to studies of small ensembles of interacting nanoparticles with the high moment sensitivity inherent to micro-Hall magnetometry.

The sensitivity and detection speed of cantilever-based mechanical sensors increases drastically through size reduction. The need for such increased performance for high-speed nanocharacterization and bio-sensing, drives their sub-micrometre miniaturization in a variety of research fields. However, existing detection methods of the cantilever motion do not scale down easily, prohibiting further increase in the sensitivity and detection speed. Here we report a nanomechanical sensor readout based on electron co-tunnelling through a nanogranular metal. The sensors can be deposited with lateral dimensions down to tens of nm, allowing the readout of nanoscale cantilevers without constraints on their size, geometry or material. By modifying the inter-granular tunnel-coupling strength, the sensors' conductivity can be tuned by up to four orders of magnitude, to optimize their performance. We show that the nanoscale printed sensors are functional on 500 nm wide cantilevers and that their sensitivity is suited even for demanding applications such as atomic force microscopy.

We report on a combined theoretical and experimental investigation of the superconducting state in the quasi-two-dimensional organic superconductor κ-(ET)&#95;{2}Cu[N(CN)&#95;{2}]Br. Applying spin-fluctuation theory to a low-energy, material-specific Hamiltonian derived from ab initio density functional theory we calculate the quasiparticle density of states in the superconducting state. We find a distinct three-peak structure that results from a strongly anisotropic mixed-symmetry superconducting gap with eight nodes and twofold rotational symmetry. This theoretical prediction is supported by low-temperature scanning tunneling spectroscopy on in situ cleaved single crystals of κ-(ET)&#95;{2}Cu[N(CN)&#95;{2}]Br with the tunneling direction parallel to the layered structure.

The local density of states (DOS) of the organic superconductor κ-(BEDT-TTF)2Cu[N(CN)2]Br, measured by scanning tunneling spectroscopy on in situ cleaved surfaces, reveals a logarithmic suppression near the Fermi edge persisting above the critical temperature T(c). The experimentally observed suppression of the DOS is in excellent agreement with a soft Hubbard gap as predicted by the Anderson-Hubbard model for systems with disorder. The electronic disorder also explains the diminished coherence peaks of the quasi-particle DOS below T(c).

Charging of physical phase plates is a problem that has prevented their routine use in transmission electron microscopy of weak-phase objects. In theory, electrostatic phase plates are superior to thin-film phase plates since they do not attenuate the scattered electron beam and allow freely adjustable phase shifts. Electrostatic phase plates consist of multiple layers of conductive and insulating materials, and are thus more prone to charging than thin-film phase plates, which typically consist of only one single layer of amorphous material. We have addressed the origins of charging of Boersch phase plates and show how it can be reduced. In particular, we have performed simulations and experiments to analyze the influence of the insulating Si3N4 layers and surface charges on electrostatic charging. To optimize the performance of electrostatic phase plates, it would be desirable to fabricate electrostatic phase plates, which (i) impart a homogeneous phase shift to the unscattered electrons, (ii) have a low cut-on frequency, (iii) expose as little material to the intense unscattered beam as possible, and (iv) can be additionally polished by a focused ion-beam instrument to eliminate carbon contamination accumulated during exposure to the unscattered electron beam (Walter et al., 2012, Ultramicroscopy, 116, 62-72). We propose a new type of electrostatic phase plate that meets the above requirements and would be superior to a Boersch phase plate. It consists of three free-standing coaxial rods converging in the center of an aperture (3-fold coaxial phase plate). Simulations and preliminary experiments with modified Boersch phase plates indicate that the fabrication of a 3-fold coaxial phase plate is feasible., (Copyright © 2015 Elsevier B.V. All rights reserved.)

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.

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≡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 the majority of cases, nanostructures prepared by focused electron beam induced deposition employing an organometallic precursor contain predominantly carbon-based ligand dissociation products. This is unfortunate with regard to using this high-resolution direct-write approach for the preparation of nanostructures for various fields, such as mesoscopic physics, micromagnetism, metaoptical phenomena in the visible spectral range, or others. Following early attempts of postprocessing Pt-based structures prepared by focused electron beam induced deposition at several hundred degrees Celsius in a reactive gas atmosphere, recent work has focused on developing in situ purification processes by using a stationary O2 flux in combination with electron irradiation to oxidize the carbonaceous component of the deposits. Here we show that this purification process is driven by the catalytic activity of Pt and in fact does not rely on the parallel electron irradiation process to function, if the O2 exposure is done in a pulsed fashion. We suggest a multistep cleaning mechanism which results in pure, nanoporous Pt. By suitably chosen beam parameters, high-resolution Pt dot and line structures with dimensions below 10 nm can thus be conveniently obtained. In temperature-dependent resistance measurements, we find the typical metallic behavior of Pt. In low-temperature magnetoresistance measurements, we see clear evidence for weak antilocalization effects and deduce a dephasing length of 234 nm at 1.2 K. We consider this to be a promising starting point for developing this approach into a versatile preparation technique for Pt-based mesoscopic structures, in particular since the purification process can be run in parallel on different deposits. We furthermore anticipate that our results will spur further research on purification approaches for nanostructures prepared by focused electron beam induced deposition containing a catalytically active metal species such as Pd-, Fe-, or Co-based deposits.

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.

The development of simple gas sensing concepts is still of great interest for science and technology. The demands on an ideal device would be a single-step fabrication method providing a device which is sensitive, analyte-selective, quantitative, and reversible without special operating/reformation conditions such as high temperatures or special environments. In this study we demonstrate a new gas sensing concept based on a nanosized PtC metal-matrix system fabricated in a single step via focused electron beam induced deposition (FEBID). The sensors react selectively on polar H2O molecules quantitatively and reversibly without any special reformation conditions after detection events, whereas non-polar species (O2, CO2, N2) produce no response. The key elements are isolated Pt nanograins (2-3 nm) which are embedded in a dielectric carbon matrix. The electrical transport in such materials is based on tunneling effects in the correlated variable range hopping regime, where the dielectric carbon matrix screens the electric field between the particles, which governs the final conductivity. The specific change of these dielectric properties by the physisorption of polar gas molecules (H2O) can change the tunneling probability and thus the overall conductivity, allowing their application as a simple and straightforward sensing concept.

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.

In this work the applicability of neopentasilane (Si(SiH(3))(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.

We present experimental results and theoretical simulations of the adsorption behavior of the metal-organic precursor Co(2)(CO)(8) on SiO(2) 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 SiO(2) 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 SiO(2) 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 SiO(2) surface (untreated surface) and chemisorption on a partially hydroxylated SiO(2) 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.

Binary systems of Pt-Si are prepared by electron-beam-induced deposition using the two precursors, trimethyl(methylcyclopentadienyl)platinum(IV) (MeCpPt(Me)(3)) and neopentasilane (Si(SiH(3))(4)), simultaneously. By varying the relative flux of the two precursors during deposition, we are able to study composites containing platinum and silicon in different ratios by means of energy-dispersive X-ray spectroscopy, atomic force microscopy, electrical transport measurements, and transmission electron microscopy. The results show strong evidence for the formation of a binary, metastable Pt(2)Si(3) phase, leading to a maximum in the conductivity for a Si/Pt ratio of 3:2.

We present temperature-dependent conductivity data obtained on a sample set of nanogranular Pt-C with finely tuned intergrain tunnel coupling strength g. For samples in the strong-coupling regime g > g(C), characterized by a finite conductivity for T→0, we find a logarithmic behavior at elevated temperatures and a crossover to a √T behavior at low temperatures over a wide range of coupling strengths g(C) ≈ 0.25 < g ≤ 3. The experimental observation for g > 1 is in very good agreement with recent theoretical findings on ordered granular metals in three spatial dimensions. The results indicate a validity of the predicted universal conductivity behavior that goes beyond the immediate range of the approach used in the theoretical derivation.

The growth of epitaxial ultrathin BaTiO(3) films on a Pt(100) substrate has been studied by scanning tunneling microscopy (STM), low-energy electron diffraction (LEED), and x-ray photoelectron spectroscopy (XPS). The films have been prepared by radio-frequency-assisted magnetron sputter deposition at room temperature and develop a long-range order upon annealing at 900 K in O(2). By adjusting the Ar and O(2) partial pressures of the sputter gas, the stoichiometry was tuned to match that of a BaTiO(3)(100) single crystal as determined by XPS. STM reveals the growth of continuous BaTiO(3) films with unit cell high islands on top. With LEED already for monolayer thicknesses, the formation of a BaTiO(3)(100)-(1 × 1) structure has been observed. Films of 2-3 unit cell thickness show a brilliant (1 × 1) LEED pattern for which an extended set of LEED I-V data has been acquired. At temperatures above 1050 K the BaTiO(3) thin film starts to decay by formation of vacancy islands. In addition (4 × 4) and (3 × 3) surface reconstructions develop upon prolonged heating., (© 2011 American Institute of Physics)

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.