3D Nanolithography by Means of Lipid Ink Spreading Inhibition.

While patterning 2D metallic nanostructures are well established through different techniques, 3D printing still constitutes a major bottleneck on the way to device miniaturization. In this work a fluid phase phospholipid ink is used as a building block for structuring with dip-pen nanolithography. Following a bioinspired approach that relies on ink-spreading inhibition, two processes are presented to build 2D and 3D metallic structures. Serum albumin, a widely used protein with an innate capability to bind to lipids, is the key in both processes. Covering the sample surface with it prior to lipid writing, anchors lipids on the substrate, which ultimately allows the creation of highly stable 3D lipid-based scaffolds to build metallic structures.

Integration of Biofunctional Molecules into 3D-Printed Polymeric Micro-/Nanostructures.

Three-dimensional printing at the micro-/nanoscale represents a new challenge in research and development to achieve direct printing down to nanometre-sized objects. Here, FluidFM, a combination of microfluidics with atomic force microscopy, offers attractive options to fabricate hierarchical polymer structures at different scales. However, little is known about the effect of the substrate on the printed structures and the integration of (bio)functional groups into the polymer inks. In this study, we printed micro-/nanostructures on surfaces with different wetting properties, and integrated molecules with different functional groups (rhodamine as a fluorescent label and biotin as a binding tag for proteins) into the base polymer ink. The substrate wetting properties strongly affected the printing results, in that the lateral feature sizes increased with increasing substrate hydrophilicity. Overall, ink modification only caused minor changes in the stiffness of the printed structures. This shows the generality of the approach, as significant changes in the mechanical properties on chemical functionalization could be confounders in bioapplications. The retained functionality of the obtained structures after UV curing was demonstrated by selective binding of streptavidin to the printed structures. The ability to incorporate binding tags to achieve specific interactions between relevant proteins and the fabricated micro-/nanostructures, without compromising the mechanical properties, paves a way for numerous bio and sensing applications. Additional flexibility is obtained by tuning the substrate properties for feature size control, and the option to obtain functionalized printed structures without post-processing procedures will contribute to the development of 3D printing for biological applications, using FluidFM and similar dispensing techniques.

3D quasi-skyrmions in thick cylindrical and dome-shape soft nanodots.

Magnetic skyrmions are widely attracting researchers due to fascinating physics and novel applications related to their non-trivial topology. Néel skyrmions have been extensively investigated in magnetic systems with Dzyaloshinskii-Moriya interaction (DMI) and/or perpendicular magnetic anisotropy. Here, by means of micromagnetic simulations and analytical calculations, we show that 3D quasi-skyrmions of Néel type, with topological charge close to 1, can exist as metastable states in soft magnetic nanostructures with no DMI, such as in Permalloy thick cylindrical and dome-shaped nanodots. The key factor responsible for the stabilization of DMI-free is the interplay of the exchange and magnetostatic energies in the nanodots. The range of geometrical parameters where the skyrmions are found is wider in magnetic dome-shape nanodots than in their cylindrical counterparts. Our results open the door for a new research line related to the nucleation and stabilization of magnetic skyrmions in a broad class of nanostructured soft magnetic materials.

Direct-Write Patterning of Biomimetic Lipid Membranes In Situ with FluidFM.

The creation of biologically inspired artificial membranes on substrates with custom size and in close proximity to each other not only provides a platform to study biological processes in a simplified manner, but they also constitute building blocks for chemical or biological sensors integrated in microfluidic devices. Scanning probe lithography tools such as dip-pen nanolithography (DPN) have opened a new paradigm in this regard, although they possess some inherent drawbacks like the need to operate in air environment or the limited choice of lipids that can be patterned. In this work, we propose the use of the fluid force microscopy (FluidFM) technology to fabricate biomimetic membranes without losing the multiplexing capability of DPN but gaining flexibility in lipid inks and patterning environment. We shed light on the driving mechanisms of the FluidFM-mediated lithography processes in air and liquid. The obtained results should prompt the creation of more realistic biomimetic membranes with arbitrary complex phospholipid mixtures, cholesterol, and potential functional membrane proteins directly patterned in physiological environment.

A multiplexed phospholipid membrane platform for curvature sensitive protein screening.

The curvature of lipid membranes plays a key role in many relevant biological processes such as membrane trafficking, vesicular budding and host-virus interactions. In vitro studies on the membrane curvature of simplified biomimetic models in the nanometer range are challenging, due to their complicated nanofabrication processes. In this work, we propose a simple and low-cost platform for curvature sensitive protein screening, prepared through scanning probe lithography (SPL) methods, where lipid bilayer patches of different compositions can be multiplexed onto substrate areas with tailored local curvature. The curvature is imposed by anchoring nanoparticles of the desired size to the substrate prior to lithography. As a proof of principle, we demonstrate that a positive curvature membrane sensitive protein derived from the BAR domain of Nadrin2 binds selectively to lipid patches patterned on substrate areas coated with 100 nm nanoparticles. The platform opens up a path for screening curvature-dependent protein-membrane interaction studies by providing a flexible and easy to prepare substrate with control over lipid composition and membrane curvature.

Half-hedgehog spin textures in sub-100 nm soft magnetic nanodots.

Topologically non-trivial structures such as magnetic skyrmions are nanometric spin textures of outstanding potential for spintronic applications due to their unique features. It is well known that Néel skyrmions of definite chirality are stabilized by the Dzyaloshinskii-Moriya exchange interaction (DMI) in bulk non-centrosymmetric materials or ultrathin films with strong spin-orbit coupling at the interface. In this work, we show that soft magnetic (permalloy) hemispherical nanodots are able to host three-dimensional chiral structures (half-hedgehog spin textures) with non-zero tropological charge. They are observed at room temperature, in absence of DMI interaction and they can be further stabilized by the magnetic field arising from the Magnetic Force Microscopy probe. Micromagnetic simulations corroborate the experimental data. Our work implies the existence of a new degree of freedom to create and manipulate complex 3D spin-textures in soft magnetic nanodots and opens up future possibilities to explore their magnetization dynamics.

Customized MFM probes based on magnetic nanorods.

Focused Electron Beam Induced Deposition (FEBID) for magnetic tip fabrication is presented in this work as an alternative to conventional sputtering-based Magnetic Force Microscopy (MFM) tips. FEBID enables the growth of a high-aspect-ratio magnetic nanorod with customized geometry and composition to overcome the key technical limitations of MFM probes currently on the market. The biggest advantage of these tips, in comparison with CoCr coated pyramidal probes, lies in the capability of creating sharp ends, nearly 10 nm in diameter, which provides remarkable (topographic and magnetic) lateral resolution in samples with magnetic features close to the resolution limits of the MFM technique itself. The shape of the nanorods produces a very confined magnetic stray field, whose interaction with the sample is extremely localized and perpendicular to the surface, with negligible in-plane components. This effect can lead to a better analytical and numerical modelling of the MFM probes and to an increase in the sensitivity without perturbing the magnetic configuration of soft samples. Besides, the high-aspect ratio achievable in FEBID nanorod tips makes them magnetically harder than the commercial ones, reaching coercive fields higher than 900 Oe. According to the results shown, tips based on magnetic nanorods grown by FEBID can be eventually used for quantitative analysis in MFM measurements. Moreover, the customized growth of Co- or Fe-based tips onto levers with different mechanical properties allows MFM studies that demand different measuring conditions. To showcase the versatility of this type of probe, as a last step, MFM is performed in a liquid environment, which still remains a challenge for the MFM community largely due to the lack of appropriate probes on the market. This opens up new possibilities in the investigation of magnetic biological samples.

Magnetization Ratchet in Cylindrical Nanowires.

The unidirectional motion of information carriers such as domain walls in magnetic nanostrips is a key feature for many future spintronic applications based on shift registers. This magnetic ratchet effect has so far been achieved in a limited number of complex nanomagnetic structures, for example, by lithographically engineered pinning sites. Here we report on a simple remagnetization ratchet originated in the asymmetric potential from the designed increasing lengths of magnetostatically coupled ferromagnetic segments in FeCo/Cu cylindrical nanowires. The magnetization reversal in neighboring segments propagates sequentially in steps starting from the shorter segments, irrespective of the applied field direction. This natural and efficient ratchet offers alternatives for the design of three-dimensional advanced storage and logic devices.

Quantitative Nanoscale Magnetic Study of Isolated Diameter-Modulated FeCoCu Nanowires.

The comprehension of the magnetic configuration in FeCoCu nanowires with a diameter-modulated cylindrical geometry will allow controlling the domain wall motion in this low-dimensional system under the application of magnetic fields and/or the injection of current pulses. Here we perform a quantitative magnetic characterization of isolated diameter-modulated FeCoCu nanowires by combining nanoscale magnetic characterization techniques such as electron holography, magnetic force microscopy, and micromagnetic simulations. Local reconstructions of the magnetic distribution show the diameter-modulated geometry of the wires induces the formation of vortex-like structures and magnetic charges in the regions where the diameter is varied. Vortex-like structures modify the axial alignment of the magnetization in large-diameter segments. Moreover, the magnetic charges control the demagnetizing field distribution, promoting a flux-closure stray field configuration around large-diameter segments and keeping the demagnetizing field parallel to the NW's magnetization around small diameter segments. The detailed description of the remanent state in diameter-modulated cylindrical FeCoCu nanowires allows us to provide a clear explanation of the origin of bright and dark contrast observed in magnetic force microscopy images, which have the same feature of magnetic domain walls. This work establishes the primary knowledge required for future magnetization reversal studies with the aim of searching efficient modulated geometries that allow an optimum and controlled domain wall propagation.

Customized MFM probes with high lateral resolution.

Magnetic force microscopy (MFM) is a widely used technique for magnetic imaging. Besides its advantages such as the high spatial resolution and the easy use in the characterization of relevant applied materials, the main handicaps of the technique are the lack of control over the tip stray field and poor lateral resolution when working under standard conditions. In this work, we present a convenient route to prepare high-performance MFM probes with sub-10 nm (sub-25 nm) topographic (magnetic) lateral resolution by following an easy and quick low-cost approach. This allows one to not only customize the tip stray field, avoiding tip-induced changes in the sample magnetization, but also to optimize MFM imaging in vacuum (or liquid media) by choosing tips mounted on hard (or soft) cantilevers, a technology that is currently not available on the market.

Domain wall pinning in FeCoCu bamboo-like nanowires.

The three dimensional nature of cylindrical magnetic nanowires has opened a new way to control the domain configuration as well as the magnetization reversal process. The pinning effect of the periodic diameter modulations on the domain wall propagation in FeCoCu individual nanowires is determined by Magnetic Force Microscopy, MFM. A main bistable magnetic configuration is firstly concluded from MFM images characterized by the spin reversal between two nearly single domain states with opposite axial magnetization. Complementary micromagnetic simulations confirm a vortex mediated magnetization reversal process. A non-standard variable field MFM imaging procedure allows us to observe metastable magnetic states where the propagating domain wall is pinned at certain positions with enlarged diameter. Moreover, it is demonstrated that it is possible to control the position of the pinned domain walls by an external magnetic field.

Spin configuration in isolated FeCoCu nanowires modulated in diameter.

Cylindrical Fe28Co67Cu5 nanowires modulated in diameter between 22 and 35 nm are synthesized by electroplating into the nanopores of alumina membranes. High-sensitivity MFM imaging (with a detection noise of 1 µN m(-1)) reveals the presence of single-domain structures in remanence with strong contrast at the ends of the nanowires, as well as at the transition regions where the diameter is modulated. Micromagnetic simulations suggest that curling of the magnetization takes place at these transition sites, extending over 10-20 nm and giving rise to stray fields measurable with our MFM. An additional weaker contrast is imaged, which is interpreted to arise from inhomogeneities in the nanowire diameter.