Influence of the Emitter Shape on the Field-of-View in Atom Probe Tomography.

Atom probe tomography (APT) is a unique analytical technique that offers three-dimensional elemental mapping with a spatial resolution down to the sub-nanometer. When APT is applied on complex heterogenous systems and/or under certain experimental conditions, that is, laser illumination, the specimen shape can deviate from an ideal hemisphere. Insufficient consideration of this aspect can introduce artifacts in the reconstructed dataset, ultimately degrading its spatial accuracy. So far, there has been limited investigation into the detailed evolution of emitter shape and its impact on the field-of-view (FOV). In this study, we numerically and experimentally investigated the FOV for asymmetric emitters and its evolution throughout the analysis depth. Our analysis revealed that, for asymmetric emitters, the ions evaporated from the topmost region of the specimen (summit) project approximately to the detector center. Furthermore, we demonstrated the implications of this finding on the FOV location for asymmetric emitters. Based on our findings, the location of the center of the FOV can deviate from the specimen central axis with an evolution depending on the evolution of the emitter shape. This study highlights the importance of accounting for the specimen shape when developing advanced data reconstruction schemes to enhance spatial resolution and accuracy.

A platinum-nickel bimetallic nanocluster ensemble-on-polyaniline nanofilm for enhanced electrocatalytic oxidation of dopamine.

We report a new approach to design flexible functional material platforms based on electropolymerized polyaniline (PANI) polymer nanofilms modified with bimetallic nanoclusters (NCs) for efficient electro-oxidation of small organic molecules. Composition defined ligand free Pt0.75Ni0.25 NCs were synthesized in the gas phase using the Cluster Beam Deposition (CBD) technology and characterized using RToF, HAADF-STEM, XAFS and XPS. NCs were then directly deposited on PANI coated templates to construct electrodes. Dopamine (DP) molecules were used as a representative organic analyte and the influence of the NC-PANI hybrid atomistic structure on the electrochemical and electrocatalytic performance was investigated. The as prepared, nearly monodispersed, Pt0.75Ni0.25 NCs of ca. 2 nm diameter featuring a PtOx surface combined with a shallow platelet-like Ni-O(OH) phase formed a densely packed active surface on PANI at ultralow metal coverages. Electrochemical measurements (EIS and CV) show a 2.5 times decrease in charge transfer resistance and a remarkable 6-fold increase at lower potential in the mass activity for Pt0.75Ni0.25 NCs in comparison with their pure Pt counterparts. The enhanced electrochemical performance of the Pt0.75Ni0.25 NC hybrid's interface is ascribed to the formation of mixed Pt metal and Ni-O(OH) phases at the surface of the alloyed PtNi cores of the bimetallic NCs under electrochemical conditions combined with an efficient charge conduction pathway between NCs.

Room temperature single electron transistor based on a size-selected aluminium cluster.

Single electron transistors (SETs) are powerful devices to study the properties of nanoscale objects. However, the capabilities of placing a nano-object between electrical contacts under pristine conditions are lacking. Here, we developed a versatile two point contacting approach that tackles this challenge, which is demonstrated by constructing in situ a prototypical SET device consisting of a single aluminium cluster of 66 ± 5 atoms, deposited directly in a gold nanogap using an innovative cluster beam deposition technique. The gate driven conductance measurements demonstrate Coulomb blockade oscillations at room temperature correlating with an extracted charging energy of 0.14 eV, which is five times larger than kBT at 300 K. Our work provides a model SET device platform to probe the quantum features of nano-objects with high precision.

Nano-SQUIDs with controllable weak links created via current-induced atom migration.

As the most sensitive magnetic field sensor, the superconducting quantum interference device (SQUID) became an essential component in many applications due to its unmatched performance. Through recently achieved miniaturization, using state-of-the-art fabrication methods, this fascinating device extended its functionality and became an important tool in nanomaterial characterization. Here, we present an accessible and yet powerful technique of targeted atom displacement in order to reduce the size of the weak links of a DC nano-SQUID beyond the limits of conventional lithography. The controllability of our protocol allows us to characterize in situ the full superconducting response after each electromigration step. From this in-depth analysis, we reveal an asymmetric evolution of the weak links at cryogenic temperatures. A comparison with time resolved scanning electron microscopy images of the atom migration process at room temperature confirms the peculiar asymmetric evolution of the parallel constrictions. Moreover, we observe that when electromigration has sufficiently reduced the junction's cross section, superconducting phase coherence is attained in the dissipative state, where magnetic flux readout from voltage becomes possible.

Controlled electromigration protocol revised.

Electromigration has evolved from an important cause of failure in electronic devices to an appealing method, capable of modifying the material properties and geometry of nanodevices. Although this technique has been successfully used by researchers to investigate low dimensional systems and nanoscale objects, its low controllability remains a serious limitation. This is in part due to the inherent stochastic nature of the process, but also due to the inappropriate identification of the relevant control parameters. In this study, we identify a suitable process variable and propose a novel control algorithm that enhances the controllability and, at the same time, minimizes the intervention of an operator. As a consequence, the algorithm facilitates the application of electromigration to systems that require exceptional control of, for example, the width of a narrow junction. It is demonstrated that the electromigration rate can be stabilized on pre-set values, which eventually defines the final geometry of the electromigrated structures.

Electrically Driven Unidirectional Optical Nanoantennas.

Directional antennas revolutionized modern day telecommunication by enabling precise beaming of radio and microwave signals with minimal loss of energy. Similarly, directional optical nanoantennas are expected to pave the way toward on-chip wireless communication and information processing. Currently, on-chip integration of such antennas is hampered by their multielement design or the requirement of complicated excitation schemes. Here, we experimentally demonstrate electrical driving of in-plane tunneling nanoantennas to achieve broadband unidirectional emission of light. Far-field interference, as a result of the spectral overlap between the dipolar emission of the tunnel junction and the fundamental quadrupole-like resonance of the nanoantenna, gives rise to a directional radiation pattern. By tuning this overlap using the applied voltage, we record directivities as high as 5 dB. In addition to electrical tunability, we also demonstrate passive tunability of the directivity using the antenna geometry. These fully configurable electrically driven nanoantennas provide a simple way to direct optical energy on-chip using an extremely small device footprint.

Decorating graphene with size-selected few-atom clusters: a novel approach to investigate graphene-adparticle interactions.

We investigated the interaction between size-selected Au2 and Au3 clusters and graphene. Hereto preformed clusters are deposited on graphene field-effect transistors, a novel approach which offers a high control over the number of atoms per cluster, the deposition energy and the deposited density. The induced p-doping and charge carrier scattering indicate that a major part of the deposited clusters remains on the graphene flake as either individual or sub-nm coalesced entities. This is independently confirmed by scanning electron microscopy on the same devices after current annealing. Our novel approach provides perspectives for the electronic sensing of metallic clusters down to their atom-by-atom size-specific properties, and exploiting the tunability of clusters for tailoring desired properties in graphene.

Healing Effect of Controlled Anti-Electromigration on Conventional and High-Tc Superconducting Nanowires.

The electromigration process has the potential capability to move atoms one by one when properly controlled. It is therefore an appealing tool to tune the cross section of monoatomic compounds with ultimate resolution or, in the case of polyatomic compounds, to change the stoichiometry with the same atomic precision. As demonstrated here, a combination of electromigration and anti-electromigration can be used to reversibly displace atoms with a high degree of control. This enables a fine adjustment of the superconducting properties of Al weak links, whereas in Nb the diffusion of atoms leads to a more irreversible process. In a superconductor with a complex unit cell (La2-x Cex CuO4 ), the electromigration process acts selectively on the oxygen atoms with no apparent modification of the structure. This allows to adjust the doping of this compound and switch from a superconducting to an insulating state in a nearly reversible fashion. In addition, the conditions needed to replace feedback controlled electromigration by a simpler technique of electropulsing are discussed. These findings have a direct practical application as a method to explore the dependence of the characteristic parameters on the exact oxygen content and pave the way for a reversible control of local properties of nanowires.

Statistics of localized phase slips in tunable width planar point contacts.

The main dissipation mechanism in superconducting nanowires arises from phase slips. Thus far, most of the studies focus on long nanowires where coexisting events appear randomly along the nanowire. In the present work we investigate highly confined phase slips at the contact point of two superconducting leads. Profiting from the high current crowding at this spot, we are able to shrink in-situ the nanoconstriction. This procedure allows us to investigate, in the very same sample, thermally activated phase slips and the probability density function of the switching current Isw needed to trigger an avalanche of events. Furthermore, for an applied current larger than Isw, we unveil the existence of two distinct thermal regimes. One corresponding to efficient heat removal where the constriction and bath temperatures remain close to each other, and another one in which the constriction temperature can be substantially larger than the bath temperature leading to the formation of a hot spot. Considering that the switching current distribution depends on the exact thermal properties of the sample, the identification of different thermal regimes is of utmost importance for properly interpreting the dissipation mechanisms in narrow point contacts.

Thermal and quantum depletion of superconductivity in narrow junctions created by controlled electromigration.

Superconducting nanowires currently attract great interest due to their application in single-photon detectors and quantum-computing circuits. In this context, it is of fundamental importance to understand the detrimental fluctuations of the superconducting order parameter as the wire width shrinks. In this paper, we use controlled electromigration to narrow down aluminium nanoconstrictions. We demonstrate that a transition from thermally assisted phase slips to quantum phase slips takes place when the cross section becomes less than ∼150 nm(2). In the regime dominated by quantum phase slips the nanowire loses its capacity to carry current without dissipation, even at the lowest possible temperature. We also show that the constrictions exhibit a negative magnetoresistance at low-magnetic fields, which can be attributed to the suppression of superconductivity in the contact leads. These findings reveal perspectives of the proposed fabrication method for exploring various fascinating superconducting phenomena in atomic-size contacts.