Metallic Islands Research Articles

Correlation-induced refrigeration with superconducting single-electron transistors

A model of a superconducting tunnel junction which refrigerates a nearby metallic island without any particle exchange is presented. Heat extraction is mediated by charge fluctuations in the coupling capacitance of the two systems. The interplay of the Coulomb interaction and the superconducting gap reduces the power consumption of the refrigerator. The island is predicted to be cooled from lattice temperatures of 200 mK down to close to 50 mK for realistic parameters. The results emphasize the role of non-equilibrium correlations in bipartite mesoscopic conductors. This mechanism can be applied to create local temperature gradients in tunnel junction arrays or explore the role of interactions in the thermalization of non-equilibrium systems.

Nucleation and growth kinetics for intercalated islands during deposition on layered materials with isolated pointlike surface defects

Theory and stochastic lattice-gas modeling is developed for the formation of intercalated metal islands in the gallery between the top layer and the underlying layer at the surface of layered materials. Our model for this process involves deposition of atoms, some fraction of which then enter the gallery through well-separated pointlike defects in the top layer. Subsequently, these atoms diffuse within the subsurface gallery leading to nucleation and growth of intercalated islands nearby the defect point source. For the case of a single point defect, continuum diffusion equation analysis provides insight into the nucleation kinetics. However, complementary tailored lattice-gas modeling produces a more comprehensive and quantitative characterization. We analyze the large spread in nucleation times and positions relative to the defect for the first nucleated island. We also consider the formation of subsequent islands and the evolution of island growth shapes. The shapes reflect in part our natural adoption of a hexagonal close-packed island structure. Motivation and support for the model is provided by scanning tunneling microscopy observations of the formation of intercalated metal islands in highly-ordered pyrolytic graphite at higher temperatures.

Thermal decay of Coulomb blockade oscillations

We study transport properties and the charge quantization phenomenon in a small metallic island connected to the leads through two quantum point contacts (QPCs). The linear conductance is calculated perturbatively with respect to weak tunneling and weak backscattering at QPCs as a function of the temperature $T$ and gate voltage. The conductance shows Coulomb blockade (CB) oscillations as a function of the gate voltage that decay with the temperature as a result of thermally activated fluctuations of the charge in the island. The regimes of quantum, $T \ll E_C$, and thermal, $T \gg E_C$, fluctuations are considered, where $E_C$ is the charging energy of an isolated island. Our predictions for CB oscillations in the quantum regime coincide with previous findings in [A. Furusaki and K. A. Matveev, Phys. Rev. B {\bf 52}, 16676 (1995)]. In the thermal regime the visibility of Coulomb blockade oscillations decays with the temperature as $\sqrt{T/E_C}\exp(-\pi^2T/E_C)$, where the exponential dependence originates from the thermal averaging over the instant charge fluctuations, while the prefactor has a quantum origin. This dependence does not depend on the strength of couplings to the leads. The differential capacitance, calculated in the case of a single tunnel junction, shows the same exponential decay, however the prefactor is linear in the temperature. This difference can be attributed to the non-locality of the quantum effects. Our results agree with the recent experiment [S. Jezouin {\em et al}., Nature {\bf 536}, 58 (2016)] in the whole range of the parameter $T/E_C$.

Sub‐Monolayer Growth of Titanium, Cobalt, and Palladium on Epitaxial Graphene

AbstractWe deposited metals (Ti, Co, Pd) typically used as seed layers for contacts on epitaxial graphene on SiC(0001) and studied the early stages of growth in the sub‐monolayer regime by Scanning Tunneling Microscopy (STM). All three metals do not wet the substrate and Ostwalt ripening occurs at temperatures below 400 K. The analysis of the epitaxial orientation of the metal adislands revealed their specific alignment to the graphene lattice. It is found that the apparent height of the islands as measured by STM strongly deviates from their true topographic height. This is interpreted as an indication of the presence of scattering processes within the metal particles that increase the transparency of the metal‐graphene interface for electrons. Even large islands are easily picked up by the tip of the STM allowing insight into the bonding between metal island and graphene surface and into mechanisms leading to metal intercalation.

Polarization-dependent Total Reflection Fluorescence X-ray Absorption Fine Structure (PTRF-XAFS) Studies on the Structure of a Pt Monolayer on Au(111) Prepared by the Surface-limited Redox Replacement Reaction

We studied the initial stage of a Pt monolayer produced by surface-limited redox replacement (SLRR) using polarization-dependent total reflection fluorescence X-ray absorption fine structure (PTRF-XAFS). Different from the widely accepted understanding that a metallic monolayer island is formed, our XAFS showed that the Pt monolayer, initially present on the Au(111) substrate, was mainly in the form of a planar [PtCl4]2- complex with its molecular plane parallel to the Au(111). This result provides a new insight into the mechanism of SLRR.

Periodic array-based substrates for surface-enhanced infrared spectroscopy

AbstractAt the beginning of the 1980s, the first reports of surface-enhanced infrared spectroscopy (SEIRS) surfaced. Probably due to signal-enhancement factors of only 101to 103, which are modest compared to those of surface-enhanced Raman spectroscopy (SERS), SEIRS did not reach the same significance up to date. However, taking the compared to Raman scattering much larger cross-sections of infrared absorptions and the enhancement factors together, SEIRS reaches about the same sensitivity for molecular species on a surface in terms of the cross-sections as SERS and, due to the complementary nature of both techniques, can valuably augment information gained by SERS. For the first 20 years since its discovery, SEIRS relied completely on metal island films, fabricated by either vapor or electrochemical deposition. The resulting films showed a strong variance concerning their structure, which was essentially random. Therefore, the increase in the corresponding signal-enhancement factors of these structures stagnated in the last years. In the very same years, however, the development of periodic array-based substrates helped SEIRS to gather momentum. This development was supported by technological progress concerning electromagnetic field solvers, which help to understand plasmonic properties and allow targeted design. In addition, the strong progress concerning modern fabrication methods allowed to implement these designs into practice. The aim of this contribution is to critically review the development of these engineered surfaces for SEIRS, to compare the different approaches with regard to their performance where possible, and report further gain of knowledge around and in relation to these structures.

Self-organization of palladium nanoislands on GaN and AlxGa1−xN/GaN heterostructures

We report on systematic study on the dewetting process of thin Pd layer and self-organized Pd nano-islands on SiO2, GaN and AlxGa1−xN/GaN heterostructures with various Al content. The influence of factors such as the thickness of metal layer, type of top layer of AlGaN/GaN heterostructures, temperature and time of annealing process on the dimensions, shapes and density of Pd islands was analyzed. Comparing the behavior of self-organization of Pd islands on Al0.25Ga0.75N/GaN and SiO2 we can conclude that solid-state dewetting process on SiO2 occures much faster than on Al0.25Ga0.75N. For substrates with SiO2 this process requires less energy and can arise for thicker layer. On the Al0.25Ga0.75N surface the islands take more crystalline shape which is probably due to surface reconstruction of Pd-Ga alloy thin layer on interface. For thin metal layer the coalescence of islands into larger islands similar to Ostwald ripening mechanism was observed. Greater surface roughness of AlxGa1−xN/GaN heterostructures with higher Al content causes an increase of surface density of islands and the reduction of their sizes which improves the roundness. In case of GaN and AlxGa1−xN layers with Al content lower than 20%, the surface degradation caused by annealing process was observed. Probably, this is due to the decomposition of layers with gallium droplet formation on catalytic metal islands.

Formation of dysprosium carbide on the graphite (0001) surface

Using scanning tunneling microscopy, we characterize a surface carbide that forms when Dy is deposited on the basal plane of graphite. To form carbide islands on terraces, Dy is first deposited at 650--800 K, which forms large metallic islands. Upon annealing at 1000 K, these clusters convert to carbide. Deposition directly at 1000 K is ineffective because nucleation on terraces is inhibited. Reaction is signaled by the fact that each carbide cluster is partially or totally surrounded by an etch pit. The etch pit is one carbon layer deep for most carbide clusters. Carbide clusters are also identifiable by striations on their surfaces. Based on mass balance, and assuming that only the surface layer of carbon is involved in the reaction, the carbide has stoichiometry $\mathrm{D}{\mathrm{y}}_{2}\mathrm{C}$. This is Dy-rich compared with the most common bulk carbide $\mathrm{Dy}{\mathrm{C}}_{2}$, which may reflect limited surface carbon transport to the carbide.

Fabrication of High-Efficiency CMUTs With Reduced Parasitics Using Embedded Metallic Layers

The transmit and receive sensitivity of the capacitive micromachined ultrasonic transducer (CMUT) is proportional to the active device capacitance formed by the vacuum gap of the device, and an insulation layer between the gap and the device electrode. In the sacrificial release process of CMUT fabrication, this insulation layer cannot be made arbitrarily thin due to conformality issues. In this paper, we propose and prove the applicability of a micromachining technique by which metallic sacrificial islands are embedded inside grooves etched on the substrate, yielding topology free surfaces. This obviates the conformality requirement, and enables the growth of a thinner insulation layer which reduces the effective gap height, and, hence, improves sensitivity. Embedded metalic layers, which provide a flat surface for subsequent process steps, have also been used as the back electrode of the CMUT, which facilitated the manufacturing of devices with reduced stray capacitance on thermally oxidized wafers. CMUT devices were fabricated using the proposed technique, and their parameters were measured to justify the performance improvement. While the dc bias requirement is reduced by 19%, the output sensitivity of the device is 10% higher than that of the conventional CMUT, and spurious capacitance is decreased by 70%.

SPICE Modeling for Metal Island Charged Confined Cellular Automata

SPICE Modeling for Metal Island Charged Confined Cellular Automata

Interaction of cobalt with ceria thin films and its influence on supported Au nanoparticles

The interaction of Co with ceria thin films and its influence on the sintering behavior of Au were investigated by scanning tunneling microscopy (STM), synchrotron radiation photoemission spectroscopy (SRPES) and X-ray photoelectron spectroscopy (XPS). The strong interaction between Co and CeO2(111) leads to oxidation of Co to Co2+ at 300K, accompanied by partial reduction of ceria surface at low Co coverages. Subsequent Co deposition results in an increasing fraction of metallic Co. Annealing to high temperatures induces Co2+ ions diffuse into the CeO2 film, while the small metallic Co islands agglomerate into larger ones. The bimetallic Co–Au particles were prepared by deposition of Au on the existing Co particles on ceria surfaces. The sintering behavior of Co–Au bimetallic surfaces is found to be highly determined by the stoichiometry of ceria supports. The addition of Co to the Au/CeO2 surface suppresses the sintering of Au particles at high temperatures in comparison with that of pure Au particles. However, Au particles are less stable on the Co/CeO1.82 layer than on CeO1.82 surface.

Feedback‐charging a metallic island

AbstractWe consider electronic transport through a single‐electron quantum dot that is tunnel‐coupled to an electronic lead and a metallic island. A background reservoir keeps the metallic island at a thermal state with the ambient temperature, while the charge accumulated on the island is reflected in a time‐dependent chemical potential. Without feedback, a current would flow through the system until the chemical potentials of island and lead are equilibrated. A feedback loop can be implemented by a quantum point contact detecting the dot state, classical processing of the result, and appropriate feedback actions on the electronic tunneling rates taken, with the objective to direct the current in a preferred direction. Since we directly take the detector counting statistics into account, this automatically includes measurement errors in the description. When mainly the rates are modified but hardly any energy is exchanged with the system, this feedback loop effectively implements a Maxwell demon, capable of transporting electrons against an electric bias and thereby charging the metallic island. Once the feedback protocol is stopped, the metallic island simply discharges. We find that a quantitative detector model may be useful for a realistic statistical description of feedback loops.Sketch of the model. The system (S) consists of a single‐electron transistor (SET) dot that can be occupied with at most a single electron. It is tunnel‐coupled to a lead (R) held at a fixed thermal equilibrium state and to a metallic island (L). The metallic island is held at a fixed temperature by an additional background reservoir (bg), with which it can exchange energy but no particles (shaded contact region). Its chemical potential would normally evolve until . A simple feedback loop can be implemented by measuring the state of the system with a quantum point contact (dt), classical signal processing (SP), and using the gate controls (GC) to obtain occupation‐dependent tunneling rates. With feedback active, it is possible to charge the island (). Expressions in brackets (green) denote abbreviations used in the paper.

Conductance Oscillations in a Graphene/Nanocluster Hybrid Material: Toward Large-Area Single-Electron Devices.

Large assemblies of self-organized aluminum nanoclusters embedded in an oxide layer are formed on graphene templates and used to build tunnel-junction devices. Unexpectedly, single-electron-transport behavior with well-defined Coulomb oscillations is observed for a record junction area of up to 100 µm2 containing millions of metal islands. Such graphene-metal nanocluster hybrid materials offer new prospects for single-electron electronics.

Recovery of SINIS turnstile accuracy in a strongly nonequilibrium regime

We perform a theoretical study of nonequilibrium effects in charge transport through a hybrid single-electron transistor based on a small normal metal (N) island with the gate-controlled number of electrons, tunnel-coupled to voltage-biased superconducting (S) electrodes (SINIS). Focusing on the turnstile mode of the transistor operation with the gate voltage driven periodically, and electrons on the island being out of equilibrium, we find that the current quantization accuracy is a nonmonotonic function of the relaxation rate ${\mathrm{\ensuremath{\Gamma}}}_{\mathcal{F}}$ of the distribution function $\mathcal{F}(\ensuremath{\epsilon})$ on the island due to tunneling, as compared to the drive frequency $f$, electron-electron $1/{\ensuremath{\tau}}_{ee}$, and electron-phonon $1/{\ensuremath{\tau}}_{eph}$ relaxation rates. Surprisingly, in the strongly nonequilibrium regime, $f\ensuremath{\gg}{\mathrm{\ensuremath{\Gamma}}}_{\mathcal{F}}\ensuremath{\gg}{\ensuremath{\tau}}_{ee}^{\ensuremath{-}1},{\ensuremath{\tau}}_{eph}^{\ensuremath{-}1}$, the turnstile current plateau is recovered, similarly to the ideal equilibrium regime, ${\ensuremath{\tau}}_{eph}^{\ensuremath{-}1}\ensuremath{\gg}{\mathrm{\ensuremath{\Gamma}}}_{\mathcal{F}}$. The plateau is destroyed in the quasiequilibrium regime when the electron-electron relaxation is faster than tunneling.

Dimensionality and Valency Dependent Quantum Growth of Metallic Nanostructures: A Unified Perspective

Quantum growth refers to the phenomena in which the quantum mechanically confined motion of electrons in metallic wires, islands, and films determines their overall structural stability as well as their physical and chemical properties. Yet to date, there has been a lack of a unified understanding of quantum growth with respect to the dimensionality of the nanostructures as well as the valency of the constituent atoms. Based on a first-principles approach, we investigate the stability of nanowires, nanoislands, and ultrathin films of prototypical metal elements. We reveal that the Friedel oscillations generated at the edges (or surfaces) of the nanostructures cause corresponding oscillatory behaviors in their stability, leading to the existence of highly preferred lengths (or thicknesses). Such magic lengths of the nanowires are further found to depend on both the number of valence electrons and the radial size, with the oscillation period monotonously increasing for alkali and group IB metals, and monotonously decreasing for transition and group IIIA-VA metals. When the radial size of the nanowires increases to reach ∼10 Å, the systems equivalently become nanosize islands, and the oscillation period saturates to that of the corresponding ultrathin films. These findings offer a generic perspective of quantum growth of different classes of metallic nanostructures.

Emergent nanoscale superparamagnetism at oxide interfaces.

Atomically sharp oxide heterostructures exhibit a range of novel physical phenomena that are absent in the parent compounds. A prominent example is the appearance of highly conducting and superconducting states at the interface between LaAlO3 and SrTiO3. Here we report an emergent phenomenon at the LaMnO3/SrTiO3 interface where an antiferromagnetic Mott insulator abruptly transforms into a nanoscale inhomogeneous magnetic state. Upon increasing the thickness of LaMnO3, our scanning nanoSQUID-on-tip microscopy shows spontaneous formation of isolated magnetic nanoislands, which display thermally activated moment reversals in response to an in-plane magnetic field. The observed superparamagnetic state manifests the emergence of thermodynamic electronic phase separation in which metallic ferromagnetic islands nucleate in an insulating antiferromagnetic matrix. We derive a model that captures the sharp onset and the thickness dependence of the magnetization. Our model suggests that a nearby superparamagnetic–ferromagnetic transition can be gate tuned, holding potential for applications in magnetic storage and spintronics.

Controlling charge quantization with quantum fluctuations

In 1909, Millikan showed that the charge of electrically isolated systems is quantized in units of the elementary electron charge e. Today, the persistence of charge quantization in small, weakly connected conductors allows for circuits in which single electrons are manipulated, with applications in, for example, metrology, detectors and thermometry. However, as the connection strength is increased, the discreteness of charge is progressively reduced by quantum fluctuations. Here we report the full quantum control and characterization of charge quantization. By using semiconductor-based tunable elemental conduction channels to connect a micrometre-scale metallic island to a circuit, we explore the complete evolution of charge quantization while scanning the entire range of connection strengths, from a very weak (tunnel) to a perfect (ballistic) contact. We observe, when approaching the ballistic limit, that charge quantization is destroyed by quantum fluctuations, and scales as the square root of the residual probability for an electron to be reflected across the quantum channel; this scaling also applies beyond the different regimes of connection strength currently accessible to theory. At increased temperatures, the thermal fluctuations result in an exponential suppression of charge quantization and in a universal square-root scaling, valid for all connection strengths, in agreement with expectations. Besides being pertinent for the improvement of single-electron circuits and their applications, and for the metal-semiconductor hybrids relevant to topological quantum computing, knowledge of the quantum laws of electricity will be essential for the quantum engineering of future nanoelectronic devices.

Quantum physics: Destruction of discrete charge.

Electric charge is quantized in units of the electron's charge. An experiment explores the suppression of charge quantization caused by quantum fluctuations and supports a long-standing theory that explains this behaviour. See Letter p.58 The charge of a single electron or proton defines the fundamental unit of electric charge. But in nanoelectronic devices, where quantum fluctuations are in play, the discreteness of this elementary charge is eroded with increasing connection strengths between conducting elements. Fundamental predictions have been difficult to verify, but now Frederic Pierre and colleagues have constructed a device, consisting of a micrometre-scale metallic island connected to electrodes via fully controllable semiconducting channels, where the complete evolution of charge quantization can be measured. The work confirms long-standing theory and opens up a platform for testing charge quantization in challenging scenarios involving correlated electrons and topological quasiparticles.

Plasmonic properties of metal nanoislands: surface integral equations approach

The surface integral equations method is used to analyse the surface plasmon resonance position in a metal island film formed by non-interacting axisymmetrical prolate/oblate hemispheroids placed on a dielectric substrate. The approach is verified via the comparison of results obtained for a hemisphere on a substrate with the ones obtained using the multipole expansion method. The preference of the integral equations method is in obtaining a simple final analytical expression for a particle polarizability in which any dielectric function of a metal can be substituted. Such simple formulae for the hemispherical particle on the substrate and calculated dependences of the hemispheroid resonant wavelength on its aspect ratio are presented.

Linear hydrogen gas sensors based on bimetallic nanoclusters

This work reports on the fabrication of hydrogen gas sensors based on bimetallic palladium-copper nanoclusters. The nanoclusters were generated by sputtering and inert-gas condensation inside an ultra-high vacuum (UHV) compatible system, and self-assembled on an insulating substrate with a pair of pre-formed interdigitated gold/nichrome electrodes. Nanocluster deposition was stopped once their coverage on the substrate reached the percolation threshold. Electrical properties of the fabricated sensors were investigated by means of electrical conductance measurements, and assigned to charge carrier transport within network of metallic islands that is dominated by tunnelling. The produced devices were utilized as conductometric gas sensors. Herein, a constant voltage was applied across the interdigitated electrodes, and the change in electrical current signal was measured which reflects gas concentration. All fabricated sensors showed increase in the conductance upon exposure to hydrogen which can be assigned to the increase in tunnelling current due to the decrease in the size of the gaps between the nanoclusters or the establishment of conducting paths through the network of percolating nanocluster film. The sensors were found to be sensitive at low concentrations of hydrogen at room temperature, and exhibit a linear relationship between hydrogen concentration and the sensitivity. Therefore, those sensors have the potential to be used for practical life applications.