arXiv subjects

Stefan Heun

Publications and source records attributed to Stefan Heun.

At least 37 records · Page 2Linked to original sources

arXiv2024

Anomalous supercurrent and diode effect in locally perturbed topological Josephson junctions

The simultaneous breaking of time-reversal and inversion symmetry can lead to peculiar effects in Josephson junctions, such as the anomalous Josephson effect or supercurrent rectification, which is a dissipationless analog of the diode effect. Due to their impact in new quantum technologies, it is important to find robust platforms and external means to manipulate the above effects in a controlled way. Here, we theoretically consider a Josephson junction based on a quantum spin Hall system as the normal channel, subjected to a magnetic field in the direction defined by spin-momentum locking, and in presence of a local tip in close proximity to one of the metallic edges in the normal region. We consider different local perturbations, model normal and magnetic tips, and study how they affect the Josephson response of the device. In particular, we argue that magnetic tips are a useful tool that allows for tunability of both $ϕ_0$ response and supercurrent rectification.

cond-mat.supr-con↗

arXiv2023

Metal Nanoparticle-Functionalized Three-Dimensional Graphene: a versatile platform towards sensors and energy-related applications

We demonstrate the first successful functionalization of epitaxial three-dimensional graphene with metal nanoparticles. The functionalization is obtained by immersing the 3D graphene in a nanoparticle colloidal solution. This method is versatile and here is demonstrated for gold and palladium, but can be extended to other types and shapes of nanoparticles. We have measured the nanoparticle density on the top-surface and in the porous layer volume by Scanning Electron Microscopy and Scanning Transmission Electron Microscopy. Samples exhibit a high coverage of nanoparticles with minimal clustering. High quality graphene has been demonstrated to promote the functionalization leading to higher nanoparticle density, both on the surface and in the pores. X-ray Photoelectron Spectroscopy allowed to verify the absence of contamination after the functionalization process. Moreover, it confirmed the thermal stability of the Au- and Pd-functionalized three-dimensional graphene up to 530°C. Our approach opens up new avenues for utilizing three-dimensional graphene as a versatile platform for catalytic applications, sensors, and energy storage and conversion.

physics.app-ph↗

arXiv2023

Platinum-Decorated Graphene: Experimental Insight into Growth Mechanisms and Hydrogen Adsorption Properties

The potential of graphene for hydrogen storage, coupled with the established role of Platinum as a catalyst for the hydrogen evolution reaction and the spillover effect, makes Pt-functionalized graphene a promising candidate for near-ambient hydrogen storage. This paper focuses on examining the process of Pt cluster formation on epitaxial graphene and assesses the suitability of the system as hydrogen storage material. Scanning tunneling microscopy unveils two primary pathways for Pt cluster growth. In the initial phase, up to ~1 ML of Pt coverage, Pt tends to randomly disperse and cover the graphene surface, while the cluster height remains essentially unchanged. Beyond a coverage of 3 ML, the nucleation of new layers on existing clusters becomes predominant. Then, the clusters mainly grow in height. Thermal desorption spectroscopy on hydrogenated Pt-decorated graphene reveals the presence of multiple hydrogen adsorption mechanisms, manifested as two Gaussian peaks superimposed on a linearly increasing background. We attribute the first peak at 150°C to hydrogen physisorbed on the surface of Pt clusters. The second peak at 430°C is attributed to chemisorption of hydrogen on the surface of the clusters, while the linearly increasing background is assigned to hydrogen bonded in the bulk of the Pt clusters. These measurements demonstrate the ability of Pt-functionalized graphene to store molecular hydrogen at temperatures that are high enough for stable hydrogen binding at room temperature.

cond-mat.mtrl-sci↗

arXiv2023

Three-dimensional graphene on a nano-porous 4H-SiC backbone: a novel material for food sensing applications

Sensors which are sensitive to volatile organic compounds and thus able to monitor the conservation state of food, are precious because they work non-destructively and allow to avoid direct contact with the food, ensuring hygienic conditions. In particular, the monitoring of rancidity would solve a widespread issue in food storage. The sensor discussed here is produced utilizing a novel three-dimensional arrangement of graphene, which is grown on a crystalline silicon carbide (SiC) wafer previously porousified by chemical etching. This approach allows a very high surface-to.volume ratio. Furthermore, the structure of the sensor surface features a large amount of edges, dangling bounds, and active sites, which make the sensor, on a chemically robust skeleton, chemically active, particularly to hydrogenated molecules. The interaction of the sensor with such compounds is read out by measuring the sensor resistance in a four wire configuration. The sensor performance has been assessed on three hazelnut samples: sound hazelnuts, spoiled hazelnuts, and stink bug hazelnuts. A resistance variation of about DeltaR = 0.13 (0.02) Ohm between sound and damaged hazelnuts has been detected. Our measurements confirm the ability of the sensor to discriminate between sound and damaged hazelnuts. The sensor signal is stable for days, providing the possibility to use this sensor for the monitoring of the storage state of fats and foods in general.

physics.app-ph↗

arXiv2023

Half-integer Shapiro steps in highly transmissive InSb nanoflag Josephson junctions

We investigate a ballistic InSb nanoflag-based Josephson junction with Nb superconducting contacts. The high transparency of the superconductor-semiconductor interfaces enables the exploration of quantum transport with parallel short and long conducting channels. Under microwave irradiation, we observe half-integer Shapiro steps that are robust to temperature, suggesting their possible non-equilibrium origin. Our results demonstrate the potential of ballistic InSb nanoflags Josephson junctions as a valuable platform for understanding the physics of hybrid devices and investigating their non-equilibrium dynamics.

cond-mat.supr-con↗

arXiv2023

Study of hydrogen absorption in a novel three-dimensional graphene structure: Towards hydrogen storage applications

The use of a novel three-dimensional graphene structure allows circumventing the limitations of the two-dimensional nature of graphene and its application in hydrogen absorption. Here we investigate hydrogen-bonding on monolayer graphene conformally grown via the epitaxial growth method on the (0001) face of a porousified 4H-SiC wafer. Hydrogen absorption is studied via Thermal Desorption Spectroscopy (TDS), exposing the samples to either atomic (D) or molecular (D2) deuterium. The graphene growth temperature, hydrogen exposure temperature, and the morphology of the structure are investigated and related to their effect on hydrogen absorption. The three-dimensional graphene structures chemically bind atomic deuterium when exposed to D2. This is the first report of such an event in unfunctionalized graphene-based materials and implies the presence of a catalytic splitting mechanism. It is further shown that the three-dimensional dendritic structure of the porous material temporarily retains the desorbed molecules and causes delayed emission. The capability of chemisorbing atoms after a catalytic splitting of hydrogen, coupled to its large surface-to-volume ratio, make these structures a promising substrate for hydrogen storage devices.

cond-mat.mtrl-sci↗

arXiv2022

Josephson Diode Effect in High Mobility InSb Nanoflags

We report evidence of non-reciprocal dissipation-less transport in single ballistic InSb nanoflag Josephson junctions, owing to a strong spin-orbit coupling. Applying an in-plane magnetic field, we observe an inequality in supercurrent for the two opposite current propagation directions. This demonstrates that these devices can work as Josephson diodes, with dissipation-less current flowing in only one direction. For small fields, the supercurrent asymmetry increases linearly with the external field, then it saturates as the Zeeman energy becomes relevant, before it finally decreases to zero at higher fields. We show that the effect is maximum when the in-plane field is perpendicular to the current vector, which identifies Rashba spin-orbit coupling as the main symmetry-breaking mechanism. While a variation in carrier concentration in these high-quality InSb nanoflags does not significantly influence the diode effect, it is instead strongly suppressed by an increase in temperature. Our experimental findings are consistent with a model for ballistic short junctions and show that the diode effect is intrinsic to this material. Our results establish InSb Josephson diodes as a useful element in superconducting electronics.

cond-mat.supr-con↗

arXiv2022

Hydrogen spillover and storage on graphene with single-site Ti catalysts

Hydrogen spillover and storage for single-site metal catalysts, including single-atom catalysts (SACs) and single nanocluster catalysts, have been elucidated for various supports but remain poorly understood for inert carbon supports. Here, we use synchrotron radiation-based methods to investigate the role of single-site Ti catalysts on graphene for hydrogen spillover and storage. Our in-situ angle-resolved photoemission spectra results demonstrate a bandgap opening and the X-ray absorption spectra reveal the formation of C-H bonds, both indicating the partial graphene hydrogenation. With increasing Ti deposition and H2 exposure, the Ti atoms tend to aggregate to form nanocluster catalysts and yield 13.5% sp3-hybridized carbon atoms corresponding to a hydrogen-storage capacity of 1.11 wt% (excluding the weight of the Ti nanoclusters [1]). Our results demonstrate how a simple spillover process at Ti SACs can lead to covalent hydrogen bonding on graphene, thereby providing a strategy for a rational design of carbon-supported single-site catalysts.

cond-mat.mtrl-sci↗

arXiv2022

Deterministic Covalent Organic Functionalization of Monolayer Graphene with 1,3-Dipolar Cycloaddition Via High Resolution Surface Engineering

Spatially-resolved organic functionalization of monolayer graphene is successfully achieved by combining low-energy electron beam irradiation with 1,3-dipolar cycloaddition of azomethine ylide. Indeed, the modification of the graphene honeycomb lattice obtained via electron beam irradiation yields to a local increase of the graphene chemical reactivity. As a consequence, thanks to the high-spatially resolved generation of structural defects (~ 100 nm), chemical reactivity patterning has been designed over the graphene surface in a well-controlled way. Atomic force microscopy and Raman spectroscopy allow to investigate the two-dimensional spatial distribution of the structural defects and the new features that arise from the 1,3-dipolar cycloaddition, confirming the spatial selectivity of the graphene functionalization achieved via defect engineering. The Raman signature of the functionalized graphene is investigated both experimentally and via ab initio molecular dynamics simulations, computing the power spectrum. Furthermore, the organic functionalization is shown to be reversible thanks to the desorption of the azomethine ylide induced by focused laser irradiation. The selective and reversible functionalization of high quality graphene using 1,3-dipolar cycloaddition is a significant step towards the controlled synthesis of graphene-based complex structures and devices at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2022

Morphology and Electronic Properties of Incipient Soot by Scanning Tunneling Microscopy and Spectroscopy

Soot nucleation is one of the most complex and debated steps of the soot formation process in combustion. In this work, we used scanning tunneling microscopy (STM) and spectroscopy (STS) to probe morphological and electronic properties of incipient soot particles formed right behind the flame front of a lightly sooting laminar premixed flame of ethylene and air. Particles were thermophoretically sampled on an atomically flat gold film on a mica substrate. High-resolution STM images of incipient soot particles were obtained for the first time showing the morphology of sub-5 nm incipient soot particles. High-resolution single-particle spectroscopic properties were measured confirming the semiconductor behavior of incipient soot particles with an electronic band gap ranging from 1.5 to 2 eV, consistent with earlier optical and spectroscopic observations.

cond-mat.mtrl-sci↗

arXiv2022

Rb-induced (3x1) and (6x1) reconstructions on Si(111)-(7x7): A LEED and STM study

We present a study of the rubidium adsorption on the Si(111)-(7x7) surface and the related Rb-induced reconstructions as a function of deposition temperature and Rb-coverage via scanning tunneling microscopy (STM) and low-energy electron diffraction (LEED). Sample analysis via LEED allowed to observe for the first time a Rb/Si(111)-(6x1) reconstruction. The STM image analysis allowed to obtain the first real space characterization of the Rb/Si(111)-(3x1) surface. In addition, STM provided a direct and local information on the surface arrangement as well as further insights on the interaction between Si and Rb atoms and on the growth dynamics.

cond-mat.mtrl-sci↗

arXiv2022

Black Phosphorus n-type doping by Cu: a microscopic surface investigation

We study surface charge transfer doping of exfoliated black phosphorus (bP) flakes by copper using scanning tunneling microscopy (STM) and spectroscopy (STS) at room temperature. The tunneling spectra reveal a gap in correspondence of Cu islands, which is attributed to Coulomb blockade phenomena. Moreover, using line spectroscopic measurements across small copper islands, we exploit the potential of the local investigation, showing that the n-type doping effect of copper on bP is short-ranged. These experimental results are substantiated by first-principles simulations, which quantify the role of cluster size for an effective n-type doping of bP and explain the Coulomb blockade by an electronic decoupling of the topmost bP layer from the underlying layers driven by the copper cluster. Our results provide novel understanding, difficult to retrieve by transport measurements, of the doping of bP by copper, which appears promising for the implementation of ultra-sharp p-n junctions in bP.

cond-mat.mtrl-sci↗

arXiv2021

Covalent Organic Functionalization of Graphene Nanosheets and Reduced Graphene Oxide via 1,3-Dipolar Cycloaddition of Azomethine Ylide

Organic functionalization of graphene is successfully performed via 1,3-dipolar cycloaddition of azomethine ylide in the liquid phase. The comparison between 1-methyl-2-pyrrolidinone and N,N-dimethylformamide as dispersant solvents, and between sonication and homogenization as dispersion techniques, proves N,N-dimethylformamide and homogenization as the most effective choice. The functionalization of graphene nanosheets and reduced graphene oxide is confirmed using different techniques. Among them, energy-dispersive X-ray spectroscopy allows to map the pyrrolidine ring of the azomethine ylide on the surface of functionalized graphene, while micro-Raman spectroscopy detects new features arising from the functionalization, which are described in agreement with the power spectrum obtained from ab initio molecular dynamics simulation. Moreover, X-ray photoemission spectroscopy of functionalized graphene allows the quantitative elemental analysis and the estimation of the surface coverage, showing a higher degree of functionalization for reduced graphene oxide. This more reactive behavior originates from the localization of partial charges on its surface due to the presence of oxygen defects, as shown by the simulation of the electrostatic features. Functionalization of graphene using 1,3-dipolar cycloaddition is shown to be a significant step towards the controlled synthesis of graphene-based complex structures and devices at the nanoscale.

cond-mat.mtrl-sci↗

arXiv2021

3D arrangement of epitaxial graphene conformally grown on porousified crystalline SiC

Nanoporous materials represent a versatile solution for a number of applications ranging from sensing, energy applications, catalysis, drug delivery, and many others. The synergy between the outstanding properties of graphene with a three-dimensional porous structure, circumventing the limits of its 2D nature, constitutes therefore a breakthrough for many fields. We report the first three-dimensional growth of epitaxial graphene on a porousified crystalline 4H-SiC(0001). The wafer porosification is performed via a sequence of metal-assisted photochemical and photoelectrochemical etching in hydrofluoric acid based electrolytes. Pore dimensions of the matrix have been evaluated by electron tomography resulting in an average diameter of 180 nm. Graphene growth is performed in an ultra high vacuum environment at a base pressure of $10^{-11}$ mbar. The graphene growth inside the pores is uniform as confirmed by Transmission Electron Microscopy (TEM) analysis. Raman spectroscopy confirms the high quality of the graphene with a 2D/G ratio $>1$ and an average graphene crystal size of $\approx$ 100 nm. Furthermore, it demonstrates a uniform coverage of graphene across the whole sample area. The surface-to-volume ratio of this novel material, its properties, the tunability of the pore size and the scalability of the surface porosification process offer a game changing perspective for a large number of applications.

cond-mat.mtrl-sci↗

arXiv2021

High Mobility Free-Standing InSb Nanoflags Grown On InP Nanowire Stems For Quantum Devices

High quality heteroepitaxial two-dimensional (2D) InSb layers are very difficult to realize owing to the large lattice mismatch with other widespread semiconductor substrates. A way around this problem is to grow free-standing 2D InSb nanostructures on nanowire (NW) stems, thanks to the capability of NWs to efficiently relax elastic strain along the sidewalls when lattice-mismatched semiconductor systems are integrated. In this work, we optimize the morphology of free-standing 2D InSb nanoflags (NFs). In particular, robust NW stems, optimized growth parameters, and the use of reflection high-energy electron diffraction (RHEED), to precisely orient the substrate for preferential growth, are implemented to increase the lateral size of the 2D InSb NFs. Transmission electron microscopy (TEM) analysis of these NFs reveals defect-free zinc blend crystal structure, stoichiometric composition, and relaxed lattice parameters. The resulting NFs are large enough to fabricate Hall-bar contacts with suitable length-to-width ratio enabling precise electrical characterization. An electron mobility of ~29,500 cm2/Vs is measured, which is the highest value reported for free-standing 2D InSb nanostrutures in literature. We envision the use of 2D InSb NFs for fabrication of advanced quantum devices.

cond-mat.mes-hall↗

arXiv2021

Gate-controlled Supercurrent in Ballistic InSb Nanoflag Josephson Junctions

High-quality III-V narrow band gap semiconductor materials with strong spin-orbit coupling and large Lande g-factor provide a promising platform for next-generation applications in the field of high-speed electronics, spintronics, and quantum computing. Indium Antimonide (InSb) offers a narrow band gap, high carrier mobility, and a small effective mass, and thus is very appealing in this context. In fact, this material has attracted tremendous attention in recent years for the implementation of topological superconducting states supporting Majorana zero modes. However, high-quality heteroepitaxial two-dimensional (2D) InSb layers are very diffcult to realize owing to the large lattice mismatch with all commonly available semiconductor substrates. An alternative pathway is the growth of free-standing single-crystalline 2D InSb nanostructures, the so-called nanoflags. Here we demonstrate fabrication of ballistic Josephson-junction devices based on InSb nanoflags with Ti/Nb contacts that show gate-tunable proximity-induced supercurrent up to 50 nA at 250 mK and a sizable excess current. The devices show clear signatures of subharmonic gap structures, indicating phase-coherent transport in the junction and a high transparency of the interfaces. This places InSb nanoflags in the spotlight as a versatile and convenient 2D platform for advanced quantum technologies.

cond-mat.mes-hall↗

arXiv2021

Evidence of Josephson coupling in a few-layer black phosphorus planar Josephson junction

Setting up strong Josephson coupling in van der Waals materials in close proximity to superconductors offers several opportunities both to inspect fundamental physics and to develop novel cryogenic quantum technologies. Here we show evidence of Josephson coupling in a planar few-layer black Phosphorus junction. The planar geometry allows us to probe the junction behavior by means of external gates, at different carrier concentrations. Clear signatures of Josephson coupling are demonstrated by measuring supercurrent flow through the junction at milli Kelvin temperatures. Manifestation of Fraunhofer pattern with a transverse magnetic field is also reported, confirming the Josephson coupling. These findings represent the first evidence of proximity Josephson coupling in a planar junction based on a van der Waals material beyond graphene and open the way to new studies, exploiting the peculiar properties of exfoliated black phosphorus thin flakes.

cond-mat.mes-hall↗

arXiv2021

Anyons in Quantum Hall Interferometry

The quantum Hall (QH) effect represents a unique playground where quantum coherence of electrons can be exploited for various applications, from metrology to quantum computation. In the fractional regime it also hosts anyons, emergent quasiparticles that are neither bosons nor fermions and possess fractional statistics. Their detection and manipulation represent key milestones in view of topologically protected quantum computation schemes. Exploiting the high degree of phase coherence, edge states in the QH regime have been investigated by designing and constructing electronic interferometers, able to reveal the coherence and statistical properties of the interfering constituents. Here, we review the two main geometries developed in the QH regime, the Mach-Zehnder and the Fabry-Perot interferometers. We present their basic working principles, fabrication methods, and the main results obtained both in the integer and fractional QH regime. We will also show how recent technological advances led to the direct experimental demonstration of fractional statistics for Laughlin quasiparticles in a Fabry-Perot interferometric setup.

cond-mat.mes-hall↗