arXiv subjects

Stefano Veronesi

Publications and source records attributed to Stefano Veronesi.

At least 19 recordsLinked to original sources

arXiv2026

Oxidation-resilient structural modifications in Nickel-functionalized 3D-graphene for hydrogen storage applications

Porous materials represent a versatile solution for several applications. Indeed, the recent development of a new material, named 3D-Graphene, which combines the exceptional characteristics of graphene with a three-dimensional structure, opens perspectives for applications where a high surface-to-volume ratio is beneficial. In this study, we explore the functionalization of 3D-Graphene with nickel (Ni)-nanoparticles as a strategy to enhance hydrogen storage capabilities, and we assess the influence of the NPs on hydrogen uptake and oxidation resilience. The morphology and structural properties of pristine and Ni-functionalized samples were characterized using Scanning Electron Microscopy. Additionally, X-ray Photoelectron Spectroscopy was employed to analyze the surface chemical composition of the functionalized samples. Samples have been hydrogenated supplying molecular or atomic hydrogen, and hydrogen storage performance was assessed through Thermal Desorption Spectroscopy. Afterwards, oxidation effects were systematically studied by exposing the samples to atmospheric oxygen, followed by further hydrogenation experiments. Our results indicate that Ni functionalization influences both hydrogen adsorption and oxidation behavior, with potential implications for improving the stability of the material, especially for hydrogen storage applications.

cond-mat.mtrl-sci↗

arXiv2026

Nickel intercalation in epitaxial graphene on SiC(0001): a novel platform for engineering two-dimensional heterostructures

Two-dimensional (2D) magnetic materials integrated with graphene offer a compelling platform for next-generation spintronic devices, yet nickel in its 2D form remains largely unexplored, due to fundamental synthesis limitations. Here, we report the controlled intercalation of Ni beneath epitaxial graphene on the Si-face of SiC(0001), achieved through a scalable colloidal nanoparticle deposition route. Chemically synthesized Ni nanoparticles (~10 nm diameter) are uniformly deposited onto graphene via immersion in colloidal solution at room temperature; subsequent thermal annealing at 650 {\deg}C drives intercalation, yielding well-ordered Ni islands at the graphene/buffer-layer interface with morphology dictated by annealing conditions. Scanning tunneling microscopy (STM) and angle-resolved photoemission spectroscopy (ARPES), supported by density functional theory (DFT) calculations, elucidate the atomic and electronic structure of the intercalated layers. DFT simulations further confirm the thermodynamic stability of the 2D nanostructures as a function of shape and lateral size, predicting a robust average magnetic moment of 0.9 $\mu_B$ per atom. The resulting Ni-intercalated graphene on SiC constitutes a well-defined 2D heterostructure combining preserved graphene band structure with robust interfacial magnetism, stable under ambient conditions. These findings establish a reproducible, scalable pathway to engineer magnetic graphene-based heterostructures and open new avenues for their integration into spintronic architectures.

cond-mat.mtrl-sci↗

arXiv2025

Impact of hydrogenation on the structure, chemistry, and electrical properties of flame-synthesized carbon nanoparticle films

The interaction between hydrogen atoms and carbon nanoparticles is a fundamental process governing the properties of carbonaceous materials in environments ranging from combustion systems to the interstellar medium. This study investigates the effects of controlled atomic hydrogen exposure on young and mature soot nanoparticles, generated in premixed ethylene-air flames, and deposited on substrates. We employed a multi-technique approach to characterize the chemical, mechanical, and electrical evolution of the films. In-situ infrared spectroscopy revealed non-monotonic behavior: an initial increase in aliphatic CH bonds was observed, followed by a decrease at higher hydrogen fluences. This was accompanied by a continuous decrease in the aromatic C=C signal. Atomic force microscopy showed a significant increase in the Young's modulus of the film for both sample types after hydrogenation. This mechanical change was correlated with an increase in the I(D)/I(G) ratio from Raman spectroscopy. Furthermore, both macroscopic current vs. voltage and local scanning tunneling spectroscopy measurements demonstrated a notable increase in electrical conductivity. For single just-formed soot particles, moreover, a hydrogen-induced transformation from a semiconductive to a semi-metallic nature was observed. The collective evidence points towards an H-induced CC cross-linking mechanism within the nanoparticle films. We propose that atomic hydrogen facilitates the formation of radical sites, which promotes covalent bond formation between adjacent particles or molecular units, creating a more interconnected and rigid network, with smaller interlayer distance. These findings provide crucial insights into the structural evolution of carbonaceous materials in hydrogen-rich environments, with direct implications for understanding soot formation and for the tailored design of carbon-based materials.

cond-mat.mes-hall↗

arXiv2025

Vortex Pinning in Niobium covered by a thin polycrystalline Gold

Owing to its superconducting properties, Niobium (Nb) is an excellent candidate material for superconducting electronics and applications in quantum technology. Here we perform scanning tunneling microscopy and spectroscopy experiments on Nb films covered by a thin gold (Au) film. We investigate the minigap structure of the proximitized region and provide evidence for a highly transparent interface between Nb and Au, beneficial for device applications. Imaging of Abrikosov vortices in presence of a perpendicular magnetic field is reported. The data show vortex pinning by the granular structure of the polycrystalline Au film. Our results show robust and homogeneous superconducting properties of thin Nb film in the presence of a gold capping layer. The Au film not only protects the Nb from surface oxidation but also preserves its excellent superconducting properties.

cond-mat.supr-con↗

arXiv2025

Novel structures of Gallenene intercalated in epitaxial Graphene

The creation of atomically thin layers of non-exfoliable materials remains a crucial challenge, requiring the development of innovative techniques. Here, confinement epitaxy is exploited to realize two-dimensional gallium via intercalation in epitaxial graphene grown on silicon carbide. Novel superstructures arising from the interaction of gallenene (a monolayer of gallium) with graphene and the silicon carbide substrate are investigated. The coexistence of different gallenene phases, including b010-gallenene and the elusive high-pressure Ga(III) phase, is identified. This work sheds new light on the formation of two-dimensional gallium and provides a platform for investigating the exotic electronic and optical properties of confined gallenene.

cond-mat.mtrl-sci↗

arXiv2025

Surface Grafting of Graphene Flakes with Fluorescent Dyes: A Tailored Functionalization Approach

The controlled functionalization of graphene is critical for tuning and enhancing its properties, thereby expanding its potential applications. Covalent functionalization offers a deeper tuning of the geometric and electronic structure of graphene compared to non-covalent methods; however, the existing techniques involve side reactions and spatially uncontrolled functionalization, pushing research toward more selective and controlled methods. A promising approach is 1,3-dipolar cycloaddition, successfully utilized with carbon nanotubes. In the present work, this method has been extended to graphene flakes with low defect concentration. A key innovation is the use of a custom-synthesized ylide with a protected amine group (Boc), facilitating subsequent attachment of functional molecules. Indeed, after Boc cleavage, fluorescent dyes (Atto 425, 465, and 633) were covalently linked via NHS ester derivatization. This approach represents a highly selective method of minimizing structural damage. Successful functionalization was demonstrated by Raman spectroscopy, photoluminescence spectroscopy, and confocal microscopy, confirming the effectiveness of the method. This novel approach offers a versatile platform, enabling its use in biological imaging, sensing, and advanced nanodevices. The method paves the way for the development of sensors and devices capable of anchoring a wide range of molecules, including quantum dots and nanoparticles. Therefore, it represents a significant advancement in graphene-based technologies.

cond-mat.mtrl-sci↗

arXiv2025

Intercalated structures formed by platinum on epitaxial graphene on SiC(0001)

Graphene on SiC intercalated with two-dimensional metal layers, such as Pt, offers a versatile platform for applications in spintronics, catalysis, and beyond. Recent studies have demonstrated that Pt atoms can intercalate at the heterointerface between SiC(0001) and the C-rich $(6\sqrt{3}\times6\sqrt{3})$R30{\deg} reconstructed surface (hereafter referred as the buffer layer). However, key aspects such as intercalated phase structure and intercalation mechanisms remain unclear. In this work, we investigate changes in morphology, chemistry, and electronic structure for both buffer layer and monolayer graphene grown on SiC(0001) following Pt deposition and annealing cycles, which eventually led to Pt intercalation at temperatures above 500{\deg}C. Atomic-resolution imaging of the buffer layer reveals a single intercalated Pt layer that removes the periodic corrugation of the buffer layer, arising from partial bonding of C-atoms with Si-atoms of the substrate. In monolayer graphene, the Pt-intercalated regions exhibit a two-level structure: the first level corresponds to a Pt layer intercalated below the buffer layer, while the second level contains a second Pt layer, giving rise to a $(12\times12)$ superstructure relative to graphene. Upon intercalation, Pt atoms appear as silicides, indicating a reaction with Si atoms from the substrate. Additionally, charge neutral $\pi$-bands corresponding to quasi-free-standing monolayer and bilayer graphene emerge. Analysis of multiple samples, coupled with a temperature-dependent study of the intercalation rate, demonstrates the pivotal role of buffer layer regions in facilitating the Pt intercalation in monolayer graphene. These findings provide valuable insight into Pt intercalation, advancing the potential for applications.

cond-mat.mtrl-sci↗

arXiv2025

Rubidium intercalation in epitaxial monolayer graphene

Alkali metal intercalation of graphene layers has been of particular interest due to potential applications in electronics, energy storage, and catalysis. Rubidium (Rb) is one of the largest alkali metals and the one less investigated as intercalant. Here, we report a systematic investigation, with a multi-technique approach, of the phase formation of Rb under epitaxial monolayer graphene on SiC(0001). We explore a wide phase space with two control parameters: the Rb density (i.e., deposition time) and sample temperature (i.e., room- and low-temperature). We reveal the emergence of $(2 \times 2)$ and $(\sqrt{3} \times \sqrt{3})$R30{\deg} structures formed by a single alkali metal layer intercalated between monolayer graphene and the interfacial C-rich reconstructed surface, also known as buffer layer. Rb intercalation also results in a strong n-type doping of the graphene layer. Progressively annealing to high temperatures, we first reveal diffusion of Rb atoms which results in the enlargement of intercalated areas. As desorption sets in, intercalated regions progressively shrink and fragment. Eventually, at approximately 600{\deg}C the initial surface is retrieved, indicating the reversibility of the intercalation process.

cond-mat.mtrl-sci↗

arXiv2024

Rapid synthesis of uniformly small nickel nanoparticles for the surface functionalization of epitaxial graphene

Nickel nanoparticles (Ni NPs), thanks to their peculiar properties, are interesting materials for many applications including catalysis, hydrogen storage, and sensors. In this work, Ni NPs are synthesized in aqueous solution by a simple and rapid procedure with cetyltrimethylammonium bromide (CTAB) as a capping agent, and are extensively characterized by dynamic light scattering (DLS), scanning electron microscopy (SEM), and atomic force microscopy (AFM). We investigated their shape, dimension, and their distribution on the surfaces of SiO2 and epitaxial graphene (EG) samples. Ni NPs have an average diameter of ~11 nm, with a narrow size dispersion, and their arrangement on the surface is strongly dependent on the substrate. EG samples functionalized with Ni NPs are further characterized by X-ray photoelectron spectroscopy (XPS), as made and after thermal annealing above 350{\deg}C to confirm the degradation of CTAB and the presence of metallic Ni(0). Moreover, high resolution scanning tunneling microscopy (STM) topographies reveal the structural stability of the NPs up to 550 {\deg}C.

cond-mat.mtrl-sci↗

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{\deg}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{\deg}C to hydrogen physisorbed on the surface of Pt clusters. The second peak at 430{\deg}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

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

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↗

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↗