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Alessandro Baraldi

Publications and source records attributed to Alessandro Baraldi.

10 recordsLinked to original sources

Electronic structure of Graphene/Co interfaces

Photoemission, from core levels and valence band, and low-energy electron diffraction (LEED) have been employed to investigate the electronic and structural properties of novel graphene-ferromagnetic (G-FM) systems,obtained by intercalation of one mono-layer (1ML) and several layers (4ML) of Co on G grown on Ir(111). Upon intercalation of 1ML of Co, the Co lattice is resized to match the Ir-Ir lattice parameter, resulting in a mismatched G/Co/Ir(111) system. The intercalation of further Co layers leads to a relaxation of the Co lattice and a progressive formation of a commensurate G layer lying on top. We show the C 1s line shape and the band structure of G in the two artificial phases, mismatched and commensurate G/Co, through a comparison with the electronic structure of G grown directly on a Co thick film. Our results show that while the G valence band mainly reflects the hybridization with the d states of Co, regardless of the structural phase, the C 1s line shape is very sensitive to the rumpling of the G layer and the coordination of carbon atoms with the underlying Co. Even in the commensurate (1x1) G/Co phase, where graphene is in register with the Co film, from the angular dependence of the C 1s core level we infer the presence of a double component, due to in-equivalent adsorption sites of carbon sub-lattices.

cond-mat.mtrl-sci

The rise and fall of an oxide: growth and evolution of Bismuth Oxide on Au(111)

We report a comprehensive, multi-technique study of bismuth oxide growth on Au(111) under different conditions such as temperature and exposure to molecular oxygen. By combining synchrotron-based X-ray photoelectron spectroscopy and diffraction with low-energy electron diffraction and scanning tunneling microscopy, we elucidate the structural evolution of the system during controlled oxidation and subsequent annealing. We find that Bi deposition induces well-defined surface reconstructions, whereas oxidation triggers the formation of a complex sequence of bismuth oxide domains. High-resolution spectroscopic and diffraction data enable us to pinpoint the structure of the oxide consistent with the $(201)$ surface of $\beta$-Bi$_2$O$_3$. In addition, angle resolved photoemission experiments and work function measurements reveal substantial electronic modifications triggered by a complex interplay of segregation of Bi and Au. Notably, a work function of 3.4 eV is achieved for oxidation at 423 K. These results provide benchmark structural and electronic insights into the Bi oxide/Au(111) system and establish a framework for integrating Bi$_2$O$_3$ as a contact material in devices using two-dimensional semiconductors, where it can enable low contact resistance.

cond-mat.mtrl-sci

Interfacial two-dimensional oxide enhances photocatalytic activity of graphene/titania via electronic structure modification

A two-dimensional layer of oxide reveals itself as a essential element to drive the photocatalytic activity in a nanostructured hybrid material, which combines high-quality epitaxial graphene and titanium dioxide nanoparticles. In particular, it has been revealed that the addition of a 2D Ti oxide layer sandwiched between graphene and metal induces a p-doping of graphene and a consistent shift in the Ti d states. These modifications induced by the interfacial oxide layer induce a reduction of the probability of charge carrier recombination and enhance the photocatalytic activity of the heterostructure. This is indicative of a capital role played by thin oxide films in fine-tuning the properties of heterostructures based on graphene and pave the way to new combinations of graphene/oxides for photocatalysis-oriented applications.

cond-mat.mtrl-sci

Electron-phonon coupling in single-layer MoS2

The electron-phonon coupling strength in the spin-split valence band maximum of single-layer MoS$_2$ is studied using angle-resolved photoemission spectroscopy and density functional theory-based calculations. Values of the electron-phonon coupling parameter $\lambda$ are obtained by measuring the linewidth of the spin-split bands as a function of temperature and fitting the data points using a Debye model. The experimental values of $\lambda$ for the upper and lower spin-split bands at K are found to be 0.05 and 0.32, respectively, in excellent agreement with the calculated values for a free-standing single-layer MoS$_2$. The results are discussed in the context of spin and phase-space restricted scattering channels, as reported earlier for single-layer WS$_2$ on Au(111). The fact that the absolute valence band maximum in single-layer MoS$_2$ at K is almost degenerate with the local valence band maximum at $\Gamma$ can potentially be used to tune the strength of the electron-phonon interaction in this material.

cond-mat.mtrl-sci

Growth and Structure of Singly-Oriented Single-Layer Tungsten Disulfide on Au(111)

We present a complete characterisation at the nanoscale of the growth and structure of single-layer tungsten disulfide (WS$_2$) epitaxially grown on Au(111). Following the growth process in real time with fast x-ray photoelectron spectroscopy, we obtain a singly-oriented layer by choosing the proper W evaporation rate and substrate temperature during the growth. Information about the morphology, size and layer stacking of the WS$_2$ layer were achieved by employing x-ray photoelectron diffraction and low-energy electron microscopy. The strong spin splitting in the valence band of WS$_2$ coupled with the single-orientation character of the layer make this material the ideal candidate for the exploitation of the spin and valley degrees of freedom.

cond-mat.mtrl-sci

Epitaxial Growth of Single-Orientation High-Quality MoS$_2$ Monolayers

We present a study on the growth and characterization of high-quality single-layer MoS$_2$ with a single orientation, i.e. without the presence of mirror domains. This single orientation of the MoS$_2$ layer is established by means of x-ray photoelectron diffraction. The high quality is evidenced by combining scanning tunneling microscopy with x-ray photoelectron spectroscopy measurements. Spin- and angle-resolved photoemission experiments performed on the sample revealed complete spin-polarization of the valence band states near the K and -K points of the Brillouin zone. These findings open up the possibility to exploit the spin and valley degrees of freedom for encoding and processing information in devices that are based on epitaxially grown materials.

cond-mat.mtrl-sci

Photoemission Investigation of Oxygen Intercalated Epitaxial Graphene on Ru(0001)

We study the formation of epitaxial graphene on Ru(0001) using fast x-ray photoelectron spectroscopy during the growth process. The assignment of different C 1s and Ru 3d core level components and their evolution during the growth process gives a detailed insight into the graphene formation and the strongly varying graphene-Ru interaction strength within the large moire unit cell. Subsequent intercalation of oxygen can be achieved at elevated temperature and the core level spectra show a conversion of the strongly corrugated to quasi free-standing graphene, characterised by a single narrow C 1s component. This conversion and the accompanying flattening of the graphene layer is also confirmed by x-ray photoelectron diffraction. The effect of oxygen intercalation on the electronic structure is studied using angle-resolved photoemission of the valence band states. For graphene/Ru(0001), the strong graphene-substrate hybridisation disrupts the {\pi}-band dispersion but oxygen intercalation fully restores the {\pi}-band with a strong p-doping that shifts the Dirac point 785 meV above the Fermi level. The doping of the system is highly tunable, as the additional exposure to rubidium can convert the carrier filling to n-type with the Dirac point 970 meV below the Fermi level.

cond-mat.mtrl-sci

Electron-phonon coupling in the spin-split valence band of single layer WS$_2$

The absence of inversion symmetry leads to a strong spin-orbit splitting of the upper valence band of semiconducting single layer transition metal dichalchogenides such as MoS$_2$ or WS$_2$. This permits a direct comparison of the electron-phonon coupling strength in states that only differ by their spin. Here, the electron-phonon coupling in the valence band maximum of single-layer WS$_2$ is studied by first principles calculations and angle-resolved photoemission. The coupling strength is found to be drastically different for the two spin-split branches, with calculated values of $\lambda_K=$0.0021 and 0.40 for the upper and lower spin-split valence band of the free-standing layer, respectively. This difference is somewhat reduced when including scattering processes involving the Au(111) substrate present in the experiment and the experimental results confirm the strongly branch-dependent coupling strength.

cond-mat.str-el

Transfer-free electrical insulation of epitaxial graphene from its metal substrate

High-quality, large-area epitaxial graphene can be grown on metal surfaces but its transport properties cannot be exploited because the electrical conduction is dominated by the substrate. Here we insulate epitaxial graphene on Ru(0001) by a step-wise intercalation of silicon and oxygen, and the eventual formation of a SiO$_2$ layer between the graphene and the metal. We follow the reaction steps by x-ray photoemission spectroscopy and demonstrate the electrical insulation using a nano-scale multipoint probe technique.

cond-mat.mes-hall

High-temperature behaviour of supported graphene: electron-phonon coupling and substrate-induced doping

One of the salient features of graphene is the very high carrier mobility that implies tremendous potential for use in electronic devices. Unfortunately, transport measurements find the expected high mobility only in freely suspended graphen. When supported on a surface, graphene shows a strongly reduced mobility, and an especially severe reduction for temperatures above 200 K. A temperature-dependent mobility reduction could be explained by scattering of carriers with phonons, but this is expected to be weak for pristine, weakly-doped graphene. The mobility reduction has therefore been ascribed to the interaction with confined ripples or substrate phonons. Here we study the temperature-dependent electronic structure of supported graphene by angle-resolved photoemission spectroscopy, a technique that can reveal the origin of the phenomena observed in transport measurements. We show that the electron-phonon coupling for weakly-doped, supported graphene on a metal surface is indeed extremely weak, reaching the lowest value ever reported for any material. However, the temperature-dependent dynamic interaction with the substrate leads to a complex and dramatic change in the carrier type and density that is relevant for transport. Using ab initio molecular dynamics simulations, we show that these changes in the electronic structure are mainly caused by fluctuations in the graphene-substrate distance.

cond-mat.mes-hall