Surfaces and Interfaces, Condensed Matter Physics, General Physics and Astronomy, Physical and Theoretical Chemistry
60
Scopus Publications
1031
Scholar Citations
18
Scholar h-index
32
Scholar i10-index
Scopus Publications
Unraveling the interaction of Ta atoms with Pt(111) Kevin Bertrang, Tobias Hinke, Sebastian Kaiser, Matthias Knechtges, Federico Loi, Luca Sbuelz, Paolo Lacovig, Luca Bignardi, Friedrich Esch, Alessandro Baraldi,et al. Elsevier BV
Unveiling Inequality of Atoms in Ultrasmall Pt Clusters: Oxygen Adsorption Limited to the Uppermost Atomic Layer Federico Loi, Luca Bignardi, Deborah Perco, Andrea Berti, Paolo Lacovig, Silvano Lizzit, Aras Kartouzian, Ulrich Heiz, Dario Alfè, and Alessandro Baraldi Wiley The concept of preferential atomic and molecular adsorption site is of primary relevance in heterogeneous catalysis. In the case of ultrasmall size‐selected clusters, distinguishing the role played by each atom in a reaction is extremely challenging due to their reduced size and peculiar structures. Herein, it is revealed how the inequivalent atoms composing graphene‐supported Pt12 and Pt13 clusters behave differently in the photoinduced dissociation of O2, with only those in the uppermost layer of the clusters being involved in the reaction. In this process, the epitaxial graphene support plays a fundamental active role: its corrugation and pinning induced by the presence of the clusters are crucial for defining the preferential adsorption site on the Pt atomic agglomerates, facilitating the lateral diffusion of physisorbed oxygen at a distance that induces its selective adsorption in the topmost layer of the clusters, and inducing an inhomogeneous charge distribution within the clusters which directly affects the O2 adsorption. The inhomogeneous oxidation of the clusters is resolved by means of synchrotron‐based X‐ray photoelectron spectroscopy and supported by ab initio density functional theory calculations. The possibility to identify the active sites on Pt clusters induced by cluster–support interactions has the potential to enhance the experimentally supported design of nanocatalysts.
Graphene growth from photo-polymerized bi-phenylthiol self-assembled monolayers Tashfeen Zehra, Ali Syari’ati, Oleksii Ivashenko, Luca Bignardi, Willem F. Van Dorp, Jeff T. M. De Hosson, and Petra Rudolf Frontiers Media SA We present an enhanced methodology for the synthesis of graphene, from photo-polymerized self-assembled monolayers (SAMs) of 1,1ʹ-biphenyl-4-thiol on both electropolished and oxidized copper substrates. The SAMs were subjected to a two-step process involving light-induced polymerization followed by annealing in a vacuum furnace to yield the two-dimensional solid. Comprehensive characterization using contact angle measurements, X-ray photoelectron spectroscopy, and Raman spectroscopy, as well as scanning electron and transmission electron microscopy, provided conclusive evidence of growth of single-layer graphene. Notably, our findings revealed superior quality graphene on oxidized copper substrates compared to their electropolished counterparts, highlighting the impact of substrate choice on the quality of the resultant material.
The highest oxidation state observed in graphene-supported sub-nanometer iron oxide clusters Deborah Perco, Federico Loi, Luca Bignardi, Luca Sbuelz, Paolo Lacovig, Ezequiel Tosi, Silvano Lizzit, Aras Kartouzian, Ueli Heiz, and Alessandro Baraldi Springer Science and Business Media LLC AbstractSize-selected iron oxide nanoclusters are outstanding candidates for technological-oriented applications due to their high efficiency-to-cost ratio. However, despite many theoretical studies, experimental works on their oxidation mechanism are still limited to gas-phase clusters. Herein we investigate the oxidation of graphene-supported size-selected Fen clusters by means of high-resolution X-ray Photoelectron Spectroscopy. We show a dependency of the core electron Fe 2p3/2 binding energy of metallic and oxidized clusters on the cluster size. Binding energies are also linked to chemical reactivity through the asymmetry parameter which is related to electron density of states at the Fermi energy. Upon oxidation, iron atoms in clusters reach the oxidation state Fe(II) and the absence of other oxidation states indicates a Fe-to-O ratio close to 1:1, in agreement with previous theoretical calculations and gas-phase experiments. Such knowledge can provide a basis for a better understanding of the behavior of iron oxide nanoclusters as supported catalysts.
In situ observation of the on-surface thermal dehydrogenation of n-octane on Pt(111) Daniel Arribas, Víctor Villalobos-Vilda, Ezequiel Tosi, Paolo Lacovig, Alessandro Baraldi, Luca Bignardi, Silvano Lizzit, José Ignacio Martínez, Pedro Luis de Andres, Alejandro Gutiérrez,et al. Royal Society of Chemistry (RSC) We study the thermal dehydrogenation of n-octane on Pt(111) under ultra-high vacuum. Combining scanning tunneling microscopy (STM), photoelectron spectroscopy and mass spectroscopy with calculations, we provide an atomic-scale view of the on-surface products.
Spotting Local Environments in Self-Assembled Monolayer-Protected Gold Nanoparticles Cristian Gabellini, Maria Şologan, Elena Pellizzoni, Domenico Marson, Mario Daka, Paola Franchi, Luca Bignardi, Stefano Franchi, Zbyšek Posel, Alessandro Baraldi,et al. American Chemical Society (ACS) Organic–inorganic (O–I) nanomaterials are versatile platforms for an incredible high number of applications, ranging from heterogeneous catalysis to molecular sensing, cell targeting, imaging, and cancer diagnosis and therapy, just to name a few. Much of their potential stems from the unique control of organic environments around inorganic sites within a single O–I nanomaterial, which allows for new properties that were inaccessible using purely organic or inorganic materials. Structural and mechanistic characterization plays a key role in understanding and rationally designing such hybrid nanoconstructs. Here, we introduce a general methodology to identify and classify local (supra)molecular environments in an archetypal class of O–I nanomaterials, i.e., self-assembled monolayer-protected gold nanoparticles (SAM-AuNPs). By using an atomistic machine-learning guided workflow based on the Smooth Overlap of Atomic Positions (SOAP) descriptor, we analyze a collection of chemically different SAM-AuNPs and detect and compare local environments in a way that is agnostic and automated, i.e., with no need of a priori information and minimal user intervention. In addition, the computational results coupled with experimental electron spin resonance measurements prove that is possible to have more than one local environment inside SAMs, being the thickness of the organic shell and solvation primary factors in the determining number and nature of multiple coexisting environments. These indications are extended to complex mixed hydrophilic–hydrophobic SAMs. This work demonstrates that it is possible to spot and compare local molecular environments in SAM-AuNPs exploiting atomistic machine-learning approaches, establishes ground rules to control them, and holds the potential for the rational design of O–I nanomaterials instructed from data.
Oxidation at the sub-nanoscale: oxygen adsorption on graphene-supported size-selected Ag clusters Federico Loi, Monica Pozzo, Luca Sbuelz, Luca Bignardi, Paolo Lacovig, Ezequiel Tosi, Silvano Lizzit, Aras Kartouzian, Ueli Heiz, Dario Alfè,et al. Royal Society of Chemistry (RSC) Oxidizing size-selected Ag11 clusters on graphene reveals the formation of a bulk-like structure already for few-atom aggregates. The appearance of a bulk AgO crystal structure differs from that observed for metallic clusters of similar size.
Anisotropic strain in epitaxial single-layer molybdenum disulfide on Ag(110) Luca Bignardi, Sanjoy K. Mahatha, Daniel Lizzit, Harsh Bana, Elisabetta Travaglia, Paolo Lacovig, Charlotte Sanders, Alessandro Baraldi, Philip Hofmann, and Silvano Lizzit Royal Society of Chemistry (RSC) Uniaxial lattice strain is introduced in the lattice of a MoS2single layer epitaxially-grown on Ag(110). Growth on a substrate with different crystalline symmetry is thus a promising way to introduce uniform strain in TMDC single layers.
Ultrafast electronic linewidth broadening in the C core level of graphene Davide Curcio, Sahar Pakdel, Klara Volckaert, Jill A. Miwa, Søren Ulstrup, Nicola Lanatà, Marco Bianchi, Dmytro Kutnyakhov, Federico Pressacco, Günter Brenner,et al. American Physical Society (APS) Core level binding energies and absorption edges are at the heart of many experimental techniques concerned with element-specific structure, electronic structure, chemical reactivity, elementary excitations and magnetism. X-ray photoemission spectroscopy (XPS) in particular, can provide information about the electronic and vibrational many-body interactions in a solid as these are reflected in the detailed energy distribution of the photoelectrons. Ultrafast pump-probe techniques add a new dimension to such studies, introducing the ability to probe a transient state of the many-body system. Here we use a free electron laser to investigate the effect of a transiently excited electron gas on the core level spectrum of graphene, showing that it leads to a large broadening of the C 1s peak. Confirming a decade-old prediction, the broadening is found to be caused by an exchange of energy and momentum between the photoemitted core electron and the hot electron system, rather than by vibrational excitations. This interpretation is supported by a line shape analysis that accounts for the presence of the excited electrons. Fitting the spectra to this model directly yields the electronic temperature of the system, in agreement with electronic temperature values obtained from valence band data. Furthermore, making use of time- and momentum-resolved C 1s spectra, we illustrate how the momentum change of the outgoing core electrons leads to a small but detectable change in the time-resolved photoelectron diffraction pattern and to a nearly complete elimination of the core level binding energy variation associated with the narrow $\\sigma$-band in the C 1s state. The results demonstrate that the XPS line shape can be used as an element-specific and local probe of the excited electron system and that X-ray photoelectron diffraction investigations remain feasible at very high electronic temperatures.
Atomic Undercoordination in Ag Islands on Ru(0001) Grown via Size-Selected Cluster Deposition: An Experimental and Theoretical High-Resolution Core-Level Photoemission Study Luca Sbuelz, Federico Loi, Monica Pozzo, Luca Bignardi, Eugenio Nicolini, Paolo Lacovig, Ezequiel Tosi, Silvano Lizzit, Aras Kartouzian, Ueli Heiz,et al. American Chemical Society (ACS) The possibility of depositing precisely mass-selected Ag clusters (Ag1, Ag3, and Ag7) on Ru(0001) was instrumental in determining the importance of the in-plane coordination number (CN) and allowed us to establish a linear dependence of the Ag 3d5/2 core-level shift on CN. The fast cluster surface diffusion at room temperature, caused by the low interaction between silver and ruthenium, leads to the formation of islands with a low degree of ordering, as evidenced by the high density of low-coordinated atomic configurations, in particular CN = 4 and 5. On the contrary, islands formed upon Ag7 deposition show a higher density of atoms with CN = 6, thus indicating the formation of islands with a close-packed atomic arrangement. This combined experimental and theoretical approach, when applied to clusters of different elements, offers the perspective to reveal nonequivalent local configurations in two-dimensional (2D) materials grown using different building blocks, with potential implications in understanding electronic and reactivity properties at the atomic level.
Unusual reversibility in molecular break-up of PAHs: The case of pentacene dehydrogenation on Ir(111) Davide Curcio, Emil Sierda, Monica Pozzo, Luca Bignardi, Luca Sbuelz, Paolo Lacovig, Silvano Lizzit, Dario Alfè, and Alessandro Baraldi Royal Society of Chemistry (RSC) In this work, we characterise the adsorption of pentacene molecules on Ir(111) and their dissociation behaviour as a function of temperature.
In Situ Synthesis of Metal-Salophene Complexes on Intercalated Graphene Micha Elsebach, Emil Sierda, Julia J. Goedecke, Luca Bignardi, Michal Hermanowicz, Michael Rohde, Roland Wiesendanger, and Maciej Bazarnik American Chemical Society (ACS) On-surface metalation provides a tool to vary magnetic and electronic properties of metal–organic complexes and produces clean samples of the desired product. We used this technique to metalate 5,5...
Layer and orbital interference effects in photoemission from transition metal dichalcogenides Habib Rostami, Klara Volckaert, Nicola Lanata, Sanjoy K. Mahatha, Charlotte E. Sanders, Marco Bianchi, Daniel Lizzit, Luca Bignardi, Silvano Lizzit, Jill A. Miwa,et al. American Physical Society (APS) In this work, we provide an effective model to evaluate the one-electron dipole matrix elements governing optical excitations and the photoemission process of single-layer (SL) and bilayer (BL) transition metal dichalcogenides. By utilizing a $\\vec{k} \\cdot \\vec{p}$ Hamiltonian, we calculate the photoemission intensity as observed in angle-resolved photoemission from the valence bands around the $\\bar{K}$-valley of MoS$_2$. In SL MoS$_2$ we find a significant masking of intensity outside the first Brillouin zone, which originates from an in-plane interference effect between photoelectrons emitted from the Mo $d$ orbitals. In BL MoS$_2$ an additional inter-layer interference effect leads to a distinctive modulation of intensity with photon energy. Finally, we use the semiconductor Bloch equations to model the optical excitation in a time- and angle-resolved pump-probe photoemission experiment. We find that the momentum dependence of an optically excited population in the conduction band leads to an observable dichroism in both SL and BL MoS$_2$.
RECENT SCHOLAR PUBLICATIONS
Unraveling the interaction of Ta atoms with Pt (111) K Bertrang, T Hinke, S Kaiser, M Knechtges, F Loi, L Sbuelz, P Lacovig, ... Surfaces and Interfaces 56, 105640 2025
Unveiling Inequality of Atoms in Ultrasmall Pt Clusters: Oxygen Adsorption Limited to the Uppermost Atomic Layer F Loi, L Bignardi, D Perco, A Berti, P Lacovig, S Lizzit, A Kartouzian, ... Small Structures 5 (11), 2400250 2024
Unraveling oxygen-driven surface segregation dynamics in platinum-gold alloys A Berti, M D’Alessio, M Bianchi, L Bignardi, P Lacovig, C Sanders, S Lizzit, ... Applied Surface Science 670, 160577 2024
Determining the atomic coordination number in the structure of β12 borophene on Ag (111) via X-ray photoelectron diffraction analysis L Bignardi, M Pozzo, A Zelenika, F Presel, P Lacovig, S Lizzit, D Alf, ... Surfaces and Interfaces 51, 104791 2024
Graphene growth from photo-polymerized bi-phenylthiol self-assembled monolayers T Zehra, A Syari’Ati, O Ivashenko, L Bignardi, WF Van Dorp, ... Frontiers in Nanotechnology 6, 1366542 2024
Attosecond dynamics of photoemission over a wide photon energy range C Schrder, J Riemensberger, R Kuzian, M Ossiander, D Potamianos, ... 2023
Breakdown of the correlation between oxidation states and core electron binding energies at the sub-nanoscale F Loi, M Pozzo, L Sbuelz, L Bignardi, P Lacovig, E Tosi, S Lizzit, ... Applied Surface Science 619, 156755 2023
The highest oxidation state observed in graphene-supported sub-nanometer iron oxide clusters D Perco, F Loi, L Bignardi, L Sbuelz, P Lacovig, E Tosi, S Lizzit, ... Communications Chemistry 6 (1), 61 2023
Interplay among hydrogen chemisorption, intercalation, and bulk diffusion at the graphene-covered Ni (111) crystal M Pozzo, T Turrini, L Bignardi, P Lacovig, D Lizzit, E Tosi, S Lizzit, ... The Journal of Physical Chemistry C 127 (14), 6938-6947 2023
Exploring 2D materials at surfaces through synchrotron-based core-level photoelectron spectroscopy L Bignardi, P Lacovig, R Larciprete, D Alfe, S Lizzit, A Baraldi Surface Science Reports 78 (1), 100586 2023
Correction: In situ observation of the on-surface thermal dehydrogenation of n-octane on Pt (111) D Arribas, V Villalobos-Vilda, E Tosi, P Lacovig, A Baraldi, L Bignardi, ... Nanoscale 15 (35), 14680-14680 2023
In situ observation of the on-surface thermal dehydrogenation of n-octane on Pt (111) D Arribas, V Villalobos-Vilda, E Tosi, P Lacovig, A Baraldi, L Bignardi, ... Nanoscale 15 (35), 14458-14467 2023
Spotting Local Environments in Self-Assembled Monolayer-Protected Gold Nanoparticles C Gabellini, M Sologan, E Pellizzoni, D Marson, M Daka, P Franchi, ... ACS nano 16 (12), 20902-20914 2022
Thiolate end-group regulates ligand arrangement, hydration and affinity for small compounds in monolayer-protected gold nanoparticles E Pellizzoni, M Şologan, M Daka, P Pengo, D Marson, Z Posel, S Franchi, ... Journal of Colloid and Interface Science 607, 1373-1381 2022
Vibrational Fine Structure in C 1s High-Resolution Core-Level Spectra of CO Chemisorbed on Ir (111) S Baronio, VD Leo, G Lautizi, P Mantegazza, E Natale, M Tuniz, S Vigneri, ... The Journal of Physical Chemistry C 126 (3), 1411-1419 2022
Oxidation at the sub-nanoscale: oxygen adsorption on graphene-supported size-selected Ag clusters F Loi, M Pozzo, L Sbuelz, L Bignardi, P Lacovig, E Tosi, S Lizzit, ... Journal of Materials Chemistry A 10, 14594-14603 2022
Ultrafast electronic linewidth broadening in the C core level of graphene D Curcio, S Pakdel, K Volckaert, JA Miwa, S Ulstrup, N Lanat, M Bianchi, ... Physical Review B 104 (16), L161104 2021
Spectroscopic view of ultrafast charge carrier dynamics in single-and bilayer transition metal dichalcogenide semiconductors P Majchrzak, K Volckaert, AG Čabo, D Biswas, M Bianchi, SK Mahatha, ... Journal of Electron Spectroscopy and Related Phenomena 250, 147093 2021
Atomic undercoordination in Ag islands on Ru (0001) grown via size-selected cluster deposition: an experimental and theoretical high-resolution core-level photoemission study L Sbuelz, F Loi, M Pozzo, L Bignardi, E Nicolini, P Lacovig, E Tosi, S Lizzit, ... The Journal of Physical Chemistry C 125 (17), 9556-9563 2021
Unusual reversibility in molecular break-up of PAHs: the case of pentacene dehydrogenation on Ir (111)(vol 12, pg 170, 2021) D Curcio, E Sierda, M Pozzo, L Bignardi, L Sbuelz, P Lacovig, S Lizzit, ... CHEMICAL SCIENCE 12 (2), 813-813 2021
MOST CITED SCHOLAR PUBLICATIONS
Comparing graphene growth on Cu (111) versus oxidized Cu (111) S Gottardi, K Müller, L Bignardi, JC Moreno-López, TA Pham, ... Nano letters 15 (2), 917-922 2015 Citations: 133
Epitaxial growth of single-orientation high-quality MoS2 monolayers H Bana, E Travaglia, L Bignardi, P Lacovig, CE Sanders, M Dendzik, ... 2D Materials 5 (3), 035012 2018 Citations: 83
Novel single-layer vanadium sulphide phases F Arnold, RM Stan, SK Mahatha, HE Lund, D Curcio, M Dendzik, H Bana, ... 2D Materials 5 (4), 045009 2018 Citations: 60
80% Valley Polarization of Free Carriers in Singly Oriented Single-Layer on Au(111) H Beyer, G Rohde, A Grubišić Čabo, A Stange, T Jacobsen, L Bignardi, ... Physical review letters 123 (23), 236802 2019 Citations: 44
Spin Structure of Valleys in Single-Layer on Au(111) P Eickholt, C Sanders, M Dendzik, L Bignardi, D Lizzit, S Lizzit, A Bruix, ... Physical review letters 121 (13), 136402 2018 Citations: 37
Free surfaces recast superconductivity in few-monolayer MgB2: Combined first-principles and ARPES demonstration J Bekaert, L Bignardi, A Aperis, P Van Abswoude, C Mattevi, S Gorovikov, ... Scientific reports 7 (1), 14458 2017 Citations: 37
Strain Lattice Imprinting in Graphene by C60 Intercalation at the Graphene/Cu Interface E Monazami, L Bignardi, P Rudolf, P Reinke Nano letters 15 (11), 7421-7430 2015 Citations: 33
Exciting H2 Molecules for Graphene Functionalization L Kyhl, R Bisson, R Balog, MN Groves, EL Kolsbjerg, AM Cassidy, ... ACS nano 12 (1), 513-520 2017 Citations: 31
Spin-dependent electron-phonon coupling in the valence band of single-layer NF Hinsche, AS Ngankeu, K Guilloy, SK Mahatha, A Grubišić Čabo, ... Physical Review B 96 (12), 121402 2017 Citations: 31
Key role of rotated domains in oxygen intercalation at graphene on Ni (1 1 1) L Bignardi, P Lacovig, MM Dalmiglio, F Orlando, A Ghafari, L Petaccia, ... 2D Materials 4 (2), 025106 2017 Citations: 31
Growth and structure of singly oriented single-layer tungsten disulfide on Au (111) L Bignardi, D Lizzit, H Bana, E Travaglia, P Lacovig, CE Sanders, ... Physical Review Materials 3 (1), 014003 2019 Citations: 30
Ultrafast electronic linewidth broadening in the C core level of graphene D Curcio, S Pakdel, K Volckaert, JA Miwa, S Ulstrup, N Lanat, M Bianchi, ... Physical Review B 104 (16), L161104 2021 Citations: 28
Photoemission investigation of oxygen intercalated epitaxial graphene on Ru (0001) S Ulstrup, P Lacovig, F Orlando, D Lizzit, L Bignardi, M Dalmiglio, ... Surface Science 678, 57-64 2018 Citations: 27
Graphene growth by molecular beam epitaxy: an interplay between desorption, diffusion and intercalation of elemental C species on islands F Presel, H Tetlow, L Bignardi, P Lacovig, CA Tache, S Lizzit, ... Nanoscale 10 (16), 7396-7406 2018 Citations: 24
Dual-route hydrogenation of the graphene/Ni interface D Lizzit, MI Trioni, L Bignardi, P Lacovig, S Lizzit, R Martinazzo, ... ACS nano 13 (2), 1828-1838 2019 Citations: 20
Facing the interaction of adsorbed silicon nano-ribbons on silver P Espeter, C Keutner, P Roese, K Shamout, U Berges, G Wenzel, ... Nanotechnology 28 (45), 455701 2017 Citations: 19
Nature of the surface states at the single-layer graphene/Cu (111) and graphene/polycrystalline-Cu interfaces S Pagliara, S Tognolini, L Bignardi, G Galimberti, S Achilli, MI Trioni, ... Physical Review B 91 (19), 195440 2015 Citations: 19
Layer and orbital interference effects in photoemission from transition metal dichalcogenides H Rostami, K Volckaert, N Lanata, SK Mahatha, CE Sanders, M Bianchi, ... Physical Review B 100 (23), 235423 2019 Citations: 18
The adsorption of silicon on an iridium surface ruling out silicene growth M Satta, P Lacovig, N Apostol, M Dalmiglio, F Orlando, L Bignardi, H Bana, ... Nanoscale 10 (15), 7085-7094 2018 Citations: 18
Momentum-resolved linear dichroism in bilayer K Volckaert, H Rostami, D Biswas, I Marković, F Andreatta, CE Sanders, ... Physical Review B 100 (24), 241406 2019 Citations: 17