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1.
Langmuir ; 38(41): 12570-12580, 2022 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-36190908

RESUMO

Colloidal probe atomic force microscopy (AFM) allows us to explore sliding friction phenomena in graphite contacts of nominal lateral size up to hundreds of nanometers. It is known that contact formation involves tribo-induced material transfer of graphite flakes from the graphitic substrate to the colloidal probe. In this context, sliding states with nearly vanishing friction, i.e., superlubricity, may set in. A comprehensive investigation of the transfer layer properties is mandatory to ascertain the origin of superlubricity. Here we explore the friction response of micrometric beads, of different size and pristine surface roughness, sliding on graphite under ambient conditions. We show that such tribosystems undergo a robust transition toward a low-adhesion, low-friction state dominated by mechanical interactions at one dominant tribo-induced nanocontact. Friction force spectroscopy reveals that the nanocontact can be superlubric or dissipative, in fact undergoing a load-driven transition from dissipative stick-slip to continuous superlubric sliding. This behavior is excellently described by the thermally activated, single-asperity Prandtl-Tomlinson model. Our results indicate that upon formation of the transfer layer, friction depends on the energy landscape experienced by the topographically highest tribo-induced nanoasperity. We consistently find larger dissipation when the tribo-induced nanoasperity is slid against surfaces with higher atomic corrugation than graphite, like MoS2 and WS2, in prototypical van der Waals layered heterojunctions.

2.
Adv Mater ; 33(32): e2100593, 2021 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-34176160

RESUMO

In strongly correlated electron materials, the electronic, spin, and charge degrees of freedom are closely intertwined. This often leads to the stabilization of emergent orders that are highly sensitive to external physical stimuli promising opportunities for technological applications. In perovskite ruthenates, this sensitivity manifests in dramatic changes of the physical properties with subtle structural details of the RuO6 octahedra, stabilizing enigmatic correlated ground states, from a hotly debated superconducting state via electronic nematicity and metamagnetic quantum criticality to ferromagnetism. Here, it is demonstrated that the rotation of the RuO6 octahedra in the surface layer of Sr2 RuO4 generates new emergent orders not observed in the bulk material. Through atomic-scale spectroscopic characterization of the low-energy electronic states, four van Hove singularities are identified in the vicinity of the Fermi energy. The singularities can be directly linked to intertwined nematic and checkerboard charge order. Tuning of one of these van Hove singularities by magnetic field is demonstrated, suggesting that the surface layer undergoes a Lifshitz transition at a magnetic field of ≈32T. The results establish the surface layer of Sr2 RuO4 as an exciting 2D correlated electron system and highlight the opportunities for engineering the low-energy electronic states in these systems.

3.
ACS Appl Mater Interfaces ; 12(25): 28894-28902, 2020 Jun 24.
Artigo em Inglês | MEDLINE | ID: mdl-32482063

RESUMO

Macroscopic current-voltage measurements and nanoscopic ballistic electron emission spectroscopy (BEES) have been used to probe the Schottky barrier height (SBH) at metal/Ge(100) junctions for two metal electrodes (Au and Pt) and different metallization methods, specifically, thermal-vapor and laser-vapor deposition. Analysis of macroscopic current-voltage characteristics indicates that a SBH of 0.61-0.63 eV controls rectification at room temperature. On the other hand, BEES measured at 80 K reveals the coexistence of two distinct barriers at the nanoscale, taking values in the ranges 0.61-0.64 and 0.70-0.74 eV for the cases studied. For each metal-semiconductor junction, the macroscopic measurement agrees well with the lower barrier found with BEES. Ab initio modeling of BEES spectra ascribes the two barriers to two different atomic registries between the metals and the Ge(100) surface, a significant relevant insight for next-generation highly miniaturized Ge-based devices.

4.
Langmuir ; 34(10): 3207-3214, 2018 03 13.
Artigo em Inglês | MEDLINE | ID: mdl-29482328

RESUMO

We report high-resolution surface morphology and friction force maps of polycrystalline organic thin films derived by deposition of the n-type perylene diimide semiconductor PDI8-CN2. We show that the in-plane molecular arrangement into ordered, cofacial slip-stacked rows results in a largely anisotropic surface structure, with a characteristic sawtooth corrugation of a few Ångstroms wavelength and height. Load-controlled experiments reveal different types of friction contrast between the alternating sloped and stepped regions, with transitions from atomic-scale dissipative stick-slip to smooth sliding with ultralow friction within the surface unit cell. Notably, such a rich phenomenology is captured under ambient conditions. We demonstrate that friction contrast is well reproduced by numerical simulations assuming a reduced corrugation of the tip-molecule potential nearby the step edges. We propose that the side alkyl chains pack into a compact low-surface-energy overlayer, and friction modulation reflects periodic heterogeneity of chains bending properties and subsurface anchoring to the perylene cores.

5.
J Phys Condens Matter ; 29(48): 485002, 2017 12 06.
Artigo em Inglês | MEDLINE | ID: mdl-29120863

RESUMO

We investigate with scanning tunneling microscopy/spectroscopy (STM/STS) and density functional theory (DFT) calculations the surface structures and the electronic properties of Fe1+y Te thin films grown by pulsed laser deposition. Contrary to the regular arrangement of antiferromagnetic nanostripes previously reported on cleaved single-crystal samples, the surface of Fe1+y Te thin films displays a peculiar distribution of spatially inhomogeneous nanostripes. Both STM and DFT calculations show the bias-dependent nature of such features and support the interpretation of spin-polarized tunneling between the FeTe surface and an unintentionally magnetized tip. In addition, the spatial inhomogeneity is interpreted as a purely electronic effect related to changes in hybridization and Fe-Fe bond length driven by local variations in the concentration of excess interstitial Fe cations. Unexpectedly, the surface density of states measured by STS strongly evolves with temperature in close proximity to the antiferromagnetic-paramagnetic first-order transition, and reveals a large pseudogap of 180-250 meV at about 50-65 K. We believe that in this temperature range a phase transition takes place, and the system orders and locks into particular combinations of orbitals and spins because of the interplay between excess interstitial magnetic Fe and strongly correlated d-electrons.

6.
Chemistry ; 21(9): 3766-71, 2015 Feb 23.
Artigo em Inglês | MEDLINE | ID: mdl-25608141

RESUMO

We have investigated thin films of a perylene diimide derivative with a cyano-functionalized core (PDI-8CN2) deposited on Au(111) single crystals from the monolayer to the multilayer regime. We found that PDI-8CN2 is chemisorbed on gold. The molecules experience a thickness-dependent reorientation, and a 2D growth mode with molecular stepped terraces is achieved adopting low deposition rates. The obtained results are discussed in terms of their impact on field effect devices, also clarifying why the use of substrate/contact treatments, decoupling PDI-8CN2 molecules from the substrate/contacts, is beneficial for such devices. Our results also suggest that perylene diimide derivatives with CN bay-functionalization are very promising candidates for single-molecule electronic devices.


Assuntos
Ouro/química , Imidas/química , Nitrilas/química , Perileno/análogos & derivados , Estrutura Molecular , Nanotecnologia , Perileno/química
7.
Nat Mater ; 13(2): 173-7, 2014 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-24336340

RESUMO

Understanding nanoscale friction and dissipation is central to nanotechnology. The recent detection of the electronic-friction drop caused by the onset of superconductivity in Nb by means of an ultrasensitive non-contact pendulum atomic force microscope (AFM) raised hopes that a wider variety of mechanical-dissipation mechanisms become accessible. Here, we report a multiplet of AFM dissipation peaks arising a few nanometres above the surface of NbSe2--a layered compound exhibiting an incommensurate charge-density wave (CDW). Each peak appears at a well-defined tip-surface interaction force of the order of a nanonewton, and persists up to 70 K, where the short-range order of CDWs is known to disappear. Comparison of the measurements with a theoretical model suggests that the peaks are associated with local, tip-induced 2π phase slips of the CDW, and that dissipation maxima arise from hysteretic behaviour of the CDW phase as the tip oscillates at specific distances where sharp local slips occur.

8.
Angew Chem Int Ed Engl ; 48(26): 4845-8, 2009.
Artigo em Inglês | MEDLINE | ID: mdl-19479918

RESUMO

Sticking together: The occupation of different sites by oxygen atoms that are produced by the dissociation of O(2) on Pd(100) is determined by the initial rotational alignment of the parent molecules. The atom locations are characterized by different chemical reactivities in the reaction with CO to form CO(2) (see picture), which are followed by synchrotron radiation (SR) experiments with a supersonic molecular beam (SMB).

9.
J Phys Chem B ; 111(7): 1679-83, 2007 Feb 22.
Artigo em Inglês | MEDLINE | ID: mdl-17263572

RESUMO

We have investigated oxygen adsorption on Cu(410) by high-resolution electron energy loss spectroscopy, dosing O2 with a supersonic molecular beam at different surface temperatures and for different angles of incidence and beam energies or by backfilling. In the investigated crystal temperature range (127 < T < 570 K), adsorption is always dissociative. Depending on T, impact energy, and angle of incidence, the oxygen atoms end up in different adsorption configurations, characterized by different vibrational signatures. In particular, at grazing incidence when only the step edge is exposed to O2, the adatoms end up initially preferentially at the step edge. An ordered overlayer forms at half monolayer coverage when the adsorbate is mobile. Oxide patches develop eventually for large exposures performed by backfilling and at high crystal temperature.

11.
J Chem Phys ; 123(22): 224709, 2005 Dec 08.
Artigo em Inglês | MEDLINE | ID: mdl-16375497

RESUMO

The control of spatial orientation of molecules has a great influence on the stereodynamics of elementary processes occurring both in homogeneous and heterogeneous phases. Nonpolar molecules have so far escaped direct experimental investigations because of their poor sensitivity to several external constraints. Recently, it has been shown that the collisional alignment produced in supersonic expansions coupled with molecular-beam velocity selection can help solve such problems. Here we show that the sticking probability of ethylene, a nonpolar molecule prototypical of unsaturated hydrocarbons, on an O(2)-precovered Ag(001) surface is larger for molecules approaching in a helicopter-like motion than for those cartwheeling. A mechanism involving a weakly bound precursor state is suggested, with helicopter molecules having a lower chance of being scattered back into the gas phase than cartwheels when colliding with preadsorbed ethylene.


Assuntos
Físico-Química/métodos , Etilenos/farmacocinética , Oxigênio/química , Prata/química , Adsorção , Alcenos/química , Desenho de Equipamento , Etilenos/química , Hidrocarbonetos/química , Modelos Teóricos , Conformação Molecular , Estrutura Molecular , Estereoisomerismo , Propriedades de Superfície
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