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1.
ACS Nano ; 2020 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-31971774

RESUMO

Two-dimensional (2D) Dirac-like electron gases have attracted tremendous research interest ever since the discovery of free-standing graphene. The linear energy dispersion and nontrivial Berry phase play a pivotal role in the electronic, optical, mechanical, and chemical properties of 2D Dirac materials. The known 2D Dirac materials are gapless only within certain approximations, for example, in the absence of spin-orbit coupling (SOC). Here, we report a route to establishing robust Dirac cones in 2D materials with nonsymmorphic crystal lattice. The nonsymmorphic symmetry enforces Dirac-like band dispersions around certain high-symmetry momenta in the presence of SOC. Through µ-ARPES measurements, we observe Dirac-like band dispersions in α-bismuthene. The nonsymmorphic lattice symmetry is confirmed by µ-low-energy electron diffraction and scanning tunneling microscopy. Our first-principles simulations and theoretical topological analysis demonstrate the correspondence between nonsymmorphic symmetry and Dirac states. This mechanism can be straightforwardly generalized to other nonsymmorphic materials. The results enlighten the search of symmetry-enforced Dirac fermions in the vast uncharted world of nonsymmorphic 2D materials.

2.
Nano Lett ; 19(10): 7013-7020, 2019 10 09.
Artigo em Inglês | MEDLINE | ID: mdl-31461291

RESUMO

The optimization of nonlinear optical processes on the nanoscale is a crucial step for the integration of complex functionalities into compact photonic devices and metasurfaces. In such systems, photon upconversion can be achieved with higher efficiencies via third-order processes, such as third-harmonic generation (THG), thanks to the resonantly enhanced volume currents. Conversely, second-order processes, such as second-harmonic generation (SHG), are often inhibited by the symmetry of metal lattices and of common nanoantenna geometries. SHG and THG processes in plasmonic nanostructures are generally treated independently because they typically represent small perturbations in the light-matter interaction mechanisms. In this work, we demonstrate that this paradigm does not hold for plasmon-enhanced nonlinear optics by providing evidence of a sum-frequency generation (SFG) process seeded by SHG, which sizably contributes to the overall THG yield. We address this mechanism by unveiling a characteristic fingerprint in the polarization state of the THG emission from gold noncentrosymmetric nanoantennas, which directly reflects the asymmetric distribution of second-harmonic fields within the structure and does not depend on the model one employs to describe photon upconversion. We suggest that such cascaded processes may also appear for structures that exhibit only moderate SHG yields. The presence of this peculiar mechanism in THG from plasmonic nanoantennas at telecommunication wavelengths allows us to gain further insight into the physics of plasmon-enhanced nonlinear optical processes. This could be crucial in the realization of nanoscale elements for photon conversion and manipulation operating at room temperature.

3.
Ultramicroscopy ; 202: 10-17, 2019 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-30928638

RESUMO

We report on a simple and cost-effective device for high-speed gating in photoemission electron microscopy (PEEM) with pulsed photon sources. This device is based on miniaturized electrode plates, which deflect the photoelectron beam inside the imaging column of the microscope so that it is either accepted or blocked in its path towards the detector. The gating device is optimized for installation on the Elmitec SPELEEM III microscope. Due to the compact design, it can be driven by voltage pulses of low amplitude (few volts), delivered by commercially available signal generators. Most notably, our device allows for stroboscopic data collection with on-time of less than 10 ns and at a rate in the range from 1 MHz to 250 MHz, making it suitable for usage in both hybrid and standard multi-bunch operation of the synchrotron ring. We demonstrate applications of pump-probe imaging at high lateral resolution, namely magnetic imaging and PEEM imaging of surface acoustic waves.

4.
Nano Lett ; 19(1): 54-60, 2019 01 09.
Artigo em Inglês | MEDLINE | ID: mdl-30241437

RESUMO

Point defects such as oxygen vacancies cause emergent phenomena such as resistive switching in transition-metal oxides, but their influence on the electron-transport properties is far from being understood. Here, we employ direct mapping of the electronic structure of a memristive device by spectromicroscopy. We find that oxygen vacancies result in in-gap states that we use as input for single-band transport simulations. Because the in-gap states are situated below the Fermi level, they do not contribute to the current directly but impact the shape of the conduction band. Accordingly, we can describe our devices with band-like transport and tunneling across the Schottky barrier at the interface.

5.
ACS Nano ; 13(1): 526-535, 2019 Jan 22.
Artigo em Inglês | MEDLINE | ID: mdl-30525448

RESUMO

The mechanism of few-layer graphene growth on the technologically relevant cubic-SiC/Si(001) substrate is uncovered using high-resolution core-level and angle-resolved photoelectron spectroscopy, low-energy electron microscopy, and microspot low-energy electron diffraction. The thickness of the graphitic overlayer supported on the silicon carbide substrate and related changes in the surface structure are precisely controlled by monitoring the progress of the surface graphitization in situ during high-temperature graphene synthesis, using a combination of microspectroscopic techniques. The experimental data reveal gradual changes in the preferential graphene lattice orientations at the initial stages of the few-layer graphene growth on SiC(001) and can act as reference data for controllable growth of single-, double-, and triple-layer graphene on silicon carbide substrates.

6.
Nano Lett ; 18(11): 6750-6755, 2018 11 14.
Artigo em Inglês | MEDLINE | ID: mdl-30277790

RESUMO

We demonstrate the shaping of the second-harmonic (SH) radiation pattern from a single AlGaAs nanodisk antenna using coplanar holographic gratings. The SH radiation emitted from the antenna toward the-otherwise forbidden-normal direction can be effectively redirected by suitably shifting the phase of the grating pattern in the azimuthal direction. The use of such gratings allows increasing the SH power collection efficiency by 2 orders of magnitude with respect to an isolated antenna and demonstrates the possibility of intensity-tailoring for an arbitrary collection angle. Such reconstruction of the nonlinear emission from nanoscale antennas represents the first step toward the application of all-dielectric nanostructures for nonlinear holography.

7.
Beilstein J Nanotechnol ; 9: 2306-2314, 2018.
Artigo em Inglês | MEDLINE | ID: mdl-30202699

RESUMO

Background: Dielectric nanoantennas have recently emerged as an alternative solution to plasmonics for nonlinear light manipulation at the nanoscale, thanks to the magnetic and electric resonances, the strong nonlinearities, and the low ohmic losses characterizing high refractive-index materials in the visible/near-infrared (NIR) region of the spectrum. In this frame, AlGaAs nanoantennas demonstrated to be extremely efficient sources of second harmonic radiation. In particular, the nonlinear polarization of an optical system pumped at the anapole mode can be potentially boosted, due to both the strong dip in the scattering spectrum and the near-field enhancement, which are characteristic of this mode. Plasmonic nanostructures, on the other hand, remain the most promising solution to achieve strong local field confinement, especially in the NIR, where metals such as gold display relatively low losses. Results: We present a nonlinear hybrid antenna based on an AlGaAs nanopillar surrounded by a gold ring, which merges in a single platform the strong field confinement typically produced by plasmonic antennas with the high nonlinearity and low loss characteristics of dielectric nanoantennas. This platform allows enhancing the coupling of light to the nanopillar at coincidence with the anapole mode, hence boosting both second- and third-harmonic generation conversion efficiencies. More than one order of magnitude enhancement factors are measured for both processes with respect to the isolated structure. Conclusion: The present results reveal the possibility to achieve tuneable metamixers and higher resolution in nonlinear sensing and spectroscopy, by means of improved both pump coupling and emission efficiency due to the excitation of the anapole mode enhanced by the plasmonic nanoantenna.

8.
ACS Appl Mater Interfaces ; 10(32): 27178-27187, 2018 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-30019889

RESUMO

We report on the proof of principle of a scalable method for writing the magnetic state by electron-stimulated molecular dissociative adsorption on ultrathin Co on Re(0001). Intense microfocused low-energy electron beams are used to promote the formation of surface carbides and graphitic carbon through the fragmentation of carbon monoxide. Upon annealing at the CO desorption temperature, carbon persists in the irradiated areas, whereas the clean surface is recovered elsewhere, giving origin to chemical patterns with nanometer-sharp edges. The accumulation of carbon is found to induce an in-plane to out-of-plane spin reorientation transition in Co, manifested by the appearance of striped magnetic domains. Irradiation at doses in excess of 1000 L of CO followed by ultrahigh vacuum annealing at 380 °C determines the formation of a graphitic overlayer in the irradiated areas, under which Co exhibits out-of-plane magnetic anisotropy. Domains with opposite magnetization are separated here by chiral Neél walls. Our fabrication protocol adds lateral control to spin reorientation transitions, permitting to tune the magnetic anisotropy within arbitrary regions of mesoscopic size. We envisage applications in the nano-engineering of graphene-spaced stacks exhibiting the desired magnetic state and properties.

9.
J Phys Chem Lett ; 9(10): 2523-2531, 2018 May 17.
Artigo em Inglês | MEDLINE | ID: mdl-29688019

RESUMO

In crystal growth, surfactants are additive molecules used in dilute amount or as dense, permeable layers to control surface morphologies. We investigate the properties of a strikingly different surfactant: a 2D and covalent layer with close atomic packing, graphene. Using in situ, real-time electron microscopy, scanning tunneling microscopy, kinetic Monte Carlo simulations, and continuum mechanics calculations, we reveal why metallic atomic layers can grow in a 2D manner below an impermeable graphene membrane. Upon metal growth, graphene dynamically opens nanochannels called wrinkles, facilitating mass transport while at the same time storing and releasing elastic energy via lattice distortions. Graphene thus behaves as a mechanically active, deformable surfactant. The wrinkle-driven mass transport of the metallic layer intercalated between graphene and the substrate is observed for two graphene-based systems, characterized by different physicochemical interactions, between graphene and the substrate and between the intercalated material and graphene. The deformable surfactant character of graphene that we unveil should then apply to a broad variety of species, opening new avenues for using graphene as a 2D surfactant forcing the growth of flat films, nanostructures, and unconventional crystalline phases.

10.
Int J Mol Sci ; 19(4)2018 Apr 06.
Artigo em Inglês | MEDLINE | ID: mdl-29642415

RESUMO

Biallelic mutations in RECQL4 gene, a caretaker of the genome, cause Rothmund-Thomson type-II syndrome (RTS-II) and confer increased cancer risk if they damage the helicase domain. We describe five families exemplifying clinical and allelic heterogeneity of RTS-II, and report the effect of pathogenic RECQL4 variants by in silico predictions and transcripts analyses. Complete phenotype of patients #39 and #42 whose affected siblings developed osteosarcoma correlates with their c.[1048_1049del], c.[1878+32_1878+55del] and c.[1568G>C;1573delT], c.[3021_3022del] variants which damage the helicase domain. Literature survey highlights enrichment of these variants affecting the helicase domain in patients with cancer outcome raising the issue of strict oncological surveillance. Conversely, patients #29 and #19 have a mild phenotype and carry, respectively, the unreported homozygous c.3265G>T and c.3054A>G variants, both sparing the helicase domain. Finally, despite matching several criteria for RTS clinical diagnosis, patient #38 is heterozygous for c.2412_2414del; no pathogenic CNVs out of those evidenced by high-resolution CGH-array, emerged as contributors to her phenotype.


Assuntos
Mutação , Fenótipo , Síndrome de Rothmund-Thomson/genética , Adolescente , Adulto , Linhagem Celular Tumoral , Criança , Feminino , Homozigoto , Humanos , Masculino , Linhagem , RecQ Helicases/genética , RecQ Helicases/metabolismo , Síndrome de Rothmund-Thomson/patologia
11.
Nanoscale ; 9(42): 16412-16419, 2017 Nov 02.
Artigo em Inglês | MEDLINE | ID: mdl-29058741

RESUMO

This work reports an electronic and micro-structural study of an appealing system for optoelectronics: tungsten disulfide (WS2) on epitaxial graphene (EG) on SiC(0001). The WS2 is grown via chemical vapor deposition (CVD) onto the EG. Low-energy electron diffraction (LEED) measurements assign the zero-degree orientation as the preferential azimuthal alignment for WS2/EG. The valence-band (VB) structure emerging from this alignment is investigated by means of photoelectron spectroscopy measurements, with both high space and energy resolution. We find that the spin-orbit splitting of monolayer WS2 on graphene is of 462 meV, larger than what is reported to date for other substrates. We determine the value of the work function for the WS2/EG to be 4.5 ± 0.1 eV. A large shift of the WS2 VB maximum is observed as well, due to the lowering of the WS2 work function caused by the donor-like interfacial states of EG. Density functional theory (DFT) calculations carried out on a coincidence supercell confirm the experimental band structure to an excellent degree. X-ray photoemission electron microscopy (XPEEM) measurements performed on single WS2 crystals confirm the van der Waals nature of the interface coupling between the two layers. In virtue of its band alignment and large spin-orbit splitting, this system gains strong appeal for optical spin-injection experiments and opto-spintronic applications in general.

13.
ACS Nano ; 11(7): 6921-6929, 2017 07 25.
Artigo em Inglês | MEDLINE | ID: mdl-28661649

RESUMO

A major obstacle for the implementation of redox-based memristive memory or logic technology is the large cycle-to-cycle and device-to-device variability. Here, we use spectromicroscopic photoemission threshold analysis and operando XAS analysis to experimentally investigate the microscopic origin of the variability. We find that some devices exhibit variations in the shape of the conductive filament or in the oxygen vacancy distribution at and around the filament. In other cases, even the location of the active filament changes from one cycle to the next. We propose that both effects originate from the coexistence of multiple (sub)filaments and that the active, current-carrying filament may change from cycle to cycle. These findings account for the observed variability in device performance and represent the scientific basis, rather than prior purely empirical engineering approaches, for developing stable memristive devices.

14.
Nanoscale ; 8(20): 10849-56, 2016 May 19.
Artigo em Inglês | MEDLINE | ID: mdl-27165117

RESUMO

We have studied (001) surface terminated cerium oxide nanoparticles grown on a ruthenium substrate using physical vapor deposition. Their morphology, shape, crystal structure, and chemical state are determined by low-energy electron microscopy and micro-diffraction, scanning probe microscopy, and synchrotron-based X-ray absorption spectroscopy. Square islands are identified as CeO2 nanocrystals exhibiting a (001) oriented top facet of varying size; they have a height of about 7 to 10 nm and a side length between about 50 and 500 nm, and are terminated with a p(2 × 2) surface reconstruction. Micro-illumination electron diffraction reveals the existence of a coincidence lattice at the interface to the ruthenium substrate. The orientation of the side facets of the rod-like particles is identified as (111); the square particles are most likely of cuboidal shape, exhibiting (100) oriented side facets. The square and needle-like islands are predominantly found at step bunches and may be grown exclusively at temperatures exceeding 1000 °C.

15.
Nat Commun ; 7: 11446, 2016 05 13.
Artigo em Inglês | MEDLINE | ID: mdl-27173154

RESUMO

Geometrical frustration in magnetic materials often gives rise to exotic, low-temperature states of matter, such as the ones observed in spin ices. Here we report the imaging of the magnetic states of a thermally active artificial magnetic ice that reveal the fingerprints of a spin fragmentation process. This fragmentation corresponds to a splitting of the magnetic degree of freedom into two channels and is evidenced in both real and reciprocal space. Furthermore, the internal organization of both channels is interpreted within the framework of a hybrid spin-charge model that directly emerges from the parent spin model of the kagome dipolar spin ice. Our experimental and theoretical results provide insights into the physics of frustrated magnets and deepen our understanding of emergent fields through the use of tailor-made magnetism.

16.
Opt Lett ; 41(3): 480-3, 2016 Feb 01.
Artigo em Inglês | MEDLINE | ID: mdl-26907402

RESUMO

We describe the coupling dynamics of one-dimensional surface plasmon polaritons supported by a pair of hetero-junctions between two-dimensional media. We first discuss the unique symmetry properties of the supermodes of such structures, and then we exploit the possibility of electrically tuning the conductivity of graphene to demonstrate tailoring and manipulation of light propagation in a graphene/graphene platform.

17.
Nat Nanotechnol ; 11(5): 449-54, 2016 05.
Artigo em Inglês | MEDLINE | ID: mdl-26809057

RESUMO

Magnetic skyrmions are chiral spin structures with a whirling configuration. Their topological properties, nanometre size and the fact that they can be moved by small current densities have opened a new paradigm for the manipulation of magnetization at the nanoscale. Chiral skyrmion structures have so far been experimentally demonstrated only in bulk materials and in epitaxial ultrathin films, and under an external magnetic field or at low temperature. Here, we report on the observation of stable skyrmions in sputtered ultrathin Pt/Co/MgO nanostructures at room temperature and zero external magnetic field. We use high lateral resolution X-ray magnetic circular dichroism microscopy to image their chiral Néel internal structure, which we explain as due to the large strength of the Dzyaloshinskii-Moriya interaction as revealed by spin wave spectroscopy measurements. Our results are substantiated by micromagnetic simulations and numerical models, which allow the identification of the physical mechanisms governing the size and stability of the skyrmions.

18.
Sci Rep ; 6: 19734, 2016 Jan 25.
Artigo em Inglês | MEDLINE | ID: mdl-26804138

RESUMO

Control over the film-substrate interaction is key to the exploitation of graphene's unique electronic properties. Typically, a buffer layer is irreversibly intercalated "from above" to ensure decoupling. For graphene/Ni(111) we instead tune the film interaction "from below". By temperature controlling the formation/dissolution of a carbide layer under rotated graphene domains, we reversibly switch graphene's electronic structure from semi-metallic to metallic. Our results are relevant for the design of controllable graphene/metal interfaces in functional devices.

19.
Small ; 11(44): 5927-31, 2015 Nov 25.
Artigo em Inglês | MEDLINE | ID: mdl-26439586

RESUMO

Substitutional doping in graphene is locally induced with very low energy nitrogen ions. Irradiated and nonirradiated areas exhibit different charge carrier densities and are separated by a sharp boundary, stable up to 750 °C. The way towards lithographic control of the electronic properties of graphene by ion irradiation is paved, providing a proof of principle for the fabrication of 2D graphene-based heterojunctions.

20.
Phys Rev Lett ; 115(13): 136102, 2015 Sep 25.
Artigo em Inglês | MEDLINE | ID: mdl-26451569

RESUMO

In catalytic methanol oxidation on ultrathin vanadium oxide layers on Rh(111) (Θ_{V}≈0.2 monolayer equivalent) we observe a 2D ripening of the VO_{x} islands that is controlled by the catalytic reaction. Neighboring VO_{x} islands move under reaction conditions towards each other and coalesce. The motion and the coalescence of the islands are explained by a polymerization-depolymerization equilibrium that is sensitive to gradients in the adsorbate coverages.

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