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1.
Nat Mater ; 23(10): 1339-1346, 2024 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-39191980

RESUMO

Most two-dimensional (2D) materials experimentally studied so far have hexagons as their building blocks. Only a few exceptions, such as PdSe2, are lower in energy in pentagonal phases and exhibit pentagons as building blocks. Although theory has predicted a large number of pentagonal 2D materials, many of these are metastable and their experimental realization is difficult. Here we report the successful synthesis of a metastable pentagonal 2D material, monolayer pentagonal PdTe2, by symmetry-driven epitaxy. Scanning tunnelling microscopy and complementary spectroscopy measurements are used to characterize this material, which demonstrates well-ordered low-symmetry atomic arrangements and is stabilized by lattice matching with the underlying Pd(100) substrate. Theoretical calculations, along with angle-resolved photoemission spectroscopy, reveal monolayer pentagonal PdTe2 to be a semiconductor with an indirect bandgap of 1.05 eV. Our work opens an avenue for the synthesis of pentagon-based 2D materials and gives opportunities to explore their applications such as multifunctional nanoelectronics.

2.
Nano Lett ; 21(5): 1968-1975, 2021 Mar 10.
Artigo em Inglês | MEDLINE | ID: mdl-33600187

RESUMO

The transition-metal dichalcogenide VSe2 exhibits an increased charge density wave transition temperature and an emerging insulating phase when thinned to a single layer. Here, we investigate the interplay of electronic and lattice degrees of freedom that underpin these phases in single-layer VSe2 using ultrafast pump-probe photoemission spectroscopy. In the insulating state, we observe a light-induced closure of the energy gap, which we disentangle from the ensuing hot carrier dynamics by fitting a model spectral function to the time-dependent photoemission intensity. This procedure leads to an estimated time scale of 480 fs for the closure of the gap, which suggests that the phase transition in single-layer VSe2 is driven by electron-lattice interactions rather than by Mott-like electronic effects. The ultrafast optical switching of these interactions in SL VSe2 demonstrates the potential for controlling phase transitions in 2D materials with light.

3.
Phys Chem Chem Phys ; 23(46): 26401-26406, 2021 Dec 01.
Artigo em Inglês | MEDLINE | ID: mdl-34792074

RESUMO

The bulk band structure of the topological insulator Sb2Te3 is investigated by angle-resolved photoemission spectroscopy. Of particular interest is the dispersion of the uppermost valence band with respect to the topological surface state Dirac point. The valence band maximum has been calculated to be either near the Brillouin zone centre or in a low-symmetry position in the -M̄ azimuthal direction. In order to observe the full energy range of the valence band, the strongly p-doped crystals are counter-doped by surface alkali adsorption. The data show that the absolute valence band maximum is likely to be found at the bulk Γ point and predictions of a low-symmetry position with an energy higher than the surface Dirac point can be ruled out.

4.
Phys Chem Chem Phys ; 23(13): 7806-7813, 2021 Apr 07.
Artigo em Inglês | MEDLINE | ID: mdl-33136112

RESUMO

We present an experimental study of inelastic scattering processes on the (111) surface of the topological insulator Sb2Te3 using helium atom scattering. In contrast to other binary topological insulators such as Bi2Se3 and Bi2Te3, Sb2Te3 is much less studied and the as-grown Sb2Te3 sample turns out to be p-doped, with the Fermi-level located below the Dirac-point as confirmed by angle-resolved photoemission spectroscopy. We report the surface phonon dispersion along both high symmetry directions in the energy region below 11 meV, where the Rayleigh mode exhibits the strongest intensity. The experimental data is compared with a study based on density functional perturbation theory calculations, providing good agreement except for a set of additional peculiar inelastic events below the Rayleigh mode. In addition, an analysis of angular scans with respect to a number of additional inelastic events is presented, including resonance enhancement, kinematical focusing, focused inelastic resonance and surfing. In the latter case, phonon-assisted adsorption of the incident helium atom gives rise to a bound state where the helium atom rides the created Rayleigh wave.

5.
Pediatr Radiol ; 51(11): 2058-2068, 2021 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-34287663

RESUMO

BACKGROUND: Axonal myelination is an important maturation process in the developing brain. Increasing myelin content correlates with the longitudinal relaxation rate (R1=1/T1) in magnetic resonance imaging (MRI). OBJECTIVE: By using magnetization-prepared 2 rapid acquisition gradient echoes (MP2RAGE) on a 3-T MRI system, we provide R1 values and myelination rates for infants and young children. MATERIALS AND METHODS: Average R1 values in white and grey matter regions in 94 children without pathological MRI findings (age range: 3 months to 6 years) were measured and fitted by a saturating-exponential growth model. For comparison, R1 values of 36 children with different brain pathologies are presented. The findings were related to a qualitative evaluation using T2, magnetization-prepared rapid acquisition gradient echo (MP-RAGE) and MP2RAGE. RESULTS: R1 changes rapidly in the first 16 months of life, then much slower thereafter. R1 is highest in pre-myelinated structures in the youngest subjects, such as the posterior limb of the internal capsule (0.74-0.76±0.04 s-1) and lowest for the corpus callosum (0.37-0.44±0.03 s-1). The myelination rate is fastest in the corpus callosum and slowest in the deep grey matter. R1 is decreased in hypo- and dysmyelination disorders. Myelin maturation is clearly visible on MP2RAGE, especially in the first year of life. CONCLUSION: MP2RAGE permits a quantitative R1 mapping method with an examination time of approximately 6 min. The age-dependent R1 values for children without MRI-identified brain pathologies are well described by a saturating-exponential function with time constants depending on the investigated brain region. This model can serve as a reference for this age group and to search for indications of subtle pathologies. Moreover, the MP2RAGE sequence can also be used for the qualitative assessment of myelinated structures.


Assuntos
Encéfalo , Imageamento por Ressonância Magnética , Encéfalo/diagnóstico por imagem , Criança , Pré-Escolar , Humanos , Lactente , Neuroimagem
6.
Phys Rev Lett ; 125(9): 096401, 2020 Aug 28.
Artigo em Inglês | MEDLINE | ID: mdl-32915590

RESUMO

Time-resolved soft-x-ray photoemission spectroscopy is used to simultaneously measure the ultrafast dynamics of core-level spectral functions and excited states upon excitation of excitons in WSe_{2}. We present a many-body approximation for the Green's function, which excellently describes the transient core-hole spectral function. The relative dynamics of excited-state signal and core levels clearly show a delayed core-hole renormalization due to screening by excited quasifree carriers resulting from an excitonic Mott transition. These findings establish time-resolved core-level photoelectron spectroscopy as a sensitive probe of subtle electronic many-body interactions and ultrafast electronic phase transitions.

7.
Phys Rev Lett ; 125(23): 236403, 2020 Dec 04.
Artigo em Inglês | MEDLINE | ID: mdl-33337178

RESUMO

The presence of an electrical transport current in a material is one of the simplest and most important realizations of nonequilibrium physics. The current density breaks the crystalline symmetry and can give rise to dramatic phenomena, such as sliding charge density waves, insulator-to-metal transitions, or gap openings in topologically protected states. Almost nothing is known about how a current influences the electron spectral function, which characterizes most of the solid's electronic, optical, and chemical properties. Here we show that angle-resolved photoemission spectroscopy with a nanoscale light spot provides not only a wealth of information on local equilibrium properties, but also opens the possibility to access the local nonequilibrium spectral function in the presence of a transport current. Unifying spectroscopic and transport measurements in this way allows simultaneous noninvasive local measurements of the composition, structure, many-body effects, and carrier mobility in the presence of high current densities. In the particular case of our graphene-based device, we are able to correlate the presence of structural defects with locally reduced carrier lifetimes in the spectral function and a locally reduced mobility with a spatial resolution of 500 nm.

8.
Phys Rev Lett ; 123(21): 216403, 2019 Nov 22.
Artigo em Inglês | MEDLINE | ID: mdl-31809169

RESUMO

Electronic screening can have direct consequences for structural arrangements on the nanoscale, such as on the periodic ordering of adatoms on a surface. So far, such ordering phenomena have been explained in terms of isotropic screening of free electronlike systems. Here, we directly illustrate the structural consequences of anisotropic screening, making use of a highly anisotropic two-dimensional electron gas (2DEG) near the surface of black phosphorous. The presence of the 2DEG and its filling is controlled by adsorbed potassium atoms, which simultaneously serve to probe the electronic ordering. Using scanning tunneling microscopy, we show that the anisotropic screening leads to the formation of potassium chains with a well-defined orientation and spacing. We quantify the mean interaction potential utilizing statistical methods and find that the dimensionality and anisotropy of the screening is consistent with the presence of a band bending-induced 2DEG near the surface. The electronic dispersion of the 2DEG inferred by electronic ordering is consistent with that measured by angle-resolved photoemission spectroscopy.

9.
Phys Rev Lett ; 121(13): 136402, 2018 Sep 28.
Artigo em Inglês | MEDLINE | ID: mdl-30312046

RESUMO

The spin structure of the valence and conduction bands at the K[over ¯] and K[over ¯]^{'} valleys of single-layer WS_{2} on Au(111) is determined by spin- and angle-resolved photoemission and inverse photoemission. The bands confining the direct band gap of 1.98 eV are out-of-plane spin polarized with spin-dependent energy splittings of 417 meV in the valence band and 16 meV in the conduction band. The sequence of the spin-split bands is the same in the valence and in the conduction bands and opposite at the K[over ¯] and the K[over ¯]^{'} high-symmetry points. The first observation explains "dark" excitons discussed in optical experiments; the latter points to coupled spin and valley physics in electron transport. The experimentally observed band dispersions are discussed along with band structure calculations for a freestanding single layer and for a single layer on Au(111).

10.
Nano Lett ; 15(9): 5883-7, 2015 Sep 09.
Artigo em Inglês | MEDLINE | ID: mdl-26315566

RESUMO

The dynamics of excited electrons and holes in single layer (SL) MoS2 have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS2 on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS2. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons.

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