ABSTRACT
The performance of time-resolved photoemission experiments at fs-pulsed photon sources is ultimately limited by the e-e Coulomb interaction, downgrading energy and momentum resolution. Here, we present an approach to effectively suppress space-charge artifacts in momentum microscopes and photoemission microscopes. A retarding electrostatic field generated by a special objective lens repels slow electrons, retaining the k-image of the fast photoelectrons. The suppression of space-charge effects scales with the ratio of the photoelectron velocities of fast and slow electrons. Fields in the range from -20 to -1100 V/mm for Ekin = 100 eV to 4 keV direct secondaries and pump-induced slow electrons back to the sample surface. Ray tracing simulations reveal that this happens within the first 40 to 3 µm above the sample surface for Ekin = 100 eV to 4 keV. An optimized front-lens design allows switching between the conventional accelerating and the new retarding mode. Time-resolved experiments at Ekin = 107 eV using fs extreme ultraviolet probe pulses from the free-electron laser FLASH reveal that the width of the Fermi edge increases by just 30 meV at an incident pump fluence of 22 mJ/cm2 (retarding field -21 V/mm). For an accelerating field of +2 kV/mm and a pump fluence of only 5 mJ/cm2, it increases by 0.5 eV (pump wavelength 1030 nm). At the given conditions, the suppression mode permits increasing the slow-electron yield by three to four orders of magnitude. The feasibility of the method at high energies is demonstrated without a pump beam at Ekin = 3830 eV using hard x rays from the storage ring PETRA III. The approach opens up a previously inaccessible regime of pump fluences for photoemission experiments.
ABSTRACT
Understanding of charge-density wave (CDW) phases is a main challenge in condensed matter due to their presence in high-Tc superconductors or transition metal dichalcogenides (TMDs). Among TMDs, the origin of the CDW in VSe2 remains highly debated. Here, by means of inelastic x-ray scattering and first-principles calculations, we show that the CDW transition is driven by the collapse at 110 K of an acoustic mode at qCDW = (2.25 0 0.7) r.l.u. The softening starts below 225 K and expands over a wide region of the Brillouin zone, identifying the electron-phonon interaction as the driving force of the CDW. This is supported by our calculations that determine a large momentum-dependence of the electron-phonon matrix-elements that peak at the CDW wave vector. Our first-principles anharmonic calculations reproduce the temperature dependence of the soft mode and the TCDW onset only when considering the out-of-plane van der Waals interactions, which reveal crucial for the melting of the CDW phase.
ABSTRACT
Topological surface states usually emerge at the boundary between a topological and a conventional insulator. Their precise physical character and spatial localization depend on the complex interplay between the chemical, structural and electronic properties of the two insulators in contact. Using a lattice-matched heterointerface of single and double bilayers of ß-antimonene and bismuth selenide, we perform a comprehensive experimental and theoretical study of the chiral surface states by means of microscopy and spectroscopic measurements complemented by first-principles calculations. We demonstrate that, although ß-antimonene is a trivial insulator in its free-standing form, it inherits the unique symmetry-protected spin texture from the substrate via a proximity effect that induces outward migration of the topological state. This "topologization" of ß-antimonene is found to be driven by the hybridization of the bands from either side of the interface.
ABSTRACT
Using angle-resolved photoelectron spectroscopy, we compare the electronic band structure of an ultrathin (1.8 nm) δ-layer of boron-doped diamond with a bulk-like boron doped diamond film (3 µm). Surprisingly, the measurements indicate that except for a small change in the effective mass, there is no significant difference between the electronic structure of these samples, irrespective of their physical dimensionality, except for a small modification of the effective mass. While this suggests that, at the current time, it is not possible to fabricate boron-doped diamond structures with quantum properties, it also means that nanoscale boron doped diamond structures can be fabricated which retain the classical electronic properties of bulk-doped diamond, without a need to consider the influence of quantum confinement.
ABSTRACT
We report a study of the interface between antimony and the prototypical topological insulator Bi2Se3. Scanning tunnelling microscopy measurements show the presence of ordered domains displaying a perfect lattice match with bismuth selenide. Density functional theory calculations of the most stable atomic configurations demonstrate that the ordered domains can be attributed to stacks of ß-antimonene.
ABSTRACT
The surface electronic structure of Si(1 1 1)-[Formula: see text] has been studied by angle-resolved photo electron spectroscopy. Replicas of the S 1 surface state are found in correspondence with several [Formula: see text] unit cells in the reciprocal space. This observation resolves in a direct way the long-standing dichotomy between the structural and electronic properties of the system previously discussed on the basis of the [Formula: see text] or [Formula: see text] R30° surface models.
ABSTRACT
An interface electron state at the junction between a three-dimensional topological insulator film, Bi2Se3, and a ferrimagnetic insulator film, Y3Fe5O12 (YIG), was investigated by measurements of angle-resolved photoelectron spectroscopy and x-ray absorption magnetic circular dichroism. The surface state of the Bi2Se3 film was directly observed and localized 3d spin states of the Fe3+ in the YIG film were confirmed. The proximity effect is likely described in terms of the exchange interaction between the localized Fe 3d electrons in the YIG film and delocalized electrons of the surface and bulk states in the Bi2Se3 film.
ABSTRACT
In-plane dispersions of quantum well (QW) states originating from the electron confinement of Ag sp electrons within the MoS(2) band gap region are investigated by means of angle-resolved photoemission spectroscopy (ARPES). A number of QW resonances have been observed in the ARPES spectra in a binding energy range lying outside the MoS(2) energy gap which is required for full confinement of the Ag sp electrons. In spite of having the expected free electron-like behavior, these QW states show a significant increase of in-plane effective mass with increasing binding energy due to the hybridization of Ag sp electrons with the MoS(2) valence bands. The binding energy dependence of the bottom of the QW states (k(//) = 0) as a function of the Ag film thickness has been analyzed. The well-established phase accumulation model has been applied for calculating the phase shifts of electrons at the boundaries. Our observations show that the total phase shift behaves differently for energies above and below the MoS(2) valence band maxima, due to the hybridizations being different in nature. The structure plot calculated considering the different quantum number dependent total phase shifts provides a good description of the experimental observations.
ABSTRACT
Angle-resolved photoemission spectroscopy (ARPES) and ab initio band structure calculations have been used to study the detailed valence band structure of molybdenite, MoS(2) and MoSe(2). The experimental band structure obtained from ARPES has been found to be in good agreement with the theoretical calculations performed using the linear augmented plane wave (LAPW) method. In going from MoS(2) to MoSe(2), the dispersion of the valence bands decreases along both k(parallel) and k(perpendicular), revealing the increased two-dimensional character which is attributed to the increasing interlayer distance or c/a ratio in these compounds. The width of the valence band and the band gap are also found to decrease, whereas the valence band maxima shift towards the higher binding energy from MoS(2) to MoSe(2).
ABSTRACT
We study the observed inhomogeneous band bending effects on cleaved MoS(2)(0001) single-crystal surfaces. Both Mo 3d and S 2p core levels were found to shift to lower binding energy in regions of the MoS(2) crystal with high step densities, as suggested by spot splitting of the LEED (low energy electron diffraction) pattern. Surface electronic band structure measurements also reveal a rigid shift of the valence bands in these regions, resulting from local Fermi level pinning effects. A surface electric field gradient on the MoS(2) crystals caused by the charged dislocations from the regions of high step densities generated by the cleaving process is found to explain most of the experimental observations.