The momentum-dependent orbital character in crystalline solids, referred to as orbital texture, is of capital importance in the emergence of symmetry-broken collective phases, such as charge density waves as well as superconducting and topological states of matter. By performing extreme ultraviolet multidimensional angle-resolved photoemission spectroscopy for two different crystal orientations linked to each other by mirror symmetry, we isolate and identify the role of orbital texture in photoemission from the transition metal dichalcogenide 1T-TiTe2. By comparing our experimental results with theoretical calculations based on both a quantitative one-step model of photoemission and an intuitive tight-binding model, we unambiguously demonstrate the link between the momentum-dependent orbital orientation and the emergence of strong intrinsic linear dichroism in the photoelectron angular distributions. Our results represent an important step towards going beyond band structure (eigenvalues) mapping and learning about electronic wavefunction and orbital texture of solids by exploiting matrix element effects in photoemission spectroscopy.
We combined a spin-resolved photoemission spectrometer with a high-harmonic generation (HHG) laser source in order to perform spin-, time-and angle-resolved photoemission spectroscopy (STARPES) experiments on the transition metal dichalcogenide bulk WTe2, a possible Weyl type-II semimetal. Measurements at different femtosecond pump-probe delays and comparison with spinresolved one-step photoemission calculations provide insight into the spin polarization of electrons above the Fermi level in the region where Weyl points of WTe2 are expected. We observe a spin accumulation above the Weyl points region, that is consistent with a spin-selective bottleneck effect due to the presence of spin polarized cone-like electronic structure. Our results support the feasibility of STARPES with HHG, which despite being experimentally challenging provides a unique way to study spin dynamics in photoemission. :1912.06572v1 [cond-mat.mtrl-sci]
arXiv
The dosing of layered materials with alkali metals has become a commonly used strategy in ARPES experiments. However, precisely what occurs under such conditions, both structurally and electronically, has remained a matter of debate. Here we perform a systematic study of 1T-HfTe 2 , a prototypical semimetal of the transition metal dichalcogenide family. By utilizing photon energy-dependent angle-resolved photoemission spectroscopy (ARPES), we have investigated the electronic structure of this material as a function of potassium (K) deposition. From the k z maps, we observe the appearance of 2D dispersive bands after electron dosing, with an increasing sharpness of the bands, consistent with the wave-function confinement at the topmost layer. In our highest-dosing cases, a monolayerlike electronic structure emerges, presumably as a result of intercalation of the alkali metal. Here, by bringing the topmost valence band below E F , we can directly measure a band overlap of ∼0.2 eV. However, 3D bulklike states still contribute to the spectra even after considerable dosing. Our work provides a reference point for the increasingly popular studies of the alkali metal dosing of semimetals using ARPES.
The layered two-dimensional material MoTe 2 in the T d crystal phase is a semimetal which has theoretically been predicted to possess topologically nontrivial bands corresponding to Weyl fermions. Clear experimental evidence by angle-resolved photoemission spectroscopy (ARPES) is, however, lacking, which calls for a careful examination of the relation between ground state band structure calculations and ARPES intensity plots. Here we report a study of the near-Fermi-energy band structure of MoTe 2 (T d ) by means of ARPES measurements, density functional theory, and one-step-model ARPES calculations. Good agreement between theory and experiment is obtained. We analyze the orbital character of the surface bands and its relation to the ARPES polarization dependence. We find that light polarization has a major effect on which bands can be observed by ARPES. For s-polarized light, the ARPES intensity is dominated by subsurface Mo d orbitals, while p-polarized light reveals the bands mainly derived from Te p orbitals. Suitable light polarization for observing either an electron or hole pocket are determined.
High-power impulse magnetron sputtering of a Ta target in precisely controlled Ar+O2+N2 gas mixtures was used to prepare amorphous N-rich tantalum oxynitride (Ta–O–N) films with a finely varied elemental composition. Postdeposition annealing of the films at 900°C for 5 min in vacuum led to their crystallization without any significant change in the elemental composition. The authors show that this approach allows preparation of a Ta–O–N film with a dominant Ta2N2O phase of the bixbyite structure. As far as the authors know, this phase has been neither experimentally nor theoretically reported yet. The film exhibits semiconducting properties characterized by two electrical (indirect or selection-rule forbidden) bandgaps of about 0.2 and 1.0 eV and one optical (direct and selection-rule allowed) bandgap of 2.0 eV (suitable for visible-light absorption up to 620 nm). This observation is in good agreement with the carried out ab initio calculations and the experimental data obtained by soft and hard X-ray photoelectron spectroscopy. Furthermore, the optical bandgap is appropriately positioned with respect to the redox potentials for water splitting, which makes this material an interesting candidate for this application.
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