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Maciej Dendzik

Publications and source records attributed to Maciej Dendzik.

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Spin structure of K valleys in single-layer WS$_2$ on Au(111)

The spin structure of the valence and conduction bands at the $\overline{\text{K}}$ and $\overline{\text{K}}$' 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 $\overline{\text{K}}$ and the $\overline{\text{K}}$' 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).

cond-mat.mtrl-sci↗

Growth and Structure of Singly-Oriented Single-Layer Tungsten Disulfide on Au(111)

We present a complete characterisation at the nanoscale of the growth and structure of single-layer tungsten disulfide (WS$_2$) epitaxially grown on Au(111). Following the growth process in real time with fast x-ray photoelectron spectroscopy, we obtain a singly-oriented layer by choosing the proper W evaporation rate and substrate temperature during the growth. Information about the morphology, size and layer stacking of the WS$_2$ layer were achieved by employing x-ray photoelectron diffraction and low-energy electron microscopy. The strong spin splitting in the valence band of WS$_2$ coupled with the single-orientation character of the layer make this material the ideal candidate for the exploitation of the spin and valley degrees of freedom.

cond-mat.mtrl-sci↗

Novel single-layer vanadium sulphide phases

VS2 is a challenging material to prepare stoichiometrically in the bulk, and the single layer has not been successfully isolated before now. Here we report the first realization of single-layer VS2, which we have prepared epitaxially with high quality on Au(111) in the octahedral (1T) structure. We find that we can deplete the VS2 lattice of S by annealing in vacuum so as to create an entirely new two-dimensional compound that has no bulk analogue. The transition is reversible upon annealing in an H2S gas atmosphere. We report the structural properties of both the stoichiometric and S-depleted compounds on the basis of low-energy electron diffraction, X-ray photoelectron spectroscopy and diffraction, and scanning tunneling microscopy experiments.

cond-mat.mtrl-sci↗

Epitaxial Growth of Single-Orientation High-Quality MoS$_2$ Monolayers

We present a study on the growth and characterization of high-quality single-layer MoS$_2$ with a single orientation, i.e. without the presence of mirror domains. This single orientation of the MoS$_2$ layer is established by means of x-ray photoelectron diffraction. The high quality is evidenced by combining scanning tunneling microscopy with x-ray photoelectron spectroscopy measurements. Spin- and angle-resolved photoemission experiments performed on the sample revealed complete spin-polarization of the valence band states near the K and -K points of the Brillouin zone. These findings open up the possibility to exploit the spin and valley degrees of freedom for encoding and processing information in devices that are based on epitaxially grown materials.

cond-mat.mtrl-sci↗

Contact-Induced Semiconductor-to-Metal Transition in Single-Layer WS$_2$

Low-resistance ohmic contacts are a challenge for electronic devices based on two-dimensional materials. We show that an atomically precise junction between a two-dimensional semiconductor and a metallic contact can lead to a semiconductor-to-metal transition in the two-dimensional material--a finding which points the way to a possible method of achieving low-resistance junctions. Specifically, single-layer WS$_2$ undergoes a semiconductor-to-metal transition when epitaxially grown on Ag(111), while it remains a direct band gap semiconductor on Au(111). The metallicity of the single layer on Ag(111) is established by lineshape analysis of core level photoemission spectra. Angle-resolved photoemission spectroscopy locates the metallic states near the Q point of the WS$_2$ Brillouin zone. Density functional theory calculations show that the metallic states arise from hybridization between Ag bulk bands and the local conduction band minimum of WS$_2$ near the Q point.

cond-mat.mtrl-sci↗

Electron-phonon coupling in the spin-split valence band of single layer WS$_2$

The absence of inversion symmetry leads to a strong spin-orbit splitting of the upper valence band of semiconducting single layer transition metal dichalchogenides such as MoS$_2$ or WS$_2$. This permits a direct comparison of the electron-phonon coupling strength in states that only differ by their spin. Here, the electron-phonon coupling in the valence band maximum of single-layer WS$_2$ is studied by first principles calculations and angle-resolved photoemission. The coupling strength is found to be drastically different for the two spin-split branches, with calculated values of $λ_K=$0.0021 and 0.40 for the upper and lower spin-split valence band of the free-standing layer, respectively. This difference is somewhat reduced when including scattering processes involving the Au(111) substrate present in the experiment and the experimental results confirm the strongly branch-dependent coupling strength.

cond-mat.str-el↗

Reconstruction-induced trefoil knot Fermi contour of Au(111)

Using angle-resolved photoemission spectroscopy (ARPES), we study the effect of the so-called herringbone reconstruction of Au(111) on the dispersion of the free electron-like surface state. While earlier ARPES investigations have only reported a minor interplay of the surface state dispersion and the underlying reconstruction, we show that the uniaxial lattice distortion and the thereby changed reciprocal lattice for the first atomic layer leads to distinct surface state dispersions around the first order reciprocal lattice points of the three domains, creating a constant energy surface resembling a trefoil knot. The findings resolve the long-standing discrepancy between, on one hand, the reconstruction-induced surface state modifications reported in scanning tunnelling microscopy and first principle calculations and, on the other hand, their conspicuous absence in photoemission.

cond-mat.mes-hall↗

Absence of superconductivity in ultra-thin layers of FeSe synthesized on a topological insulator

The structural and electronic properties of FeSe ultra-thin layers on Bi$_{2}$Se$_{3}$ have been investigated with a combination of scanning tunneling microscopy and spectroscopy and angle-resolved photoemission spectroscopy. The FeSe multi-layers, which are predominantly 3-5 monolayers (ML) thick, exhibit a hole pocket-like electron band at \barΓ and a dumbbell-like feature at \bar{M}, similar to multi-layers of FeSe on SrTiO$_{3}$. Moreover, the topological state of the Bi2Se3 is preserved beneath the FeSe layer, as indicated by a heavily \it{n}-doped Dirac cone. Low temperature STS does not exhibit a superconducting gap for any investigated thickness down to a temperature of 5 K.

cond-mat.supr-con↗

Spin and Valley Control of Free Carriers in Single-Layer WS$_2$

The semiconducting single-layer transition metal dichalcogenides have been identified as ideal materials for accessing and manipulating spin- and valley-quantum numbers due to a set of favorable optical selection rules in these materials. Here, we apply time- and angle-resolved photoemission spectroscopy to directly probe optically excited free carriers in the electronic band structure of a high quality single layer of WS$_2$. We observe that the optically generated free hole density in a single valley can be increased by a factor of 2 using a circularly polarized optical excitation. Moreover, we find that by varying the photon energy of the excitation we can tune the free carrier density in a given spin-split state around the valence band maximum of the material. The control of the photon energy and polarization of the excitation thus permits us to selectively excite free electron-hole pairs with a given spin and within a single valley.

cond-mat.mes-hall↗

Crystalline and electronic structure of single-layer TaS$_2$

Single-layer TaS$_2$ is epitaxially grown on Au(111) substrates. The resulting two-dimensional crystals adopt the 1H polymorph. The electronic structure is determined by angle-resolved photoemission spectroscopy and found to be in excellent agreement with density functional theory calculations. The single layer TaS$_2$ is found to be strongly n-doped, with a carrier concentration of 0.3(1) extra electrons per unit cell. No superconducting or charge density wave state is observed by scanning tunneling microscopy at temperatures down to 4.7 K.

cond-mat.str-el↗

Ultrafast Band Structure Control of a Two-Dimensional Heterostructure

The electronic structure of two-dimensional (2D) semiconductors can be significantly altered by screening effects, either from free charge carriers in the material itself, or by environmental screening from the surrounding medium. The physical properties of 2D semiconductors placed in a heterostructure with other 2D materials are therefore governed by a complex interplay of both intra- and inter-layer interactions. Here, using time- and angle-resolved photoemission, we are able to isolate both the layer-resolved band structure and, more importantly, the transient band structure evolution of a model 2D heterostructure formed of a single layer of MoS$_2$ on graphene. Our results reveal a pronounced renormalization of the quasiparticle gap of the MoS$_2$ layer. Following optical excitation, the band gap is reduced by up to $\sim\!$400 meV on femtosecond timescales due to a persistence of strong electronic interactions despite the environmental screening by the $n$-doped graphene. This points to a large degree of tuneability of both the electronic structure and electron dynamics for 2D semiconductors embedded in a van der Waals-bonded heterostructure.

cond-mat.mtrl-sci↗

Single-layer MoS$_2$ on Au(111): band gap renormalization and substrate interaction

The electronic structure of epitaxial single-layer MoS$_2$ on Au(111) is investigated by angle-resolved photoemission spectroscopy, scanning tunnelling spectroscopy, and first principles calculations. While the band dispersion of the supported single-layer is close to a free-standing layer in the vicinity of the valence band maximum at $\bar{K}$ and the calculated electronic band gap on Au(111) is similar to that calculated for the free-standing layer, significant modifications to the band structure are observed at other points of the two-dimensional Brillouin zone: At $\barΓ$, the valence band maximum has a significantly higher binding energy than in the free MoS$_2$ layer and the expected spin-degeneracy of the uppermost valence band at the $\bar{M}$ point cannot be observed. These band structure changes are reproduced by the calculations and can be explained by the detailed interaction of the out-of-plane MoS$_2$ orbitals with the substrate.

cond-mat.str-el↗

Synthesis of Epitaxial Single-Layer MoS$_2$ on Au(111)

We present a method for synthesizing large area epitaxial single-layer MoS$_2$ on the Au(111) surface in ultrahigh vacuum. Using scanning tunneling microscopy and low energy electron diffraction, the evolution of the growth is followed from nanoscale single-layer MoS$_2$ islands to a continuous MoS$_2$ layer. An exceptionally good control over the MoS$_2$ coverage is maintained using an approach based on cycles of Mo evaporation and sulfurization to first nucleate the MoS$_2$ nano-islands and then gradually increase their size. During this growth process the native herringbone reconstruction of Au(111) is lifted as shown by low energy electron diffraction measurements. Within these MoS$_2$ islands, we identify domains rotated by 60$^{\circ}$ that lead to atomically sharp line defects at domain boundaries. As the MoS$_2$ coverage approaches the limit of a complete single-layer, the formation of bilayer MoS$_2$ islands is initiated. Angle-resolved photoemission spectroscopy measurements of both single and bilayer MoS$_2$ samples show a dramatic change in their band structure around the center of the Brillouin zone. Brief exposure to air after removing the MoS$_2$ layer from vacuum is not found to affect its quality.

cond-mat.mtrl-sci↗

Growth and electronic structure of epitaxial single-layer WS$_2$ on Au(111)

Large-area single-layer WS$_2$ is grown epitaxially on Au(111) using evaporation of W atoms in a low pressure H$_2$S atmosphere. It is characterized by means of scanning tunneling microscopy, low-energy electron diffraction and core-level spectroscopy. Its electronic band structure is determined by angle-resolved photoemission spectroscopy. The valence band maximum at $\bar{K}$ is found to be significantly higher than at $\barΓ$. The observed dispersion around $\bar{K}$ is in good agreement with density functional theory calculations for a free-standing monolayer, whereas the bands at $\barΓ$ are found to be hybridized with states originating from the Au substrate. Strong spin-orbit coupling leads to a large spin-splitting of the bands in the neighborhood of the $\bar{K}$ points, with a maximum splitting of 419(11)~meV. The valence band dispersion around $\bar{K}$ is found to be highly anisotropic with spin-branch dependent effective hole masses of $0.40(02)m_e$ and $0.57(09)m_e$ for the upper and lower split valence band, respectively. The large size of the spin-splitting and the low effective mass of the valence band maximum make single-layer WS$_2$ a promising alternative to the widely studied MoS$_2$ for applications in electronics, spintronics and valleytronics.

cond-mat.str-el↗

Strongly anisotropic spin-orbit splitting in a two-dimensional electron gas

Near-surface two-dimensional electron gases on the topological insulator Bi$_2$Te$_2$Se are induced by electron doping and studied by angle-resolved photoemission spectroscopy. A pronounced spin-orbit splitting is observed for these states. The $k$-dependent splitting is strongly anisotropic to a degree where a large splitting ($\approx 0.06$ Å$^{-1}$) can be found in the $\barΓ\bar{M}$ direction while the states are hardly split along $\barΓ\bar{K}$. The direction of the anisotropy is found to be qualitatively inconsistent with results expected for a third-order anisotropic Rashba Hamiltonian. However, a $\mathbf{k} \cdot \mathbf{p}$ model that includes the possibility of band structure anisotropy as well as both isotropic and anisotropic third order Rashba splitting can explain the results. The isotropic third order contribution to the Rashba Hamiltonian is found to be negative, reducing the energy splitting at high $k$. The interplay of band structure, higher order Rashba effect and tuneable doping offers the opportunity to engineer not only the size of the spin-orbit splitting but also its direction.

cond-mat.str-el↗

Electronic Structure of Epitaxial Single-Layer MoS$_2$

The electronic structure of epitaxial single-layer MoS$_2$ on Au(111) is investigated by angle-resolved photoemission spectroscopy. Pristine and potassium-doped layers are studied in order to gain access to the conduction band. The potassium-doped layer is found to have a (1.39$\pm$0.05)~eV direct band gap at $\bar{K}$ with the valence band top at $\barΓ$ having a significantly higher binding energy than at $\bar{K}$. The moiré superstructure of the epitaxial system does not lead to the presence of observable replica bands or minigaps. The degeneracy of the upper valence band at $\bar{K}$ is found to be lifted by the spin-orbit interaction, leading to a splitting of (145$\pm$4)~meV. This splitting is anisotropic and in excellent agreement with recent calculations. Finally, it is shown that the strength of the potassium doping is $k$-dependent, leading to the possibility of band structure engineering in single-layers of transition metal dichalcogenides.

cond-mat.mtrl-sci↗

Tailoring the electronic texture of a topological insulator via its surface orientation

Three dimensional topological insulator crystals consist of an insulating bulk enclosed by metallic surfaces, and detailed theoretical predictions about the surface state band topology and spin texture are available. While several topological insulator materials are currently known, the existence and topology of these metallic states have only ever been probed for one particular surface orientation of a given material. For most topological insulators, such as Bi$_{1-x}$Sb$_{x}$ and Bi$_2$Se$_3$, this surface is the closed-packed (111) surface and it supports one topologically guaranteed surface state Dirac cone. Here we experimentally realise a non closed-packed surface of a topological insulator, Bi$_{1-x}$Sb$_{x}$(110), and probe the surface state topology by angle-resolved photoemission. As expected, this surface also supports metallic states but the change in surface orientation drastically modifies the band topology, leading to three Dirac cones instead of one, in excellent agreement with the theoretical predictions but in contrast to any other experimentally studied TI surface. This illustrates the possibility to tailor the basic topological properties of the surface via its crystallographic direction. Here it introduces a valley degree of freedom not previously achieved for topological insulator systems.

cond-mat.str-el↗