arXiv subjects

Søren Ulstrup

Publications and source records attributed to Søren Ulstrup.

At least 55 records · Page 3Linked to original sources

arXiv2019

Transient Hot Electron Dynamics in Single-Layer TaS$_2$

Using time- and angle-resolved photoemission spectroscopy, we study the response of metallic single layer TaS$_2$ in the 1H structural modification to the generation of excited carriers by a femtosecond laser pulse. A complex interplay of band structure modifications and electronic temperature increase is observed and analyzed by direct fits of model spectral functions to the two-dimensional (energy and $k$-dependent) photoemission data. Upon excitation, the partially occupied valence band is found to shift to higher binding energies by up to 150 meV, accompanied by electronic temperatures exceeding 3000~K. These observations are explained by a combination of temperature-induced shifts of the chemical potential, as well as temperature-induced changes in static screening. Both contributions are evaluated in a semi-empirical tight-binding model. The shift resulting from a change in the chemical potential is found to be dominant.

cond-mat.str-el↗

arXiv2018

Emergence of a Metal-Insulator Transition and High Temperature Charge Density Waves in VSe2 at the Monolayer Limit

Emergent phenomena driven by electronic reconstructions in oxide heterostructures have been intensively discussed. However, the role of these phenomena in shaping the electronic properties in van der Waals heterointerfaces has hitherto not been established. By reducing the material thickness and forming a heterointerface, we find two types of charge-ordering transitions in monolayer VSe2 on graphene substrates. Angle-resolved photoemission spectroscopy (ARPES) uncovers that Fermi-surface nesting becomes perfect in ML VSe2. Renormalization group analysis confirms that imperfect nesting in three dimensions universally flows into perfect nesting in two dimensions. As a result, the charge density wave transition temperature is dramatically enhanced to a value of 350 K compared to the 105 K in bulk VSe2. More interestingly, ARPES and scanning tunneling microscopy measurements confirm an unexpected metal-insulator transition at 135 K, driven by lattice distortions. The heterointerface plays an important role in driving this novel metal-insulator transition in the family of monolayered transition metal dichalcogenides.

cond-mat.str-el↗

arXiv2018

Electronic Structure of Exfoliated and Epitaxial Hexagonal Boron Nitride

Hexagonal boron nitride (hBN) is an essential component in van der Waals heterostructures as it provides high quality and weakly interacting interfaces that preserve the electronic properties of adjacent materials. While exfoliated flakes of hBN have been extensively studied using electron transport and optical probes, detailed experimental measurements of the energy- and momentum- dependent electronic excitation spectrum are lacking. Here, we directly determine the full valence band (VB) electronic structure of micron-sized exfoliated flakes of hBN using angle-resolved photoemission spectroscopy with micrometer spatial resolution. We identify the π- and σ-band dispersions, the hBN stacking order and determine a total VB bandwidth of 19.4 eV. We compare these results with electronic structure data for epitaxial hBN on graphene on silicon carbide grown in situ using a borazine precursor. The epitaxial growth and electronic properties are investigated using photoe- mission electron microscopy. Our measurements show that the fundamental electronic properties of hBN are highly dependent on the fabrication strategy.

cond-mat.mtrl-sci↗

arXiv2018

Photoemission Investigation of Oxygen Intercalated Epitaxial Graphene on Ru(0001)

We study the formation of epitaxial graphene on Ru(0001) using fast x-ray photoelectron spectroscopy during the growth process. The assignment of different C 1s and Ru 3d core level components and their evolution during the growth process gives a detailed insight into the graphene formation and the strongly varying graphene-Ru interaction strength within the large moire unit cell. Subsequent intercalation of oxygen can be achieved at elevated temperature and the core level spectra show a conversion of the strongly corrugated to quasi free-standing graphene, characterised by a single narrow C 1s component. This conversion and the accompanying flattening of the graphene layer is also confirmed by x-ray photoelectron diffraction. The effect of oxygen intercalation on the electronic structure is studied using angle-resolved photoemission of the valence band states. For graphene/Ru(0001), the strong graphene-substrate hybridisation disrupts the π-band dispersion but oxygen intercalation fully restores the π-band with a strong p-doping that shifts the Dirac point 785 meV above the Fermi level. The doping of the system is highly tunable, as the additional exposure to rubidium can convert the carrier filling to n-type with the Dirac point 970 meV below the Fermi level.

cond-mat.mtrl-sci↗

arXiv2018

Giant spin-splitting and gap renormalization driven by trions in single-layer WS$_2$/h-BN heterostructures

In two-dimensional (2D) semiconducting transition metal dichalcogenides (TMDs), new electronic phenomena such as tunable band gaps and strongly bound excitons and trions emerge from strong many-body effects, beyond spin-orbit coupling- and lattice symmetry-induced spin and valley degrees of freedom. Combining single-layer (SL) TMDs with other 2D materials in van der Waals heterostructures offers an intriguing means of controlling the electronic properties through these many-body effects via engineered interlayer interactions. Here, we employ micro-focused angle-resolved photoemission spectroscopy (microARPES) and in-situ surface doping to manipulate the electronic structure of SL WS$_2$ on hexagonal boron nitride (WS$_2$/h-BN). Upon electron doping, we observe an unexpected giant renormalization of the SL WS$_2$ valence band (VB) spin-orbit splitting from 430~meV to 660~meV, together with a band gap reduction of at least 325~meV, attributed to the formation of trionic quasiparticles. These findings suggest that the electronic, spintronic and excitonic properties are widely tunable in 2D TMD/h-BN heterostructures, as these are intimately linked to the quasiparticle dynamics of the materials.

cond-mat.mtrl-sci↗

arXiv2017

NaSn2As2: An Exfoliatable Layered van der Waals Zintl Phase

The discovery of new families of exfoliatable 2D crystals that have diverse sets of electronic, optical, and spin-orbit coupling properties, enables the realization of unique physical phenomena in these few-atom thick building blocks and in proximity to other materials. Herein, using NaSn2As2 as a model system, we demonstrate that layered Zintl phases having the stoichiometry ATt2Pn2 (A = Group 1 or 2 element, Tt = Group 14 tetrel element and Pn = Group 15 pnictogen element) and feature networks separated by van der Waals gaps can be readily exfoliated with both mechanical and liquid-phase methods. We identified the symmetries of the Raman active modes of the bulk crystals via polarized Raman spectroscopy. The bulk and mechanically exfoliated NaSn2As2 samples are resistant towards oxidation, with only the top surface oxidizing in ambient conditions over a couple of days, while the liquid-exfoliated samples oxidize much more quickly in ambient conditions. Employing angle-resolved photoemission spectroscopy (ARPES), density functional theory (DFT), and transport on bulk and exfoliated samples, we show that NaSn2As2 is a highly conducting 2D semimetal, with resistivities on the order of 10-6 Ω m. Due to peculiarities in the band structure, the dominating p-type carriers at low temperature are nearly compensated by the opening of n-type conduction channels as temperature increases. This work further expands the family of exfoliatable 2D materials to layered van der Waals Zintl phases, opening up opportunities in electronics and spintronics.

cond-mat.mtrl-sci↗

arXiv2016

Spatially Resolved Electronic Properties of Single-Layer WS$_2$ on Transition Metal Oxides

There is a substantial interest in the heterostructures of semiconducting transition metal dichalcogenides (TMDCs) amongst each other or with arbitrary materials, through which the control of the chemical, structural, electronic, spintronic, and optical properties can lead to a change in device paradigms. A critical need is to understand the interface between TMDCs and insulating substrates, for example high-$κ$ dielectrics, which can strongly impact the electronic properties such as the optical gap. Here we show that the chemical and electronic properties of the single-layer (SL) TMDC, WS$_2$, can be transferred onto high-$κ$ transition metal oxide substrates TiO$_2$ and SrTiO$_3$. The resulting samples are much more suitable for measuring their electronic and chemical structures with angle-resolved photoemission than their native-grown SiO$_2$ substrates. We probe the WS$_2$ on the micron scale across 100-micron flakes, and find that the occupied electronic structure is exactly as predicted for freestanding SL WS$_2$ with a strong spin-orbit splitting of 420~meV and a direct band gap at the valence band maximum. Our results suggest that TMDCs can be combined with arbitrary multi-functional oxides, which may introduce alternative means of controlling the optoelectronic properties of such materials.

cond-mat.mtrl-sci↗

arXiv2016

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↗

arXiv2016

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↗

arXiv2016

Manifestation of nonlocal electron-electron interaction in graphene

Graphene is an ideal platform to study many-body effects due to its semimetallic character and the possibility to dope it over a wide range. Here we study the width of graphene's occupied $π$-band as a function of doping using angle-resolved photoemission. Upon increasing electron doping, we observe the expected shift of the band to higher binding energies. However, this shift is not rigid and the bottom of the band moves less than the Dirac point. We show that the observed shift cannot be accounted for by band structure calculations in the local density approximation but that non-local exchange interactions must be taken into account.

cond-mat.str-el↗

arXiv2016

Ultrafast Electron Dynamics in Epitaxial Graphene Investigated with Time- and Angle-Resolved Photoemission Spectroscopy

In order to exploit the intriguing optical properties of graphene it is essential to gain a better understanding of the light-matter interaction in the material on ultrashort timescales. Exciting the Dirac fermions with intense ultrafast laser pulses triggers a series of processes involving interactions between electrons, phonons and impurities. Here we study these interactions in epitaxial graphene supported on silicon carbide (semiconducting) and iridium (metallic) substrates using ultrafast time- and angle-resolved photoemission spectroscopy (TR-ARPES) based on high harmonic generation. For the semiconducting substrate we reveal a complex hot carrier dynamics that manifests itself in an elevated electronic temperature and an increase in linewidth of the $π$ band. By analyzing these effects we are able to disentangle electron relaxation channels in graphene. On the metal substrate this hot carrier dynamics is found to be severely perturbed by the presence of the metal, and we find that the electronic system is much harder to heat up than on the semiconductor due to screening of the laser field by the metal.

cond-mat.str-el↗

arXiv2016

Tunable Carrier Multiplication and Cooling in Graphene

Time- and angle-resolved photoemission measurements on two doped graphene samples displaying different doping levels reveal remarkable differences in the ultrafast dynamics of the hot carriers in the Dirac cone. In the more strongly ($n$-)doped graphene, we observe larger carrier multiplication factors ($>$ 3) and a significantly faster phonon-mediated cooling of the carriers back to equilibrium compared to in the less ($p$-)doped graphene. These results suggest that a careful tuning of the doping level allows for an effective manipulation of graphene's dynamical response to a photoexcitation.

cond-mat.mtrl-sci↗

arXiv2016

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↗

arXiv2015

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↗

arXiv2015

Observation of Ultrafast Free Carrier Dynamics in Single Layer MoS$_2$

The dynamics of excited electrons and holes in single layer (SL) MoS$_2$ 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 MoS$_2$ 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 MoS$_2$. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons.

cond-mat.mtrl-sci↗

arXiv2015

Ramifications of Optical Pumping on the Interpretation of Time-Resolved Photoemission Experiments on Graphene

In pump-probe time and angle-resolved photoemission spectroscopy (TR-ARPES) experiments the presence of the pump pulse adds a new level of complexity to the photoemission process in comparison to conventional ARPES. This is evidenced by pump-induced vacuum space-charge effects and surface photovoltages, as well as multiple pump excitations due to internal reflections in the sample-substrate system. These processes can severely affect a correct interpretation of the data by masking the out-of-equilibrium electron dynamics intrinsic to the sample. In this study, we show that such effects indeed influence TR-ARPES data of graphene on a silicon carbide (SiC) substrate. In particular, we find a time- and laser fluence-dependent spectral shift and broadening of the acquired spectra, and unambiguously show the presence of a double pump excitation. The dynamics of these effects is slower than the electron dynamics in the graphene sample, thereby permitting us to deconvolve the signals in the time domain. Our results demonstrate that complex pump-related processes should always be considered in the experimental setup and data analysis.

cond-mat.str-el↗

arXiv2014

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↗

arXiv2014

High Crystallinity and Decoupling of Graphene on a Metal: Reduced Coulomb Screening and Tunable pn-Junctions

High quality epitaxial graphene films can be applied as templates for tailoring graphene-substrate interfaces that allow for precise control of the charge carrier behavior in graphene through doping and many-body effects. By combining scanning tunneling microscopy, angle-resolved photoemission spectroscopy and density functional theory we demonstrate that oxygen intercalated epitaxial graphene on Ir(111) has high structural quality, is quasi free-standing, and shows signatures of many-body interactions. Using this system as a template, we show that tunable pn-junctions can be patterned by adsorption and intercalation of rubidium, and that the n-doped graphene regions exhibit a reduced Coulomb screening via enhanced electron-plasmon coupling. These findings are central for understanding and tailoring the properties of graphene-metal contacts e.g. for realizing quantum tunneling devices.

cond-mat.mtrl-sci↗