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Stefan Muff

Publications and source records attributed to Stefan Muff.

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Large differential attosecond delays in solid state photoemission

Time-resolved photoelectron spectroscopy provides access to the electronic structure and non-equilibrium electron dynamics in matter. At solid surfaces photoemission dynamics can be investigated on its natural time scale by measuring attosecond time delays of emitted electrons. Photoelectrons with final state energies of several tens of eV need tens to hundreds of attoseconds to be released into the vacuum. Competing effects determine the emission dynamics and, hence, the full picture of the process is still under debate. The rather large energy differences between the final states probed in commonly reported relative photoemission delays obscure their complex fine structure and hinders the interpretation of the measurements. Here we report differential attosecond delays $\tau_{\mathrm{DAD}}$, i.e., relative photoemission delays for energetically close-lying spin-orbit split states. Differential attosecond delays on the order of 30 to 100 as for Bi 5d, Te 4d, and Se 3d core level photoemission from Bi$_2$Te$_3$ and Bi$_2$Se$_3$ can neither be attributed to intra-atomic delays, nor to ballistic transport and subsequent emission. Instead, calculations based on the one-step photoemission theory reveal that photoemission delays vary strongly on the energy scale of the spin-orbit splitting and quantitatively match experimental observations. This strong variation arises from multiple scattering at the surface leading to final states that involve both evanescent and propagating Bloch waves. Their relative amplitudes vary strongly affecting thereby the timing of the photoemission event since evanescent and propagating components exhibit inherently different dynamics.

physics.optics

Universal Structural Influence on the 2D Electron Gas at SrTiO$_3$ Surfaces

The two-dimensional electron gas found at the surface of SrTiO$_3$ and related interfaces has attracted significant attention as a promising basis for oxide electronics. In order to utilize its full potential, the response of this 2DEG to structural changes and surface modification must be understood in detail. Here, we present a study of the detailed electronic structure evolution of the 2DEG as a function of sample temperature and surface step density. By comparing our experimental results with \textit{ab initio} calculations, we found that a SrO-rich surface layer is a prerequisite for electronic confinement. We also show that local structure relaxations cause a metal-insulator transition of the system around 135~K. Our study presents a new and simple way of tuning the 2DEG via surface vicinality and identifies how the operation of prospective devices will respond to changes in temperature.

cond-mat.mtrl-sci

Single spin-polarised Fermi surface in SrTiO$_3$ thin films

The 2D electron gas (2DEG) formed at the surface of SrTiO$_3$(001) has attracted great interest because of its fascinating physical properties and potential as a novel electronic platform, but up to now has eluded a comprehensible way to tune its properties. Using angle-resolved photoemission spectroscopy with and without spin detection we here show that the band filling can be controlled by growing thin SrTiO$_3$ films on Nb doped SrTiO$_3$(001) substrates. This results in a single spin-polarised 2D Fermi surface, which bears potential as platform for Majorana physics. Based on our results it can furthermore be concluded that the 2DEG does not extend more than 2 unit cells into the film and that its properties depend on the amount of SrO$_x$ at the surface and possibly the dielectric response of the system.

cond-mat.str-el

Spin-resolved electronic response to the phase transition in MoTe$_2$

The semimetal MoTe$_2$ is studied by spin- and angle- resolved photoemission spectroscopy to probe the detailed electronic structure underlying its broad range of response behavior. A novel spin-texture is uncovered in the bulk Fermi surface of the non-centrosymmetric structural phase that is consistent with first-principles calculations. The spin-texture is three-dimensional, both in terms of momentum dependence and spin-orientation, and is not completely suppressed above the centrosymmetry-breaking transition temperature. Two types of surface Fermi arc are found to persist well above the transition temperature. The appearance of a large Fermi arc depends strongly on thermal history, and the electron quasiparticle lifetimes are greatly enhanced in the initial cooling. The results indicate that polar instability with strong electron-lattice interactions exists near the surface when the bulk is largely in a centrosymmetric phase.

cond-mat.mtrl-sci

Observation of Wannier-Stark localization at the surface of BaTiO$_3$ films by photoemission

Observation of Bloch oscillations and Wannier-Stark localization of charge carriers is typically impossible in single-crystals, because an electric field higher than the breakdown voltage is required. In BaTiO$_3$ however, high intrinsic electric fields are present due to its ferroelectric properties. With angle-resolved photoemission we directly probe the Wannier-Stark localized surface states of the BaTiO$_3$ film-vacuum interface and show that this effect extends to thin SrTiO$_3$ overlayers. The electrons are found to be localized along the in-plane polarization direction of the BaTiO$_3$ film.

cond-mat.mes-hall

Observation of a two-dimensional electron gas at CaTiO$_3$ film surfaces

The two-dimensional electron gas at the surface of titanates gathered attention due to its potential to replace conventional silicon based semiconductors in the future. In this study, we investigated films of the parent perovskite CaTiO$_3$, grown by pulsed laser deposition, by means of angular-resolved photoelectron spectroscopy. The films show a c(4x2) surface reconstruction after the growth that is reduced to a p(2x2) reconstruction under UV-light. At the CaTiO$_3$ film surface, a two-dimensional electron gas (2DEG) is found with an occupied band width of 400 meV. With our findings CaTiO$_3$ is added to the group of oxides with a 2DEG at their surface. Our study widens the phase space to investigate strontium and barium doped CaTiO$_3$ and the interplay of ferroelectric properties with the 2DEG at oxide surfaces. This could open up new paths to tailor two-dimensional transport properties of these systems towards possible applications.

cond-mat.mes-hall

Spin polarization and attosecond time delay in photoemission from spin degenerate states of solids

After photon absorption, electrons from a dispersive band of a solid require a finite time in the photoemission process before being photoemitted as free particles, in line with recent attosecondresolved photoemission experiments. According to the Eisenbud-Wigner-Smith model, the time delay is due to a phase shift of different transitions that occur in the process. Such a phase shift is also at the origin of the angular dependent spin polarization of the photoelectron beam, observable in spin degenerate systems without angular momentum transfer by the incident photon. We propose a semi-quantitative model which permits to relate spin and time scales in photoemission from condensed matter targets and to better understand spin- and angle-resolved photoemission spectroscopy (SARPES) experiments on spin degenerate systems. We also present the first experimental determination by SARPES of this time delay in a dispersive band, which is found to be greater than 26 as for electrons emitted from the sp-bulk band of the model system Cu(111).

cond-mat.mes-hall

Sputtering induced re-emergence of the topological surface state in Bi$_2$Se$_3$

We study the fate of the surface states of Bi$_2$Se$_3$ under disorder with strength larger than the bulk gap, caused by neon sputtering and nonmagnetic adsorbates. We find that neon sputtering introduces strong but dilute defects, which can be modeled by a unitary impurity distribution, whereas adsorbates, such as water vapor or carbon monoxide, are best described by Gaussian disorder. Remarkably, these two disorder types have a dramatically different effect on the surface states. Our soft x-ray ARPES measurements combined with numerical simulations show that unitary surface disorder pushes the Dirac state to inward quintuplet layers, burying it below an insulating surface layer. As a consequence, the surface spectral function becomes weaker, but retains its quasiparticle peak. This is in contrast to Gaussian disorder, which smears out the quasiparticle peak completely. At the surface of Bi$_2$Se$_3$, the effects of Gaussian disorder can be reduced by removing surface adsorbates using neon sputtering, which, however, introduces unitary scatterers. Since unitary disorder has a weaker effect than Gaussian disorder, the ARPES signal of the Dirac surface state becomes sharper upon sputtering.

cond-mat.mes-hall

Response of the topological surface state to surface disorder in TlBiSe$_2$

Through a combination of experimental techniques we show that the topmost layer of the topo- logical insulator TlBiSe$_2$ as prepared by cleavage is formed by irregularly shaped Tl islands at cryogenic temperatures and by mobile Tl atoms at room temperature. No trivial surface states are observed in photoemission at low temperatures, which suggests that these islands can not be re- garded as a clear surface termination. The topological surface state is, however, clearly resolved in photoemission experiments. This is interpreted as a direct evidence of its topological self-protection and shows the robust nature of the Dirac cone like surface state. Our results can also help explain the apparent mass acquisition in S-doped TlBiSe$_2$.

cond-mat.mes-hall

Separating the bulk and surface n- to p-type transition in the topological insulator GeBi(4-x)SbxTe7

We identify the multi-layered compound GeBi4Te7 to be a topological insulator with a freestanding Dirac point, slightly above the valence band maximum, using angle-resolved photoemission spectroscopy (ARPES) measurements. The spin polarization satisffies the time reversal symmetry of the surface states, visible in spin-resolved ARPES. For increasing Sb content in GeBi(4-x)SbxTe7 we observe a transition from n- to p-type in bulk sensitive Seebeck coefficient measurements at a doping of x = 0.6. In surface sensitive ARPES measurements a rigid band shift is observed with Sb doping, accompanied by a movement of the Dirac point towards the Fermi level. Between x = 0.8 and x = 1 the Fermi level crosses the band gap, changing the surface transport regime. This difference of the n- to p-type transition between the surface region and the bulk is caused by band bending effects which are also responsible for a non-coexistence of insulating phases in the bulk and in the near surface region.

cond-mat.mtrl-sci

Interband spin-orbit coupling between anti-parallel spin states in Pb quantum well states

Using spin and angle-resolved photoemission spectroscopy we investigate a momentum region in Pb quantum well states on Si(111) where hybridization between Rashba-split bands alters the band structure significantly. Starting from the Rashba regime where the dispersion of the quasi-free two-dimensional electron gas is well described by two spin-polarized parabolas, we find a breakdown of the Rashba behavior which manifests itself (i) in a spin splitting that is no longer proportional to the in-plane momentum and (ii) in a reversal of the sign of the momentum splitting. Our experimental findings are well explained by including interband spin-orbit coupling that mixes Rashba-split states with anti-parallel rather than parallel spins. Similar results for Pb/Cu(111) reveal that the proposed hybridization scenario is independent on the supporting substrate.

cond-mat.mtrl-sci

Surface and bulk Fermiology and band dispersion in non-centrosymmetric BiTeI

BiTeI has a layered and non-centrosymmetric structure where strong spin-orbit interaction leads to a giant spin splitting in the bulk bands. Here we present high-resolution angle-resolved photoemission (ARPES) data in the UV and soft x-ray regime that clearly disentangle the surface from the bulk electronic structure. Spin-resolved UV-ARPES measurements on opposite, non-equivalent surfaces show identical spin structures, thus clarifying the surface state character. Soft x-ray ARPES data clearly reveal the spindle-torus shape of the bulk Fermi surface, induced by the spin-orbit interaction.

cond-mat.mtrl-sci