arXiv subjects

L. Dudy

Publications and source records attributed to L. Dudy.

15 recordsLinked to original sources

arXiv2024

Anomalous 4$f$ fine structure in TmSe$_{1-x}$Te$_x$ across the metal-insulator transition

Hybridization between localized 4$f$ and itinerant 5$d$6$s$ states in heavy fermion compounds is a well-studied phenomenon and commonly captured by the paradigmatic Anderson model. However, the investigation of additional electronic interactions, beyond the standard Anderson model, has been limited, despite their predicted important role in the exotic quasiparticle formation in mixed-valence systems. We investigate the 4$f$ states in TmSe$_{1-x}$Te$_x$ throughout a semimetal-insulator phase transition, which drastically varies the interactions related to the 4$f$ states. Using synchrotron-based hard x-ray and extreme ultraviolet photoemission spectroscopy, we resolve subtle peak splitting in the 4$f$ peaks near the Fermi level in the mixed-valent semimetal phase. The separation is enhanced by several tens of meV by increasing the lattice parameter by a few percent. Our results elucidate the evolving nature of the 4$f$ state across the phase transition, and provide direct experimental evidence for electronic interactions beyond the standard Anderson model in mixed-valence systems.

cond-mat.str-el↗

arXiv2022

Global perspectives of the bulk electronic structure of URu$_2$Si$_2$ from angle-resolved photoemission

Previous high-resolution angle-resolved photoemission (ARPES) studies of URu$_2$Si$_2$ have characterized the temperature-dependent behavior of narrow-band states close to the Fermi level ($E_\mathrm{F}$) at low photon energies near the zone center, with an emphasis on electronic reconstruction due to Brillouin zone folding. A substantial challenge to a proper description is that these states interact with other hole-band states that are generally absent from bulk-sensitive soft x-ray ARPES measurements. Here we provide a more global $k$-space context for the presence of such states and their relation to the bulk Fermi surface topology using synchrotron-based wide-angle and photon energy-dependent ARPES mapping of the electronic structure using photon energies intermediate between the low-energy regime and the high-energy soft x-ray regime. Small-spot spatial dependence, $f$-resonant photoemission, Si 2$p$ core-levels, x-ray polarization, surface-dosing modification, and theoretical surface slab calculations are employed to assist identification of bulk versus surface state character of the $E_\mathrm{F}$-crossing bands and their relation to specific U- or Si-terminations of the cleaved surface. The bulk Fermi surface topology is critically compared to density functional theory and to dynamical mean field theory calculations. In addition to clarifying some aspects of the previously measured high symmetry $Γ$, Z and X points, incommensurate 0.6a* nested Fermi-edge states located along Z-N-Z are found to be distinctly different from the density functional theory Fermi surface prediction. The temperature evolution of these states above $T_{HO}$, combined with a more detailed theoretical investigation of this region, suggests a key role of the N-point in the hidden order transition.

cond-mat.str-el↗

arXiv2018

Wannier-Orbital theory and ARPES for the quasi-1D conductor LiMo$_{6}$O$_{17}$

In this set of three papers, we present the results of a combined study by density-functional (LDA) band theory (NMTO) and angle-resolved photoemission spectroscopy (ARPES) of lithium purple bronze, 2(Li$_{1x}$Mo$_{6}$O$_{17}$). This material is particularly notable for its unusually robust quasi-one-dimensional (quasi-1D) behavior. The band structure, in a large energy window around the Fermi energy, is basically 2D and formed by three Mo $t_{2g}$-like extended Wannier orbitals (WOs) per cell, each one giving rise to a 1D band running at a 120$^{\circ }$ angle to the two others. A structural "dimerization" from $\mathbf{c}/2$ to $\mathbf{c}$ gaps the $xz$ and $yz$ bands while leaving the $xy$ bands metallic in the gap but resonantly coupled to the gap edges and, hence, to the two other directions. The resulting complex shape of the quasi-1D Fermi surface (FS), verified by our ARPES, thus depends strongly on the Fermi energy position in the gap, implying a great sensitivity to Li stoichiometry of properties dependent on the FS, such as FS nesting or superconductivity. The band structure, expressed as a six-band, analytical tight-binding (TB) Hamiltonian, is verified in detail by the recognition and application of an ARPES selection rule that enables, for the first time, the separation in ARPES spectra of the two barely split $xy$ bands and the observation of their complex split FS. The strong resonances prevent either a two-band TB model or a related real-space ladder picture from giving a valid description of the low-energy electronic structure. Down to a temperature of 6$\,$K we find no evidence for a theoretically expected downward renormalization of perpendicular single particle hopping due to LL fluctuations in the quasi-1D chains.

cond-mat.str-el↗

arXiv2017

The topological surface state of $α$-Sn on InSb(001) as studied by photoemission

We report on the electronic structure of the elemental topological semimetal $α$-Sn on InSb(001). High-resolution angle-resolved photoemission data allow to observe the topological surface state (TSS) that is degenerate with the bulk band structure and show that the former is unaffected by different surface reconstructions. An unintentional $p$-type doping of the as-grown films was compensated by deposition of potassium or tellurium after the growth, thereby shifting the Dirac point of the surface state below the Fermi level. We show that, while having the potential to break time-reversal symmetry, iron impurities with a coverage of up to 0.25 monolayers do not have any further impact on the surface state beyond that of K or Te. Furthermore, we have measured the spin-momentum locking of electrons from the TSS by means of spin-resolved photoemission. Our results show that the spin vector lies fully in-plane, but it also has a finite radial component. Finally, we analyze the decay of photoholes introduced in the photoemission process, and by this gain insight into the many-body interactions in the system. Surprisingly, we extract quasiparticle lifetimes comparable to other topological materials where the TSS is located within a bulk band gap. We argue that the main decay of photoholes is caused by intraband scattering, while scattering into bulk states is suppressed due to different orbital symmetries of bulk and surface states.

cond-mat.str-el↗

arXiv2017

Microscopic origin of the mobility enhancement at a spinel/perovskite oxide heterointerface revealed by photoemission spectroscopy

The spinel/perovskite heterointerface $γ$-Al$_2$O$_3$/SrTiO$_3$ hosts a two-dimensional electron system (2DES) with electron mobilities exceeding those in its all-perovskite counterpart LaAlO$_3$/SrTiO$_3$ by more than an order of magnitude despite the abundance of oxygen vacancies which act as electron donors as well as scattering sites. By means of resonant soft x-ray photoemission spectroscopy and \textit{ab initio} calculations we reveal the presence of a sharply localized type of oxygen vacancies at the very interface due to the local breaking of the perovskite symmetry. We explain the extraordinarily high mobilities by reduced scattering resulting from the preferential formation of interfacial oxygen vacancies and spatial separation of the resulting 2DES in deeper SrTiO$_3$ layers. Our findings comply with transport studies and pave the way towards defect engineering at interfaces of oxides with different crystal structures.

cond-mat.str-el↗

arXiv2017

Dimensionality-driven metal-insulator-transition in spin-orbit coupled SrIrO$_3$

Upon reduction of the film thickness we observe a metal-insulator transition in epitaxially stabilized, spin-orbit coupled SrIrO$_3$ ultrathin films. By comparison of the experimental electronic dispersions with density functional theory at various levels of complexity we identify the leading microscopic mechanisms, i.e., a dimensionality-induced re-adjustment of octahedral rotations, magnetism, and electronic correlations. The astonishing resemblance of the band structure in the two-dimensional limit to that of bulk Sr$_2$IrO$_4$ opens new avenues to unconventional superconductivity by "clean" electron doping through electric field gating.

cond-mat.str-el↗

arXiv2016

Bismuthene on a SiC Substrate: A Candidate for a New High-Temperature Quantum Spin Hall Paradigm

Quantum spin Hall (QSH) materials promise revolutionary device applications based on dissipationless propagation of spin currents. They are two-dimensional (2D) representatives of the family of topological insulators, which exhibit conduction channels at their edges inherently protected against scattering. Initially predicted for graphene, and eventually realized in HgTe quantum wells, in the QSH systems realized so far, the decisive bottleneck preventing applications is the small bulk energy gap of less than 30 meV, requiring cryogenic operation temperatures in order to suppress detrimental bulk contributions to the edge conductance. Room-temperature functionalities, however, require much larger gaps. Here we show how this can be achieved by making use of a new QSH paradigm based on substrate-supported atomic monolayers of a high-Z element. Experimentally, the material is synthesized as honeycomb lattice of bismuth atoms, forming "bismuthene", on top of the wide-gap substrate SiC(0001). Consistent with the theoretical expectations, the spectroscopic signatures in experiment display a huge gap of ~0.8 eV in bismuthene, as well as conductive edge states. The analysis of the layer-substrate orbitals arrives at a QSH phase, whose topological gap - as a hallmark mechanism - is driven directly by the atomic spin-orbit coupling (SOC). Our results demonstrate how strained artificial lattices of heavy atoms, in contact with an insulating substrate, can be utilized to evoke a novel topological wide-gap scenario, where the chemical potential is located well within the global system gap, ensuring pure edge state conductance. We anticipate future experiments on topological signatures, such as transport measurements that probe the QSH effect via quantized universal conductance, notably at room temperature.

cond-mat.str-el↗

arXiv2016

Structural behavior of Pb$_y$Bi$_{1.95-y}$Sr$_{1.49}$La$_{0.4}$Cu$_{1.15}$O$_{6+δ}$ for 0<y<0.53

In the Bi cuprates, the presence of a near 1$\times$5 superstructure is well known. Usually, this superstructure is suppressed by the substitution of lead, but there have been reports of a phase separation in so called α and β phases. This paper shows in high detail time how and why the phase separation develops and what happens to the quasi-1$\times$5 superstructure upon lead substitution. For this purpose, the lanthanum- and lead-substituted single-layered superconductor Bi$_{2+z}$Sr$_{2-z}$CuO$_{6+δ}$ has been investigated by scanning tunneling microscopy and low-energy electron diffraction. The La content was kept constant at slightly under-doped concentration while the Pb content was changed systematically. Thermodynamic considerations show that a phase mixture of α and β phases is inevitable.

cond-mat.supr-con↗

arXiv2013

Elemental Topological Insulator with a Tunable Fermi Level: Strained α-Sn on InSb(001)

We report on the epitaxial fabrication and electronic properties of a topological phase in strained α-Sn on InSb. The topological surface state forms in the presence of an unusual band order not based on direct spin-orbit coupling, as shown in density functional and GW slab-layer calculations. Angle-resolved photoemission including spin detection probes experimentally how the topological spin-polarized state emerges from the second bulk valence band. Moreover, we demonstrate the precise control of the Fermi level by dopants.

cond-mat.mes-hall↗

arXiv2013

Yb Valence Change in (Ce,Yb)CoIn5 from spectroscopy and bulk properties

The electronic structure of (Ce,Yb)CoIn5 has been studied by a combination of photoemission, x-ray absorption and bulk property measurements. Previous findings of a Ce valence near 3+ for all x and of an Yb valence near 2.3+ for x>0.3 were confirmed. One new result of this study is that the Yb valence for x<0.2 increases rapidly with decreasing x from 2.3+ toward 3+, which correlates well with de Haas van Alphen results showing a change of Fermi surface around x=0.2. Another new result is the direct observation by angle resolved photoemission Fermi surface maps of about 50% cross sectional area reductions of the α- and β-sheets for x=1 compared to x=0, and a smaller, essentially proportionate, size change of the α-sheet for x=0.2. These changes are found to be in good general agreement with expectations from simple electron counting. The implications of these results for the unusual robustness of superconductivity and Kondo coherence with increasing x in this alloy system are discussed.

cond-mat.str-el↗

arXiv2013

Photoemission Spectroscopy and the Unusually Robust One Dimensional Physics of Lithium Purple Bronze

Temperature dependent photoemission spectroscopy in Li0.9Mo6O17 contributes to evidence for one dimensional physics that is unusually robust. Three generic characteristics of the Luttinger liquid are observed, power law behavior of the k-integrated spectral function down to temperatures just above the superconducting transition, k-resolved lineshapes that show holon and spinon features, and quantum critical (QC) scaling in the lineshapes. Departures of the lineshapes and the scaling from expectations in the Tomonaga Luttinger model can be partially described by a phenomenological momentum broadening that is presented and discussed. The possibility that some form of 1d physics obtains even down to the superconducting transition temperature is assessed.

cond-mat.str-el↗

arXiv2010

Anomalies in the superconducting dome of the Bi-cuprates

We report characterization results by energy dispersive x-ray analysis and AC-susceptibility for a statistically relevant number of single layer Bi-cuprate single crystals. We show that the two structurally quite different modifications of the single-layered Bi-cuprate, namely (La,Pb=0.4)-Bi2201 and La-Bi2201, exhibit anomalies in the superconducting transition temperature at certain hole doping, e.g. at 1/8 holes per Cu. These doping values agree well with the 'magic doping fractions' found in the temperature dependent resistance of LSCO by Komiya et al. This new set of findings suggests that all these anomalies are generic for the hole-doped high-temperature superconductors.

cond-mat.supr-con↗

arXiv2007

Charge modulation driven Fermi surface of Pb-Bi2201

It is well known that the (1x5) superstructure of Bi cuprate superconductors will be suppressed due to optimum doping with Pb. Nevertheless, a Fermi surface map of (Pb,La)-Bi2201 (Pb = 0.4 and La = 0.4) determined by angular resolved photoemission (ARPES) revealed additional Fermi surface features. Low energy electron diffraction and X-ray diffraction of these samples showed no sign of any superstructure. Scanning tunneling microscopy (STM), on the other hand, revealed two distinct modulations of the charge density, one of (1x32) and a second of (6x6) periodicity. The wave vectors of both modulations have been extracted and used to simulate the corresponding Fermi surface, which is compared with the experimental one. The origin of these modulations is discussed in terms of dopant ordering.

cond-mat.supr-con↗

arXiv2001

Unusual electronic ground state of a prototype cuprate: band splitting of single CuO_2-plane Bi_2 Sr_(2-x) La_x CuO_(6+delta)

By in-situ change of polarization a small splitting of the Zhang-Rice singlet state band near the Fermi level has been resolved for optimum doped (x=0.4) Bi$_{2}$Sr$_{2-x}$La$_{x}$CuO$_{6+δ}$ at the (pi,0)-point (R.Manzke et al. PRB 63, R100504 (2001). Here we treat the momentum dependence and lineshape of the split band by photoemission in the EDC-mode with very high angular and energy resolution. The splitting into two destinct emissions could also be observed over a large portion of the major symmetry line $Γ$M, giving the dispersion for the individual contributions. Since bi-layer effects can not be present in this single-layer material the results have to be discussed in the context of one-particle removal spectral functions derived from current theoretical models. The most prominent are microscopic phase separation including striped phase formation, coexisting antiferromagnetic and incommensurate charge-density-wave critical fluctuations coupled to electrons (hot spots) or even spin charge separation within the Luttinger liquid picture, all leading to non-Fermi liquid like behavior in the normal state and having severe consequences on the way the superconducting state forms. Especially the possibilty of observing spinon and holon excitations is discussed.

cond-mat.supr-con↗

arXiv2001

Fermi surface and superconducting gap of triple-layered Bi2Sr2Ca2Cu3O10+d

We present a comprehensive study performed with high-resolution angle-resolved photoemission spectroscopy on triple-layered Bi2Sr2Ca2Cu3O10+d single crystals. By measurements above TC the Fermi surface topology defined by the Fermi level crossings of the CuO2-derived band was determined. A hole-like Fermi surface as for single and double-CuO2 layered Bi-based cuprates is found, giving new input to the current debate of the general Fermi surface topology of the high Tc superconductors. Furthermore, we present measurements of the superconducting gap of Bi-2223 and show that there are clear indications for a strong anisotropy of the superconducting gap. The universal properties of this phase in comparison to the other Bi-based cuprates will be discussed.

cond-mat.supr-con↗