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F. Baumberger

Publications and source records attributed to F. Baumberger.

At least 19 recordsLinked to original sources

Electron-phonon coupling across the TMD/hBN van der Waals interface

Many-body interactions can couple electronic states in one layer with collective excitations in the adjacent layer, providing a route to tailor properties of heterostructures. However, detecting and quantifying interlayer many-body interactions proved a major challenge. Here, we demonstrate that quasiparticles in monolayer transition metal dichalcogenides (TMDs) are dressed by a remote cloud of phonons in the adjacent hexagonal boron nitride slab. Using angle resolved photoemission, we identify replica bands in the TMDs which are a clear fingerprint of long-range electron-phonon interaction. We develop a modified Fr\"ohlich model that shows semi-quantitative agreement with the experimental spectral functions. Our analysis shows that remote electron-phonon coupling is a generic property of interfaces with hBN. This has implications for electron mobilities in 2D materials, for superconductivity and possibly for moir\'e correlated phases.

cond-mat.mtrl-sci

Non-Fermi liquid quasiparticles in strain-tuned Sr2RuO4

Interacting electrons can form metallic states beyond the Fermi liquid paradigm, a conceptual frontier of many-body physics mainly explored via bulk thermodynamics and transport. In contrast, the microscopics of anomalous single-particle excitations underlying non-Fermi liquid properties have largely remained in the dark. Here we spectroscopically map such quantum-critical excitations in Sr$_2$RuO$_4$ under uniaxial pressure, an experimental challenge overcome by technical advances combining focused ion beam micro-milling with laser angle resolved photoemission. We show that quasiparticle excitations acquire a non-Fermi liquid scattering rate near the critical point but remain remarkably robust throughout the transition. These experiments serve as a benchmark for the theory of anomalous metals and settle the long-standing question if quantum-critical systems host quasiparticle excitations.

cond-mat.str-el

Fermi surface and pseudogap in highly doped Sr$_{2}$IrO$_{4}$

The fate of the Fermi surface in bulk electron-doped Sr$_{2}$IrO$_{4}$ remains elusive, as does the origin and extension of its pseudogap phase. Here, we use high-resolution angle-resolved photoelectron spectroscopy (ARPES) to investigate the electronic structure of Sr$_{2-x}$La$_{x}$IrO$_{4}$ up to $x=0.2$, a factor of two higher than in previous work. We find that the antinodal pseudogap persists up to the highest doping level, and thus beyond the sharp increase in Hall carrier density to $\simeq 1+x$ recently observed above $x^{*}\simeq 0.16$ [Y.-T. Hsu et al., Nature Physics 20, 1593 (2024)]. This suggests that doped iridates host a unique phase of matter in which a large Hall density coexists with an anisotropic pseudogap, breaking up the Fermi surface into disconnected arcs. The temperature boundary of the pseudogap is $T^{*}\simeq 200$ K for $x=0.2$, comparable to cuprates and to the energy scale of short range antiferromagnetic correlations in cuprates and iridates.

cond-mat.str-el

Nature of metallic and insulating domains in the CDW system 1T-TaSe2

We study the electronic structure of bulk 1T-TaSe$_2$ in the charge density wave phase at low temperature. Our spatially and angle resolved photoemission (ARPES) data show insulating areas coexisting with metallic regions characterized by a chiral Fermi surface and moderately correlated quasiparticle bands. Additionally, high-resolution laser ARPES reveals variations in the metallic regions, with series of low-energy states, whose energy, number and dispersion can be explained by the formation of quantum well states of different thicknesses. Dynamical mean field theory calculations show that the observed rich behaviour can be rationalized by assuming occasional stacking faults of the charge density wave. Our results indicate that the diverse electronic phenomena reported previously in 1T-TaSe$_2$ are dictated by the stacking arrangement and the resulting quantum size effects while correlation effects play a secondary role.

cond-mat.str-el

Controlling crystal cleavage in Focused Ion Beam shaped specimens for surface spectroscopy

Our understanding of quantum materials is commonly based on precise determinations of their electronic spectrum by spectroscopic means, most notably angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). Both require atomically clean and flat crystal surfaces which traditionally are prepared by in-situ mechanical cleaving in ultrahigh vacuum chambers. We present a new approach that addresses three main issues of the current state-of-the-art methods: 1) Cleaving is a highly stochastic and thus inefficient process; 2) Fracture processes are governed by the bonds in a bulk crystal, and many materials and surfaces simply do not cleave; 3) The location of the cleave is random, preventing data collection at specified regions of interest. Our new workflow is based on Focused Ion Beam (FIB) machining of micro-stress lenses in which shape (rather than crystalline) anisotropy dictates the plane of cleavage, which can be placed at a specific target layer. As proof-of-principle we show ARPES results from micro-cleaves of Sr$_2$RuO$_4$ along the ac plane and from two surface orientations of SrTiO$_3$, a notoriously difficult to cleave cubic perovskite.

cond-mat.mtrl-sci

The fate of quasiparticles at high-temperature

We study the temperature evolution of quasiparticles in the correlated metal Sr$_2$RuO$_4$. Our angle resolved photoemission data show that quasiparticles persist up to temperatures above 200~K, far beyond the Fermi liquid regime. Extracting the quasiparticle self-energy we demonstrate that the quasiparticle residue $Z$ increases with increasing temperature. Quasiparticles eventually disappear on approaching the bad metal state of Sr$_2$RuO$_4$ not by losing weight but via excessive broadening from super-Planckian scattering. We further show that the Fermi surface of Sr$_2$RuO$_4$ - defined as the loci where the spectral function peaks - deflates with increasing temperature. These findings are in semi-quantitative agreement with dynamical mean field theory calculations.

cond-mat.str-el

Electronic structure of the highly conductive perovskite oxide SrMoO$_3$

We use angle-resolved photoemission to map the Fermi surface and quasiparticle dispersion of bulk-like thin films of SrMoO$_3$ grown by pulsed laser deposition. The electronic self-energy deduced from our data reveals weak to moderate correlations in SrMoO$_3$, consistent with our observation of well-defined electronic states over the entire occupied band width. We further introduce spectral function calculations that combine dynamical mean-field theory with an unfolding procedure of density functional calculations and demonstrate good agreement of this approach with our experiments.

cond-mat.str-el

Magnetic order, disorder, and excitations under pressure in the Mott insulator Sr$_2$IrO$_4$

Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr$_2$IrO$_4$ at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr$_2$IrO$_4$ under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered state beyond 18 GPa. A strong first-order structural phase transition drives the magnetic evolution at $\sim$10 GPa with reduced structural anisotropy in the IrO$_6$ cages, leading to increasingly isotropic exchange interactions between the Heisenberg spins and a spin-flip transition to $c$-axis-aligned antiferromagnetic order. In the disordered phase of Heisenberg $J_\mathrm{eff}=1/2$ pseudospins, the spin excitations are quasi-elastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr$_2$IrO$_4$.

cond-mat.str-el

Direct comparison of ARPES, STM, and quantum oscillation data for band structure determination in Sr$_2$RhO$_4$

Discrepancies in the low-energy quasiparticle dispersion extracted from angle resolved photoemission, scanning tunneling spectroscopy and quantum oscillation data are common and have long haunted the field of quantum matter physics. Here, we directly test the consistency of results from these three techniques by comparing data from the correlated metal Sr$_2$RhO$_4$. Using established schemes for the interpretation of the experimental data, we find good agreement for the Fermi surface topography and carrier effective masses. Hence, the apparent absence of such an agreement in other quantum materials, including the cuprates, suggests that the electronic states in these materials are of different, non-Fermi liquid like nature. Finally, we discuss the potential and challenges in extracting carrier lifetimes from photoemission and quasiparticle interference data.

cond-mat.str-el

Correlated electron metal properties of the honeycomb ruthenate Na$_2$RuO$_3$

We report the synthesis and characterisation of polycrystalline Na$_2$RuO$_3$, a layered material in which the Ru$^{4+}$ ($4d^4$ configuration) form a honeycomb lattice. The optimal synthesis condition was found to produce a nearly ordered Na$_2$RuO$_3$ ($C2/c$ phase), as assessed from the refinement of the time-of-flight neutron powder diffraction. Magnetic susceptibility measurements reveal a large temperature-independent Pauli paramagnetism ($χ_0 \sim 1.42(2)\times10^{-3}$ emu/mol Oe) with no evidence of magnetic ordering down to 1.5 K, and with an absence of dynamic magnetic correlations, as evidenced by neutron scattering spectroscopy. The intrinsic susceptibility ($χ_0$) together with the Sommerfeld coeficient of $γ=11.7(2)$ mJ/Ru mol K$^2$ estimated from heat capacity measurements, gives an enhanced Wilson ratio of $R_W\approx8.9(1)$, suggesting that magnetic correlations may be present in this material. While transport measurements on pressed pellets show nonmetallic behaviour, photoemission spectrocopy indicate a small but finite density of states at the Fermi energy, suggesting that the bulk material is metallic. Except for resistivity measurements, which may have been compromised by near surface and interface effects, all other probes indicate that Na$_2$RuO$_3$ is a moderately correlated electron metal. Our results thus stand in contrast to earlier reports that Na$_2$RuO$_3$ is an antiferromagnetic insulator at low temperatures.

cond-mat.str-el

Bulk and surface electronic structure of the dual-topology semimetal Pt2HgSe3

We report high-resolution angle resolved photoemission measurements on single crystals of Pt2HgSe3 grown by high-pressure synthesis. Our data reveal a gapped Dirac nodal line whose (001)-projection separates the surface Brillouin zone in topological and trivial areas. In the non-trivial $k$-space range we find surface states with multiple saddle-points in the dispersion resulting in two van Hove singularities in the surface density of states. Based on density functional theory calculations, we identify these surface states as signatures of a topological crystalline state which coexists with a weak topological phase.

cond-mat.mtrl-sci

Momentum-resolved lattice dynamics of parent and electron-doped Sr$_{2}$IrO$_{4}$

The mixing of orbital and spin character in the wave functions of the $5d$ iridates has led to predictions of strong couplings among their lattice, electronic and magnetic degrees of freedom. As well as realizing a novel spin-orbit assisted Mott-insulating ground state, the perovskite iridate Sr$_{2}$IrO$_{4}$ has strong similarities with the cuprate La$_{2}$CuO$_{4}$, which on doping hosts a charge-density wave that appears intimately connected to high-temperature superconductivity. These phenomena can be sensitively probed through momentum-resolved measurements of the lattice dynamics, made possible by meV-resolution inelastic x-ray scattering. Here we report the first such measurements for both parent and electron-doped Sr$_{2}$IrO$_{4}$. We find that the low-energy phonon dispersions and intensities in both compounds are well described by the same nonmagnetic density functional theory calculation. In the parent compound, no changes of the phonons on magnetic ordering are discernible within the experimental resolution, and in the doped compound no anomalies are apparent due to charge-density waves. These measurements extend our knowledge of the lattice properties of (Sr$_{1-x}$La$_{x}$)$_{2}$IrO$_{4}$ and constrain the couplings of the phonons to magnetic and charge order.

cond-mat.str-el

High-resolution photoemission on Sr2RuO4 reveals correlation-enhanced effective spin-orbit coupling and dominantly local self-energies

We explore the interplay of electron-electron correlations and spin-orbit coupling in the model Fermi liquid Sr2RuO4 using laser-based angle-resolved photoemission spectroscopy. Our precise measurement of the Fermi surface confirms the importance of spin-orbit coupling in this material and reveals that its effective value is enhanced by a factor of about two, due to electronic correlations. The self-energies for the $β$ and $γ$ sheets are found to display significant angular dependence. By taking into account the multi-orbital composition of quasiparticle states, we determine self-energies associated with each orbital component directly from the experimental data. This analysis demonstrates that the perceived angular dependence does not imply momentum-dependent many-body effects, but arises from a substantial orbital mixing induced by spin-orbit coupling. A comparison to single-site dynamical mean-field theory further supports the notion of dominantly local orbital self-energies, and provides strong evidence for an electronic origin of the observed non-linear frequency dependence of the self-energies, leading to `kinks' in the quasiparticle dispersion of Sr2RuO4.

cond-mat.str-el

Band Structure and Spin-Orbital Texture of the (111)-KTaO3 Two-Dimensional Electron Gas

Two-dimensional electron gases (2DEGs) in oxides show great potential for discovering new physical phenomena and at the same time hold promise for electronic applications. In this work we use angle resolved photoemission to determine the electronic structure of a 2DEG stabilized in the (111)-oriented surface of the strong spin orbit coupling material KTaO3. Our measurements reveal multiple sub-bands that emerge as a consequence of quantum confinement and form a six-fold symmetric Fermi surface. This electronic structure is well reproduced by self-consistent tight-binding supercell calculations. Based on these calculations we determine the spin and orbital texture of the 2DEG. We show that the 2DEG Fermi surface is derived from bulk J = 3/2 states and exhibits an unconventional anisotropic Rashba-like lifting of the spin-degeneracy. Spin-momentum locking holds only for high symmetry directions and a strong out-of-plane spin component renders the spin-texture three-fold symmetric. We find that the average spin-splitting on the Fermi surface is an order of magnitude larger than in SrTiO3, which should translate into an enhancement in the spin-orbitronic response of (111)-KTaO3 2DEG based devices.

cond-mat.mtrl-sci

In-situ strain-tuning of the metal-insulator-transition of Ca$_{2}$RuO$_{4}$ in angle-resolved photoemission experiments

We report the evolution of the $k$-space electronic structure of lightly doped bulk Ca$_{2}$RuO$_{4}$ with uniaxial strain. Using ultrathin plate-like crystals, we achieve strain levels up to $-4.1\%$, sufficient to suppress the Mott phase and access the previously unexplored metallic state at low temperature. Angle-resolved photoemission experiments performed while tuning the uniaxial strain reveal that metallicity emerges from a marked redistribution of charge within the Ru $t_{2g}$ shell, accompanied by a sudden collapse of the spectral weight in the lower Hubbard band and the emergence of a well defined Fermi surface which is devoid of pseudogaps. Our results highlight the profound roles of lattice energetics and of the multiorbital nature of Ca$_{2}$RuO$_{4}$ in this archetypal Mott transition and open new perspectives for spectroscopic measurements.

cond-mat.str-el

Persistence of antiferromagnetic order upon La substitution in the $4d^4$ Mott insulator Ca$_2$RuO$_4$

The chemical and magnetic structures of the series of compounds Ca$_{2-x}$La$_x$RuO$_4$ [$x = 0$, $0.05(1)$, $0.07(1)$, $0.12(1)$] have been investigated using neutron diffraction and resonant elastic x-ray scattering. Upon La doping, the low temperature S-Pbca space group of the parent compound is retained in all insulating samples [$x\leq0.07(1)$], but with significant changes to the atomic positions within the unit cell. These changes can be characterised in terms of the local RuO$_6$ octahedral coordination: with increasing doping the structure, crudely speaking, evolves from an orthorhombic unit cell with compressed octahedra to a quasi-tetragonal unit cell with elongated ones. The magnetic structure on the other hand, is found to be robust, with the basic $k=(0,0,0)$, $b$-axis antiferromagnetic order of the parent compound preserved below the critical La doping concentration of $x\approx0.11$. The only effects of La doping on the magnetic structure are to suppress the A-centred mode, favouring the B mode instead, and to reduce the Néel temperature somewhat. Our results are discussed with reference to previous experimental reports on the effects of cation substitution on the $d^4$ Mott insulator Ca$_2$RuO$_4$, as well as with regard to theoretical studies on the evolution of its electronic and magnetic structure. In particular, our results rule out the presence of a proposed ferromagnetic phase, and suggest that the structural effects associated with La substitution play an important role in the physics of the system.

cond-mat.str-el

Mott transition and collective charge pinning in electron doped Sr2IrO4

We studied the in-plane dynamic and static charge conductivity of electron doped Sr2IrO4 using optical spectroscopy and DC transport measurements. The optical conductivity indicates that the pristine material is an indirect semiconductor with a direct Mott-gap of 0.55 eV. Upon substitution of 2% La per formula unit the Mott-gap is suppressed except in a small fraction of the material (15%) where the gap survives, and overall the material remains insulating. Instead of a zero energy mode (or Drude peak) we observe a soft collective mode (SCM) with a broad maximum at 40 meV. Doping to 10% increases the strength of the SCM, and a zero-energy mode occurs together with metallic DC conductivity. Further increase of the La substitution doesn't change the spectral weight integral up to 3 eV. It does however result in a transfer of the SCM spectral weight to the zero-energy mode, with a corresponding reduction of the DC resistivity for all temperatures from 4 to 300 K. The presence of a zero-energy mode signals that at least part of the Fermi surface remains ungapped at low temperatures, whereas the SCM appears to be caused by pinning a collective frozen state involving part of the doped electrons.

cond-mat.str-el

Observation of out-of-plane spin texture in a SrTiO3 (111) two-dimensional electron gas

We explore the second order bilinear magnetoelectric resistance (BMER) effect in the d-electron-based two-dimensional electron gas (2DEG) at the SrTiO3 (111) surface. We find an evidence of a spin-split band structure with the archetypal spin-momentum locking of the Rashba effect for the in-plane component. Under an out-of-plane magnetic field, we find a BMER signal that breaks the six-fold symmetry of the electronic dispersion, which is a fingerprint for the presence of a momentum dependent out-of-plane spin component. Relativistic electronic structure calculations reproduce this spin-texture and indicate that the out-of-plane component is a ubiquitous property of oxide 2DEGs arising from strong crystal field effects. We further show that the BMER response of the SrTiO3 (111) 2DEG is tunable and unexpectedly large.

cond-mat.mes-hall