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Niels B. M. Schröter

Publications and source records attributed to Niels B. M. Schröter.

At least 19 recordsLinked to original sources

Change in charge density wave order beyond the Lifshitz transition in 2H-Ta\textsubscript{1$\pmδ$}S\textsubscript{2}

We investigate electronic instabilities in 2H-TaS\textsubscript{2} and a self-intercalated variant, 2H$^\dagger$-Ta\textsubscript{1+$δ$}S\textsubscript{2}. In conventional samples, which we determine to be slightly hole-doped, spectral gaps and backfolded features are found as fingerprints of the $3\times3$ charge density wave (CDW). Notably, the backfolded features emerge only at a temperatures below $T\approx$~65~K, substantially lower than the established CDW temperature of 78~K, suggesting an incommensurate-commensurate lock-in transition analogous to the phenomenology of the 2H-TaSe\textsubscript{2}. In contrast, the self-intercalated 2H$^\dagger$ sample exhibits substantial electron doping and signatures of a novel \tworootthree CDW. Using \textit{ab initio} calculations of the phonon spectrum, we demonstrate that the \threebythree instability ($\mathbf{q}=\sfrac{2}{3}\mathbf{ΓM}$) is highly sensitive to band filling. Furthermore, with increased interlayer spacing, a competing soft phonon mode emerges near $\mathbf{q}=\sfrac{1}{2}\mathbf{ΓK}$, corresponding to the superstructure observed in the 2H$^\dagger$ phase, although in our calculations this instability arises under hole doping rather than the electron doping inferred experimentally. These results establish band filling and interlayer spacing as key control parameters for CDW ordering vectors in 2H-TaS\textsubscript{2}, and highlight a route to engineering electronic instabilities in a prototypical layered material.

cond-mat.str-el↗

Quantifying quasiparticle chirality in a chiral topological semimetal

Recently, the projection of the electron's spin on its crystal momentum has been proposed as a metric to quantify electronic chirality of Bloch states in crystals, which is expected to affect a wide range of physical properties, such as magnetoelectric and optical responses. However, a direct experimental quantification of this chirality metric over an entire iso-energy surface has remained elusive. Here, we have used spin- and angle-resolved photoemission spectroscopy to directly probe the electronic chirality by measuring the bulk spin texture of Kramers-Weyl and Weyl cones in RhSi, a chiral topological semimetal with strong spin-orbit coupling (SOC). After quantifying the SOC splitting of Weyl cones, we determine their spin direction along different azimuthal angles to extract energy dependent the deviations (up to ~40°) from perfect parallel spin-momentum locking. From these deviations we define an energy-dependent normalized electron chirality density (NECD), a directly accessible metric of bulk electronic chirality. In RhSi, the NECD decreases from 1 at the Kramers-Weyl point to ~0.8 at ~200 meV below it. Finally, we show that this experimentally grounded NECD provides predictive power for magneto-optical and transport responses of chiral materials, exemplified by the longitudinal Edelstein effect.

cond-mat.mes-hall↗

Suppression of Spectral Gap and Flat Bands on a Cuprate Superconductor Side-Surface

Side surfaces of cuprate superconductors are expected to display a suppressed $d$-wave order parameter and zero-energy topological flat bands with a large density of states, making them susceptible to symmetry broken orders. Yet such surfaces have never been investigated with momentum-resolved, surface-sensitive probes, because high-temperature superconductors rarely cleave along them. Using focused-ion-beam milling to define a controlled breaking point, we expose pristine (110) side surfaces of overdoped La$_{2-x}$Sr$_x$CuO$_4$ ($x=0.22$) suitable for angle-resolved photoemission. We observe the suppression of the superconducting spectral gap within our energy resolution ($\sim 4~\mathrm{meV}$), and surprisingly, the expected zero-energy flat band peak is also suppressed, despite the high topographic quality of the surface. Self-consistent Bogoliubov--de~Gennes calculations show that the measured geometric roughness of the cleaved surface is too weak to eliminate these modes. The calculations further demonstrate that bulk inhomogeneities characteristic of high-temperature superconductors, modelled as moderate Anderson-type disorder, can broaden the flat-band states beyond detectability. Our results provide the first momentum-resolved view of the electronic structure on a cuprate side surface and reveal disorder as the key factor currently preventing appearance of flat bands and their associated correlated orders.

cond-mat.supr-con↗

Charge transfer empties the flat band in 4H$_b$-TaS$_2$ -- except at the surface

The 4H\textsubscript{b} polytype of TaS$_2$ is a natural heterostructure of H and T-type layers. Intriguing recent evidence points towards a possibly chiral superconducting ground state, unlike the superconductivity found in other polytypes where the T layers are absent, requiring understanding of the possible contributions of electrons from the T layers. Here we use micro-focused angle resolved photoemission spectroscopy to reveal that the T termination of the 4H\textsubscript{b} structure is metallic, but a subsurface T layer -- seen below an H termination and thus more representative of the bulk case -- is gapped. The results imply a complete charge transfer of 1 electron per 13 Ta from the T to adjacent H layers in the bulk, but an incomplete charge transfer at the T termination, yielding a metallic Fermi surface with a planar-chiral character. A similar metallic state is found in an anomalous region with likely T-H-H' stacking at the surface. Our results exclude cluster Mott localisation in either the bulk or surface of 4H$_b$-TaS$_2$ and point to a scenario of superconductivity arising from Josephson-like tunneling between the H layers.

cond-mat.supr-con↗

Tunable Octdong and Spindle-Torus Fermi Surfaces in Kramers Nodal Line Metals

It has recently been proposed that all achiral non-centrosymmetric crystals host so-called Kramers nodal lines, which are doubly degenerate band crossings connecting time-reversal invariant momenta in the Brillouin zone that arise due to spin-orbit coupling. When Kramers nodal lines intersect the Fermi level, they form exotic three-dimensional Fermi surfaces which is certain configurations can be fully described by two-dimensional massless Dirac fermions. These Fermi surfaces are predicted to realize a quantized optical conductivity with multiple quantized levels a large light- and field-induced anomalous Hall effect. However, until now, no Kramers nodal line metal with such unconventional Fermi surfaces has been experimentally observed. Here, we extend the search for Kramers nodal line metals beyond the previously considered case in which the Fermi surfaces enclose a single time-reversal invariant momentum. Using angle-resolved photoelectron spectroscopy measurements and ab-initio calculations, we present evidence that the 3R polytypes of TaS$_2$ and NbS$_2$ are Kramers nodal line metals with open Octdong and Spindle-torus Fermi surfaces, respectively. We show that by reducing the band filling, a transition between these two configurations can be observed. Moreover, our data suggests a naturally occurring size quantization effect of inclusions of 3R-TaS$_2$ in commercially available 2H-TaS$_2$ crystals, which could enable the observation of quantized optical conductivity. Finally, since the open Fermi-surfaces encircle two time-reversal invariant momenta each, we predict a phase transition from a Kramers nodal line metal to a conventional metal by strain or uniaxial pressure. Our work establishes the 3R phase of metallic transition metal dichalcogenides as a tunable platform to explore new phenomena expected from exotic Fermi surfaces in Kramers nodal line metals.

cond-mat.mtrl-sci↗

Momentum-Resolved Fingerprint of Mottness in Layer-Dimerized Nb$_3$Br$_8$

In a well-ordered crystalline solid, insulating behaviour can arise from two mechanisms: electrons can either scatter off a periodic potential, thus forming band gaps that can lead to a band insulator, or they localize due to strong interactions, resulting in a Mott insulator. For an even number of electrons per unit cell, either band- or Mott-insulators can theoretically occur. However, unambiguously identifying an unconventional Mott-insulator with an even number of electrons experimentally has remained a longstanding challenge due to the lack of a momentum-resolved fingerprint. This challenge has recently become pressing for the layer dimerized van der Waals compound Nb$_3$Br$_8$, which exhibits a puzzling magnetic field-free diode effect when used as a weak link in Josephson junctions, but has previously been considered to be a band-insulator. In this work, we present a unique momentum-resolved signature of a Mott-insulating phase in the spectral function of Nb$_3$Br$_8$: the top of the highest occupied band along the out-of-plane dimerization direction $k_z$ has a momentum space separation of $Δk_z=2π/d$, whereas the valence band maximum of a band insulator would be separated by less than $Δk_z=π/d$, where $d$ is the average spacing between the layers. As the strong electron correlations inherent in Mott insulators can lead to unconventional superconductivity, identifying Nb$_3$Br$_8$ as an unconventional Mott-insulator is crucial for understanding its apparent time-reversal symmetry breaking Josephson diode effect. Moreover, the momentum-resolved signature employed here could be used to detect quantum phase transition between band- and Mott-insulating phases in van der Waals heterostructures, where interlayer interactions and correlations can be easily tuned to drive such transition.

cond-mat.str-el↗

Novel electronic structures from anomalous stackings in NbS$_2$ and MoS$_2$

We show that in some transition metal dichalcogenides, minority regions of the cleaved sample surfaces show - unexpectedly and anomalously - a finite number of 2D electronic states instead of the expected 3D valence bands. In the case of NbS\textsubscript{2}, in addition to the typical spectrum associated with bulk 2Ha stacking, we also find minority regions with electronic structures consistent with few-layers of 3R stacking. In MoS\textsubscript{2} we find areas of both bulk 2Hc and 3R stackings, and regions exhibiting finite-layer quantisation of both types. We further find evidence for a more exotic 4Ha stacking of MoS\textsubscript{2}, in which the valence band maximum is quasi-2D. The results highlight how variation of the interlayer stacking of van der Waals materials beyond the commonly-reported bulk polytypes can yield novel electronic structures.

cond-mat.str-el↗

Controllable orbital angular momentum monopoles in chiral topological semimetals

The emerging field of orbitronics aims at generating and controlling currents of electronic orbital angular momentum (OAM) for information processing. Structurally chiral topological crystals could be particularly suitable orbitronic materials because they have been predicted to host topological band degeneracies in reciprocal space that are monopoles of OAM. Around such a monopole, the OAM is locked isotopically parallel or antiparallel to the direction of the electron's momentum, which could be used to generate large and controllable OAM currents. However, OAM monopoles have not yet been directly observed in chiral crystals, and no handle to control their polarity has been discovered. Here, we use circular dichroism in angle-resolved photoelectron spectroscopy (CD-ARPES) to image OAM monopoles in the chiral topological semimetals PtGa and PdGa. Moreover, we also demonstrate that the polarity of the monopole can be controlled via the structural handedness of the host crystal by imaging OAM monopoles and anti-monopoles in the two enantiomers of PdGa, respectively. For most photon energies used in our study, we observe a sign change in the CD-ARPES spectrum when comparing positive and negative momenta along the light direction near the topological degeneracy. This is consistent with the conventional view that CD-ARPES measures the projection of the OAM monopole along the photon momentum. For some photon energies, however, this sign change disappears, which can be understood from our numerical simulations as the interference of polar atomic OAM contributions, consistent with the presence of OAM monopoles. Our results highlight the potential of chiral crystals for orbitronic device applications, and our methodology could enable the discovery of even more complicated nodal OAM textures that could be exploited for orbitronics.

cond-mat.str-el↗

Parallel spin-momentum locking in a chiral topological semimetal

Spin-momentum locking in solids describes a directional relationship between the electron's spin angular momentum and its linear momentum over the entire Fermi surface. While orthogonal spin-momentum locking, such as Rashba spin-orbit coupling, has been studied for decades and inspired a vast number of applications, its natural counterpart, the purely parallel spin-momentum locking, has remained elusive in experiments. Recently, chiral topological semimetals that host single- and multifold band crossings have been predicted to realize such parallel locking. Here, we use spin- and angle-resolved photoelectron spectroscopy to probe spin-momentum locking of a multifold fermion in the chiral topological semimetal PtGa via the spin-texture of its topological Fermi-arc surface states. We find that the electron spin of the Fermi-arcs points orthogonal to their Fermi surface contour for momenta close to the projection of the bulk multifold fermion, which is consistent with parallel spin-momentum locking of the latter. We anticipate that our discovery of parallel spin-momentum locking of multifold fermions will lead to the integration of chiral topological semimetals in novel spintronic devices, and the search for spin-dependent superconducting and magnetic instabilities in these materials.

cond-mat.mes-hall↗

Hydrogen-impurity induced unconventional magnetism in semiconducting molybdenum ditelluride

Layered transition-metal dichalcogenides are proposed as building blocks for van der Waals (vdW) heterostructures due to their graphene-like two dimensional structure. For this purpose, a magnetic semiconductor could represent an invaluable component for various spintronics and topotronics devices. Here, we combine different local magnetic probe spectroscopies with angle-resolved photoemission and density-functional theory calculations to show that 2H-MoTe2 is on the verge of becoming magnetic. Our results present clear evidence that the magnetism can be "switched on" by a hydrogen-like impurity. We also show that this magnetic state survives up to the free surface region, demonstrating the material's potential applicability as a magnetic component for thin-film heterostructures.

cond-mat.mtrl-sci↗

What's knot to like? Observation of a linked loop quantum state

Quantum phases can be classified by topological invariants, which take on discrete values capturing global information about the quantum state. Over the past decades, these invariants have come to play a central role in describing matter, providing the foundation for understanding superfluids, magnets, the quantum Hall effect, topological insulators, Weyl semimetals and other phenomena. Here we report a remarkable linking number (knot theory) invariant associated with loops of electronic band crossings in a mirror-symmetric ferromagnet. Using state-of-the-art spectroscopic methods, we directly observe three intertwined degeneracy loops in the material's bulk Brillouin zone three-torus, $\mathbb{T}^3$. We find that each loop links each other loop twice. Through systematic spectroscopic investigation of this linked loop quantum state, we explicitly draw its link diagram and conclude, in analogy with knot theory, that it exhibits linking number $(2,2,2)$, providing a direct determination of the invariant structure from the experimental data. On the surface of our samples, we further predict and observe Seifert boundary states protected by the bulk linked loops, suggestive of a remarkable Seifert bulk-boundary correspondence. Our observation of a quantum loop link motivates the application of knot theory to the exploration of exotic properties of quantum matter.

cond-mat.mes-hall↗

Spin-momentum locking from topological quantum chemistry: applications to multifold fermions

In spin-orbit coupled crystals, symmetries can protect multifold degeneracies with large Chern numbers and Brillouin zone spanning topological surface states. In this work, we explore the extent to which the nontrivial topology of chiral multifold fermions impacts the spin texture of bulk states. To do so, we formulate a definition of spin-momentum locking in terms of reduced density matrices. Using tools from the theory of topological quantum chemistry, we show how the reduced density matrix can be determined from the knowledge of the basis orbitals and band representation forming the multifold fermion. We show how on-site spin orbit coupling, crystal field splitting, and Wyckoff position multiplicity compete to determine the spin texture of states near chiral fermions. We compute the spin texture of multifold fermions in several representative examples from space groups $P432$ (207) and $P2_13$ (198). We show that the winding number of the spin around the Fermi surface can take many different integer values, from zero all the way to $\pm 7$. Finally, we conclude by showing how to apply our theory to real materials using the example of PtGa in space group $P2_13$.

cond-mat.mes-hall↗

Josephson diode effect from Cooper pair momentum in a topological semimetal

In the presence of an external magnetic field Cooper pairs in noncentrosymmetric superconductors can acquire finite momentum. Recent theory predicts that such finite-momentum pairing can lead to an asymmetric critical current, where a dissipationless supercurrent can flow along one direction but not the opposite. However, to date this has not been observed. Here we report the discovery of a giant Josephson diode effect (JDE) in Josephson junctions formed from a type II Dirac semimetal, NiTe2. A distinguishing feature is that the asymmetry in the critical current depends sensitively on the magnitude and direction of an applied magnetic field and achieves its maximum value of ~60% when the magnetic field is perpendicular to the current and is of the order of just 10 mT. Moreover the asymmetry changes sign several times with increasing field. These characteristic features are accounted for in a theoretical model based on finite-momentum Cooper pairing derived from spin-helical topological surface states, in an otherwise centrosymmetric system. The finite pairing momentum is further established, and its value determined, from the evolution of the interference pattern under an in-plane magnetic field. The observed giant magnitude of the asymmetry in critical current and the clear exposition of its underlying mechanism paves the way to building novel superconducting computing devices using the Josephson diode effect.

cond-mat.supr-con↗

Theoretical study of topological properties of ferromagnetic pyrite CoS$_2$

Since the discovery of the first topological material 15 years ago, the search for material realizations of novel topological phases has become the driving force of the field. While oftentimes we search for new materials, we forget that well established materials can also display very interesting topological properties. In this work, we revisit CoS$_2$ , a metallic ferromagnetic pyrite that has been extensively studied in the literature due to its magnetic properties. We study the topological features of its electronic band structure and identify Weyl nodes and Nodal lines, as well as a symmetry-protected 4-fold fermion close to the Fermi level. Looking at different surface cleavage planes, we observe both spin polarized Fermi arcs in the majority channel and drumhead states. These findings suggest that CoS$_2$ is a promising platform to study topological phenomena, as well as a good candidate for spintronic applications.

cond-mat.mtrl-sci↗

Electronic structure of InAs and InSb surfaces: density functional theory and angle-resolved photoemission spectroscopy

The electronic structure of surfaces plays a key role in the properties of quantum devices. However, surfaces are also the most challenging to simulate and engineer. Here, we study the electronic structure of InAs(001), InAs(111), and InSb(110) surfaces using a combination of density functional theory (DFT) and angle-resolved photoemission spectroscopy (ARPES). We were able to perform large-scale first principles simulations and capture effects of different surface reconstructions by using DFT calculations with a machine-learned Hubbard U correction [npj Comput. Mater. 6, 180 (2020)]. To facilitate direct comparison with ARPES results, we implemented a "bulk unfolding" scheme by projecting the calculated band structure of a supercell surface slab model onto the bulk primitive cell. For all three surfaces, we find a good agreement between DFT calculations and ARPES. For InAs(001), the simulations clarify the effect of the surface reconstruction. Different reconstructions are found to produce distinctive surface states. For InAs(111) and InSb(110), the simulations help elucidate the effect of oxidation. Owing to larger charge transfer from As to O than from Sb to O, oxidation of InAs(111) leads to significant band bending and produces an electron pocket, whereas oxidation of InSb(110) does not. Our combined theoretical and experimental results may inform the design of quantum devices based on InAs and InSb semiconductors, e.g., topological qubits utilizing the Majorana zero modes.

cond-mat.mtrl-sci↗

Observation and control of maximal Chern numbers in a chiral topological semimetal

Topological semimetals feature protected nodal band degeneracies characterized by a topological invariant known as the Chern number (C). Nodal band crossings with linear dispersion are expected to have at most |C|=4, which sets an upper limit to the magnitude of many topological phenomena in these materials. Here we show that the chiral crystal PdGa displays multifold band crossings, which are connected by exactly four surface Fermi-arcs, thus proving that they carry the maximal Chern number magnitude of 4. By comparing two enantiomers, we observe a reversal of their Fermi-arc velocities, which demonstrates that the handedness of chiral crystals can be used to control the sign of their Chern numbers.

cond-mat.mes-hall↗

Weyl-fermions, Fermi-arcs, and minority-spin carriers in ferromagnetic CoS2

The pyrite compound CoS2 has been intensively studied in the past due to its itinerant ferromagnetism and potential for half-metallicity, which make it a promising material for spintronic applications. However, its electronic structure remains only poorly understood. Here we use complementary bulk- and surface-sensitive angle-resolved photoelectron spectroscopy and ab-initio calculations to provide a complete picture of its band structure. We discover Weyl-cones at the Fermi-level, which presents CoS2 in a new light as a rare member of the recently discovered class of magnetic topological metals. We directly observe the topological Fermi-arc surface states that link the Weyl-nodes, which will influence the performance of CoS2 as a spin-injector by modifying its spin-polarization at interfaces. Additionally, we are for the first time able to directly observe a minority-spin bulk electron pocket in the corner of the Brillouin zone, which proves that CoS2 cannot be a true half-metal. Beyond settling the longstanding debate about half-metallicity in CoS2, our results provide a prime example of how the topology of magnetic materials can affect their use in spintronic applications.

cond-mat.mtrl-sci↗

Direct observation of handedness-dependent quasiparticle interference in the two enantiomers of topological chiral semimetal PdGa

It has recently been proposed that combining chirality with topological band theory may result in a totally new class of fermions. These particles have distinct properties: they appear at high symmetry points of the reciprocal lattice, they are connected by helicoidal surface Fermi arcs spanning the entire Brillouin zone, and they are expected to exist over a large energy range. Additionally, they are expected to give rise to totally new effects forbidden in other topological classes. Understanding how these unconventional quasiparticles propagate and interact is crucial for exploiting their potential in innovative chirality-driven device architectures. These aspects necessarily rely on the detection of handedness-dependent effects in the two enantiomers and remain largely unexplored so far. Here, we use scanning tunnelling microscopy to visualize the electronic properties of both enantiomers of the prototypical chiral topological semimetal PdGa at the atomic scale. We reveal that the surface-bulk connectivity goes beyond ensuring the existence of topological Fermi arcs, but also determines how quasiparticles propagate and scatter at impurities, giving rise to chiral quantum interference patterns of opposite handedness and opposite spiralling direction for the two different enantiomers, a direct manifestation of the change of sign of their Chern number. Additionally, we demonstrate that PdGa remains topologically non-trivial over a large energy range, experimentally detecting Fermi arcs in an energy window of more than 1.6 eV symmetrically centerd around the Fermi level. These results are rationalized in terms of the deep connection between chirality in real and reciprocal space in this class of materials, and they allow to identify PdGa as an ideal topological chiral semimetal.

cond-mat.mes-hall↗