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Oliver J. Clark

Publications and source records attributed to Oliver J. Clark.

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Robust spin splitting and fermiology in a layered altermagnet

Altermagnetism defies conventional classifications of collinear magnetic phases, standing apart from ferromagnetism and antiferromagnetism with its unique combination of spin-dependent symmetries, net-zero magnetization, and anomalous Hall transport. Although altermagnetic states have been realized experimentally, their integration into functional devices has been hindered by the structural rigidity and poor tunability of existing materials. First, through cobalt intercalation of the superconducting 2H-NbSe$_2$ polymorph, we induce and stabilize a robust altermagnetic phase and using both theory and experiment, we directly observe the lifting of Kramers degeneracy. Additionally, we present spectroscopic insight into a previously hinted low-temperature phase, and provide evidence of its electronic origin. While shedding light on overlooked aspects of altermagnetism, these findings open pathways to spin-based technologies and lay a foundation for advancing the emerging field of altertronics.

cond-mat.str-el

Extreme Strain Controlled Correlated Metal-Insulator Transition in the Altermagnet CrSb

Correlated flat bands and altermagnetism are two important directions in quantum materials, centred respectively on interaction-dominated phases and symmetry-enforced spin-textured states, yet both derive from lattice symmetry and orbital hybridization. This common origin implies that extreme crystal distortion, by narrowing bandwidths, enhancing correlations and reshaping the symmetries of altermagnetic spin splittings, could unify flat-band and altermagnetic physics in a single material; in practice, however, achieving such large distortions in a crystalline altermagnet is a formidable challenge. Here we combine a dedicated strain device with a tailored single-crystal mounting scheme to impose a highly tensile strain gradient in bulk CrSb, a prototypical altermagnet, creating a near-surface layer in which the in-plane lattice is strongly distorted relative to the weakly strained bulk, while the average bulk distortion remains small. Angle-resolved photoemission reveals a reversible regime at moderate strain, where a deeper flat-band feature, attributed to a strain-gradient-driven suppression of Cr-Sb hybridization, coexists with a correlation-enhanced Cr 3d flat band, and an irreversible regime at larger strain where partial bond decoupling drives a predominantly insulating spectral response. Density-functional calculations show that an orbital-selective altermagnetic spin texture persists across this correlated regime despite strong bandwidth renormalisation. These results define a strain-symmetry-correlation map for CrSb and establish extreme tensile strain as a route to co-engineer flat-band tendencies and spin-textured, zero-net-moment correlated states in altermagnets, pointing toward strain-adaptive, spin-selective Mott filtering and related device concepts.

cond-mat.str-el

Spin Texture Control and Magnetic Gap Engineering in a Ferromagnetic Insulator-Topological Insulator Sandwiched Heterostructure

Quantum materials combining magnetism and topological fermions are a key platform for low-energy electronics, spintronics, and quantum phases that break time-reversal symmetry (TRS), such as the quantum anomalous Hall effect (QAHE). Coupling a topological insulator to a magnetic material allows proximity magnetization with the potential to achieve these phases at elevated temperatures. One potential architecture for realizing QAHE at elevated temperature is a heterostructure comprising two single-septuple layers (1SL) of MnBi2Te4 (a 2D ferromagnetic insulator) with four-quintuple layer (4QL) Bi2Te3 in the middle. However, the origin of this gap has not yet been explicitly determined, as there are other non-magnetic mechanisms that have been shown to produce bandgaps in similar systems. Here, through spin- and angle-resolved photoemission, the magnetic nature of the gap opening is investigated to demonstrates direct control of the spin state via small magnetic fields and confirm the magnetic origin of the gap through spin splitting and broken TRS. Furthermore, the hallmark chiral spin texture of non-magnetic topological insulators is preserved away from the Γ-point, despite the large 72+/-10 meV exchange gap at the Dirac point. The robust magnetic gap and controllable spin texture hold significant promise for future technologies requiring both magnetic properties and topological protection.

cond-mat.mtrl-sci

Spin-polarised surface fermiology of ohmic WSe$_2$/NbSe$_2$ interfaces

Discovering and engineering spin-polarised surface states in the electronic structures of condensed matter systems is a crucial first step in development of spintronic devices, wherein spin-polarised bands crossing the Fermi level can facilitate information transfer. Here, we show how the spin-orbit split K-point valleys of monolayer WSe$_2$ can be made potentially suitable for this purpose, despite the semiconducting ground state. By interfacing with metallic 2H-NbSe$_2$, these valence band extrema are shifted by $\sim$800~meV to produce a surface-localised Fermi surface populated only by spin-polarised carriers. By increasing the WSe$_2$ thickness, the Fermi pockets can be moved from K to $Γ$, demonstrating tunability of novel semi-metallic phases that exist atop a substrate additionally possessing charge density wave and superconducting transitions. Together, this study provides spectroscopic understanding into $p$-type, Schottky barrier-free interfaces, which are of urgent interest for bypassing the limitations of current-generation vertical field effect transistors, in addition to longer-term spintronics development.

cond-mat.mtrl-sci

Designer three-dimensional electronic bands in asymmetric transition metal dichalcogenide heterostructures

Van der Waals materials enable the construction of atomically sharp interfaces between compounds with distinct crystal and electronic properties. This is dramatically exploited in moiré systems, where a lattice mismatch or twist between monolayers generates an emergent in-plane periodicity, giving rise to electronic properties absent in the constituent materials. In contrast, vertical superlattices, formed by stacking dissimilar materials in the out-of-plane direction on the nanometer scale, have received far less attention despite their potential to realize analogous emergent phenomena in three dimensions. Through angle-resolved photoemission spectroscopy and density functional theory, we investigate six-to-eight-layer transition metal dichalcogenide (TMD) heterostructures constructed from pairs of stacked few-layer materials. Counterintuitively, we find that even these single superlattice units can host fully-delocalised bands, evidencing a robust coherent interlayer coupling across lattice-mismatched interfaces over extended spatial scales. We show how uncompensated semimetallic phases and energetically-mismatched topological surface states are readily and exclusively stabilized within such asymmetrical architectures. These findings establish two-component heterostructures in the intermediate layer-regime as platforms to invoke and control unprecedented combinations and instances of the diverse quantum phases native to many-layer TMDs.

cond-mat.mtrl-sci

Anomalous spin-optical helical effect in Ti-based kagome metal

The kagome lattice stands as a rich platform for hosting a wide array of correlated quantum phenomena, ranging from charge density waves and superconductivity to electron nematicity and loop current states. Direct detection of loop currents in kagome systems has remained a formidable challenge due to their intricate spatial arrangements and the weak magnetic field signatures they produce. This has left their existence and underlying mechanisms a topic of intense debate. In this work, we uncover a hallmark reconcilable with loop currents: spin handedness-selective signals that surpass conventional dichroic, spin, and spin-dichroic responses. We observe this phenomenon in the kagome metal CsTi$_3$Bi$_5$ and we call it the anomalous spin-optical helical effect. This effect arises from the coupling of light' s helicity with spin-orbital electron correlations, providing a groundbreaking method to visualize loop currents in quantum materials. Our discovery not only enriches the debate surrounding loop currents but also paves the way for new strategies to exploit the electronic phases of quantum materials via light-matter interaction.

cond-mat.str-el

Angle-resolved photoemission of topological materials

Topological materials have gained significant attention in condensed matter physics due to their unique electronic and transport properties. Three-dimensional (3D) topological materials are characterized by robust electronic states that are protected by symmetries and exhibit peculiar spin textures. They offer a rich platform for for future information technology including spintronics and topological quantum computing. Here, we review the investigation by angle-resolved photoelectron spectroscopy (ARPES) of topological phases such as strong topological insulators, topological crystalline insulators, magnetic topological insulators, and 3D Dirac, Weyl, nodal, and chiral semimetals and address the status of correlated topological insulators and topological superconductors. A special emphasis is laid on examples from the transition metal dichalcogenide family. Moreover, insights from ultrafast pump-probe experiments are reviewed and a brief outlook is provided.

cond-mat.mtrl-sci

Bilayer orthogonal ferromagnetism in CrTe$_2$-based van der Waals system

Systems with pronounced spin anisotropy play a pivotal role in advancing magnetization switching and spin-wave generation mechanisms, which are fundamental for spintronic technologies. Quasi-van der Waals ferromagnets, particularly Cr$_{1+δ}$Te$_2$ compounds, represent seminal materials in this field, renowned for their delicate balance between frustrated layered geometries and magnetism. Despite extensive investigation, the precise nature of their magnetic ground state, typically described as a canted ferromagnet, remains contested, as does the mechanism governing spin reorientation under external magnetic fields and varying temperatures. In this work, we leverage a multimodal approach, integrating complementary techniques, to reveal that Cr$_{1+δ}$Te$_2$ ($δ= 0.25 - 0.50$) hosts a previously overlooked magnetic phase, which we term orthogonal-ferromagnetism. This single phase consists of alternating atomically sharp single layers of in-plane and out-of-plane ferromagnetic blocks, coupled via exchange interactions and as such, it differs significantly from crossed magnetism, which can be achieved exclusively by stacking multiple heterostructural elements together. Contrary to earlier reports suggesting a gradual spin reorientation in CrTe$_2$-based systems, we present definitive evidence of abrupt spin-flop-like transitions. This discovery, likely due to the improved crystallinity and lower defect density in our samples, repositions Cr$_{1+δ}$Te$_2$ compounds as promising candidates for spintronic and orbitronic applications, opening new pathways for device engineering.

cond-mat.str-el

Charge transfer and Spin-Valley locking in 4Hb-TaS$_{2}$

4Hb-TaS$_2$ is a superconductor that exhibits unique characteristics such as time-reversal symmetry breaking, hidden magnetic memory, and topological edge modes. It is a naturally occurring heterostructure comprising of alternating layers of 1H-TaS$_2$ and 1T-TaS$_2$. The former is a well-known superconductor, while the latter is a correlated insulator with a possible non-trivial magnetic ground state. In this study, we use angle resolved photoemission spectroscopy to investigate the normal state electronic structure of this unconventional superconductor. Our findings reveal that the band structure of 4H-TaS$_2$ fundamentally differs from that of its constituent materials. Specifically, we observe a significant charge transfer from the 1T layers to the 1H layers that drives the 1T layers away from half-filling. In addition, we find a substantial reduction in inter-layer coupling in 4Hb-TaS$_2$ compared to the coupling in 2H-TaS$_2$ that results in a pronounced spin-valley locking within 4Hb-TaS$_2$

cond-mat.supr-con

Magnetic Dirac semimetal state of (Mn,Ge)Bi$_2$Te$_4$

For quantum electronics, the possibility to finely tune the properties of magnetic topological insulators (TIs) is a key issue. We studied solid solutions between two isostructural Z$_2$ TIs, magnetic MnBi$_2$Te$_4$ and nonmagnetic GeBi$_2$Te$_4$, with Z$_2$ invariants of 1;000 and 1;001, respectively. For high-quality, large mixed crystals of Ge$_x$Mn$_{1-x}$Bi$_2$Te$_4$, we observed linear x-dependent magnetic properties, composition-independent pairwise exchange interactions along with an easy magnetization axis. The bulk band gap gradually decreases to zero for $x$ from 0 to 0.4, before reopening for $x>0.6$, evidencing topological phase transitions (TPTs) between topologically nontrivial phases and the semimetal state. The TPTs are driven purely by the variation of orbital contributions. By tracing the x-dependent $6p$ contribution to the states near the fundamental gap, the effective spin-orbit coupling variation is extracted. As $x$ varies, the maximum of this contribution switches from the valence to the conduction band, thereby driving two TPTs. The gapless state observed at $x=0.42$ closely resembles a Dirac semimetal above the Neel temperature and shows a magnetic gap below, which is clearly visible in raw photoemission data. The observed behavior of the Ge$_x$Mn$_{1-x}$Bi$_2$Te$_4$ system thereby demonstrates an ability to precisely control topological and magnetic properties of TIs.

cond-mat.mtrl-sci

Rashba-like spin textures in Graphene promoted by ferromagnet-mediated Electronic-Hybridization with heavy metal

Epitaxial graphene/ferromagnetic metal (Gr/FM) heterostructures deposited onto heavy metals (HM) have been proposed for the realization of novel spintronic devices because of their perpendicular magnetic anisotropy and sizeable Dzyaloshinskii-Moriya interaction (DMI), allowing for both enhanced thermal stability and stabilization of chiral spin textures. However, establishing routes towards this goal requires the fundamental understanding of the microscopic origin of their unusual properties. Here, we elucidate the nature of the induced spin-orbit coupling (SOC) at Gr/Co interfaces on Ir. Through spin- and angle-resolved photoemission along with density functional theory, we show that the interaction of the HM with the C atomic layer via hybridization with the FM is the source of strong SOC in the Gr layer. Furthermore, our studies on ultrathin Co films underneath Gr reveal an energy splitting of $\sim$\,100 meV (negligible) for in-plane (out-of-plane) spin polarized Gr $π$ bands, consistent with a Rashba-SOC at the Gr/Co interface, which is either the fingerprint or the origin of the DMI. This mechanism vanishes at large Co thicknesses, where neither in-plane nor out-of-plane spin-orbit splitting is observed, indicating that Gr $π$ states are electronically decoupled from the HM. The present findings are important for future applications of Gr-based heterostructures in spintronic devices.

cond-mat.mtrl-sci

Coexistence of bulk-nodal and surface-nodeless Cooper pairings in a superconducting Dirac semimetal

The interplay of nontrivial topology and superconductivity in condensed matter physics gives rise to exotic phenomena. However, materials are extremely rare where it is possible to explore the full details of the superconducting pairing. Here, we investigate the momentum dependence of the superconducting gap distribution in a novel Dirac material PdTe. Using high resolution, low temperature photoemission spectroscopy, we establish it as a spin-orbit coupled Dirac semimetal with the topological Fermi arc crossing the Fermi level on the (010) surface. This spin-textured surface state exhibits a fully gapped superconducting Cooper pairing structure below Tc~4.5K. Moreover, we find a node in the bulk near the Brillouin zone boundary, away from the topological Fermi arc.These observations not only demonstrate the band resolved electronic correlation between topological Fermi arc states and the way it induces Cooper pairing in PdTe, but also provide a rare case where surface and bulk states host a coexistence of nodeless and nodal gap structures enforced by spin-orbit coupling.

cond-mat.supr-con

Hidden spin-orbital texture at the $\barΓ$-located valence band maximum of a transition metal dichalcogenide semiconductor

Finding stimuli capable of driving an imbalance of spin-polarised electrons within a solid is the central challenge in the development of spintronic devices. However, without the aid of magnetism, routes towards this goal are highly constrained with only a few suitable pairings of compounds and driving mechanisms found to date. Here, through spin- and angle-resolved photoemission along with density functional theory, we establish how the $p$-derived bulk valence bands of semiconducting 1T-HfSe$_2$ possess a local, ground-state spin texture spatially confined within each Se-sublayer due to strong sublayer-localised electric dipoles orientated along the $c$-axis. This hidden spin-polarisation manifests in a `coupled spin-orbital texture' with in-equivalent contributions from the constituent $p$-orbitals. While the overall spin-orbital texture for each Se sublayer is in strict adherence to time-reversal symmetry (TRS), spin-orbital mixing terms with net polarisations at time-reversal invariant momenta are locally maintained. These apparent TRS-breaking contributions dominate, and can be selectively tuned between with a choice of linear light polarisation, facilitating the observation of pronounced spin-polarisations at the Brillouin zone centre for all $k_z$. We discuss the implications for the generation of spin-polarised populations from 1T-structured transition metal dichalcogenides using a fixed energy, linearly polarised light source.

cond-mat.mtrl-sci

Emergence of Fermi arcs and novel magnetic splitting in an antiferromagnet

The Fermi arcs are signatures of exotic states in solids because they defy conventional concept of Fermi surfaces as closed contours in momentum space. Fermi arcs were first discovered in cuprates, and caused by the pseudogap. Weyl semimetals provided another way to generate Fermi arcs by breaking either the time reversal symmetry (TRS) or inversion symmetry of a 3D Dirac semimetal, which can result in a Weyl semimetal with pairs of Weyl nodes that have opposite chirality. The bulk-boundary correspondence associated with the Chern number leads to the emergence of Fermi arcs on the boundary. Here, we present experimental evidence that pairs of magnetically split hole- and electron-like Fermi arcs emerge below the Neel temperature, in the antiferromagnetic (AFM) state of cubic NdBi due to a novel band splitting effect. Whereas TRS is broken by the AFM order, both inversion and nonsymmorphic TRS are preserved in the bulk, precluding the possibility of a Weyl semimetal. The observed magnetic splitting is highly unusual, as it creates bands of opposing curvature, that changes with temperature and follows the antiferromagnetic order parameter. This is completely different from previously reported cases of magnetic splittings such as traditional Zeeman and Rashba, where the curvature of the bands is preserved. Therefore, our finding represents a new Fermionic state created by new type of magnetic band splitting in the presence of a long-range AFM order that are not readily explained by existing theoretical ideas.

cond-mat.str-el

Tuneable electron-magnon coupling of ferromagnetic surface states in PdCoO$_2$

Controlling spin wave excitations in magnetic materials underpins the burgeoning field of magnonics. Yet, little is known about how magnons interact with the conduction electrons of itinerant magnets, or how this interplay can be controlled. Via a surface-sensitive spectroscopic approach, we demonstrate a strong and highly-tuneable electron-magnon coupling at the Pd-terminated surface of the delafossite oxide PdCoO$_2$, where a polar surface charge mediates a Stoner transition to itinerant surface ferromagnetism. We show how the coupling can be enhanced 7-fold with increasing surface disorder, and concomitant charge carrier doping, becoming sufficiently strong to drive the system into a polaronic regime, accompanied by a significant quasiparticle mass enhancement. Our study thus sheds new light on electron-magnon interactions in solid-state materials, and the ways in which these can be controlled.

cond-mat.str-el

Changes of Fermi Surface Topology due to the Rhombohedral Distortion in SnTe

Stoichiometric SnTe is theoretically a small gap semiconductor that undergoes a ferroelectric distortion on cooling. In reality however, crystals are always non-stoichiometric and metallic; the ferroelectric transition is therefore more accurately described as a polar structural transition. Here we study the Fermi surface using quantum oscillations as a function of pressure. We find the oscillation spectrum changes at high pressure, due to the suppression of the polar transition and less than 10 kbar is sufficient to stabilize the undistorted cubic lattice. This is accompanied by a large decrease in the Hall and electrical resistivity. Combined with our density functional theory (DFT) calculations and angle resolved photoemission spectroscopy (ARPES) measurements this suggests the Fermi surface $L$-pockets have lower mobility than the tubular Fermi surfaces that connect them. Also captured in our DFT calculations is a small widening of the band gap and shift in density of states for the polar phase. Additionally we find the unusual phenomenon of a linear magnetoresistance that exists irrespective of the distortion that we attribute to regions of the Fermi surface with high curvature.

cond-mat.str-el

Orbital- and $k_z$-selective hybridisation of Se 4p and Ti 3d states in the charge density wave phase of TiSe$_2$

We revisit the enduring problem of the $2\times{}2\times{}2$ charge density wave (CDW) order in TiSe$_2$, utilising photon energy-dependent angle-resolved photoemission spectroscopy to probe the full three-dimensional high- and low-temperature electronic structure. Our measurements demonstrate how a mismatch of dimensionality between the 3D conduction bands and the quasi-2D valence bands in this system leads to a hybridisation that is strongly $k_z$-dependent. While such a momentum-selective coupling can provide the energy gain required to form the CDW, we show how additional "passenger" states remain, which couple only weakly to the CDW and thus dominate the low-energy physics in the ordered phase of TiSe$_2$.

cond-mat.str-el