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Craig Polley

Publications and source records attributed to Craig Polley.

At least 19 recordsLinked to original sources

Spin- and Angle-resolved Photoelectron Spectroscopy Study of the Quantum Spin Hall Insulator Bismuthene and its Precursor Phase

Recent studies have revealed that a confined bismuth layer at the graphene/SiC interface can be reversibly switched between a topologically trivial precursor phase and the quantum spin Hall insulator bismuthene. Here, we present a detailed spin- and angle-resolved photoelectron spectroscopy study of both structures, resolving the spin texture of their low-energy electronic states. Owing to the strong intrinsic spin-orbit coupling of bismuth and the asymmetric confinement potential at the interface, the valence bands of both structures are Rashba-split. We demonstrate the expected spin-momentum locking for both phases and Kramers' doublets through the investigation of the valence bands' spin polarization at multiple positions in reciprocal space.

cond-mat.mtrl-sci

Disentangling bulk and surface states in the electronic structure of PtBi$_2$(0001)

Recent reports of surface-localized topological superconductivity in trigonal PtBi$_2$ highlight the importance of understanding its surface electronic structure. We investigate the bulk and surface band structure of PtBi$_2$ using angle-resolved photoemission spectroscopy (ARPES) and first-principles calculations. Through photon-energy- and polarization-dependent measurements, we disentangle bulk dispersions from surface states on the two distinct surface terminations of PtBi$_2$(0001). For both terminations, we assign several different surface states and find good agreement between experiment and calculations. Based on our calculations, we analyze the orbital composition in the surface and bulk bands and compare the results to polarization-dependent ARPES measurements. Together, our results provide a coherent picture of the surface electronic structure of PtBi$_2$ across both surface terminations.

cond-mat.str-el

Fermiology and spin polarization of topological surface states in PtBi$_2$

Layered PtBi$_2$ is a candidate for topological superconductivity arising in Fermi-arc surface states. Using spin- and angle-resolved photoemission spectroscopy, we demonstrate that the Fermi arcs in PtBi$_2$ are singly degenerate and spin-polarized, which establishes their nontrivial topology and constitutes a necessary condition for topological superconductivity. We further uncover a pronounced surface-termination dependence of the Fermi-arc dispersion, yielding either nearly flat or approximately linear bands in agreement with first-principles calculations. Together, the observed spin polarization and termination-dependent bandwidth of the Fermi-arc surface states identify key ingredients underlying the potential emergence of topological superconductivity in PtBi$_2$.

cond-mat.supr-con

p-Wave Orbital Angular Momentum Texture in a Chiral Crystal

The spin and orbital angular momentum (SAM and OAM) are conceptually analogous, yet their roles in condensed matter systems have not been often treated on equal footing. While SAM has been extensively explored, OAM has long been regarded as quenched in crystalline environments and thus largely overlooked. Recent experimental and theoretical advances, however, have demonstrated that OAM can drive a variety of novel electronic phenomena, highlighting the importance of probing OAM textures in the electronic band structure. Here, we investigate the momentum-space OAM texture of (TaSe4)2I, a one-dimensional chiral crystal. Using circular-dichroism angle-resolved photoemission spectroscopy (CD-ARPES), we uncover a p-wave OAM texture accompanied by OAM dipole structures. This orbital p-wave texture is intimately connected to, and thus controllable by the chirality of the host lattice. Complementary spin-resolved ARPES measurements and first-principles calculations reveal that the OAM polarization overwhelmingly dominates the low-energy electronic properties of (TaSe4)2I, far exceeding the SAM polarization. These observations represent the experimental verification of a new type of OAM texture in crystalline materials. Most importantly, these findings underscore a promising material platform for spinless orbitronics applications and lay the foundation for realizing multipolar OAM textures-orbital counterparts of the spin texture in unconventional magnets.

cond-mat.mtrl-sci

Disentangling bulk and surface electronic structure using targeted cleave planes in RuO$_2$

Rutile RuO$_2$ has attracted significant interest due to its putative unconventional electronic and magnetic properties and its proximity to superconductivity. However, the measurement and interpretation of its electronic structure has been complicated by a strongly three-dimensional crystal structure. Here, we demonstrate how the preparation of targeted $(110)$ and $(100)$ surfaces via focused ion beam (FIB)-engineered cleaving allows the acquisition of high-quality measurements of the electronic structure using angle-resolved photoemission spectroscopy. Our results demonstrate that ARPES spectra of RuO$_2$ are, in fact, largely dominated by signatures of distinct surface electronic states. From comparison with density-functional theory, we resolve a surface termination-dependent variation of these, and disentangle them from highly-three-dimensional bulk states and surface resonances. Moreover, we find a marked role of the substantial spin-orbit coupling of the Ru 4$d$ orbitals in the surface region, where a breaking of spatial inversion symmetry leads to significant Rashba-type spin splittings of the surface bands.

cond-mat.str-el

A correlated insulator at the surface of the polar metal Ca$_3$Ru$_2$O$_7$

We investigate the electronic structure at the surface of the correlated oxide Ca$_3$Ru$_2$O$_7$, a low-symmetry ruthenate oxide which hosts an unconventional polar-metal phase. From a combination of angle-resolved photoemission spectroscopy and scanning tunneling spectroscopy measurements, we demonstrate that the surface hosts an insulating phase, a distinct departure from metallicity within the bulk. Utilizing quantitative low-energy electron diffraction in conjunction with electronic structure calculations, we show how this results from a combined surface structure relaxation and the impact of marked electronic correlations in this system. Our findings highlight the proximity of Ca$_3$Ru$_2$O$_7$ to an insulating metallic state, and illustrate how subtle structural distortions can control its emergent electronic phases.

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

Persistence of charge ordering instability to Coulomb engineering in the excitonic insulator candidate TiSe$_2$

TiSe$_2$ has long been considered one of the best candidate materials to host the elusive excitonic insulator (EI) phase. However, a finite coupling to the lattice can generically be expected, while a lack of "smoking-gun" signatures for the importance of the electron-hole interaction in driving the phase transition has rendered it challenging to distinguish the EI from the conventional charge-density-wave (CDW) phase. Here, we demonstrate a new approach, exploiting the susceptibility of excitons to dielectric screening. We combine mechanical exfoliation with molecular-beam epitaxy to fabricate ultra-clean van der Waals heterostructures of monolayer (ML-)TiSe$_2$/graphite and ML-TiSe$_2$/hBN. We observe how the modified substrate screening environment drives a renormalisation of the quasi-particle band gap of the TiSe$_2$ layer, signifying its susceptibility to Coloumb engineering. The temperature-dependent evolution of its electronic structure, however, remains unaffected, indicating that excitons are not required to drive the CDW transition in TiSe$_2$.

cond-mat.mtrl-sci

Charge transfer between van der Waals coupled metallic 2D layers

Van der Waals heterostructures have become a rapidly growing field in condensed matter research, offering a platform to engineer novel quantum systems by stacking different two-dimensional (2D) materials. A diverse range of material combinations, including hexagonal boron nitride, transition metal dichalcogenides and graphene, with electronic properties spanning from insulating to semiconducting, metallic, and semimetallic, have been explored to tune the properties of these heterostacks. However, understanding the interactions and charge transfer between the stacked layers remains challenging, particularly when more than two layers are involved. In this study, we investigate the charge transfer in a potassium-adlayer/graphene/lead-monolayer heterostructure stacked on a SiC substrate. Using synchrotron-based angle-resolved photoemission spectroscopy, we analyze the band structure of each layer, focusing on the charge transfer from K to the underlying 2D layers. Since K forms a $(2 \times 2)$ overlayer with respect to graphene, the amount of charge carriers donated by K can be determined. Our findings reveal that adsorption of K not only leads to a significant $n$-doping of the adjacent graphene layer but also to an electron transfer into the Pb monolayer. Remarkably, $\approx 44\%$ of the electrons donated by the K adlayer are transferred into its second nearest neighbouring layer, i.e. Pb, while $\approx 56\%$ remain in the graphene.

cond-mat.mes-hall

Fermiology and Band Structure of Oxygen-Terminated Ti3C2Tx MXene

The class of two-dimensional carbides and nitrides known as MXenes exhibit remarkable electronic properties. Tailoring these properties, however, requires an in-depth understanding of the band structure and Fermi-surface topology. Surface oxidation of MXenes has previously hampered the characterization of their Fermi surface, which is crucial for understanding the topology and anisotropy in the electronic structure and, ultimately, for tailoring electronic properties. Here, we reveal the Fermi surface topology and band structure of purely oxygen-terminated Ti3C2Tx MXene achieved through rigorous thin film sample preparation and ultrahigh vacuum annealing. Polarized synchrotron radiation-based angle-resolved photoemission spectroscopy reveals electron pockets, bulk band gaps, and a Dirac-like feature in the anisotropic electronic band structure. This paves the way for a fundamental understanding of band engineering of electronic transport properties, providing insights of importance for energy storage devices, transparent conductors, and catalysis.

cond-mat.mtrl-sci

Hund flat band in a frustrated spinel oxide

Electronic flat bands associated with quenched kinetic energy and heavy electron mass have attracted great interest for promoting strong electronic correlations and emergent phenomena such as high-temperature charge fractionalization and superconductivity. Intense experimental and theoretical research has been devoted to establishing the rich non-trivial metallic and heavy fermion phases intertwined with such localized electronic states. Here, we investigate the transition metal oxide spinel LiV2O4, an enigmatic heavy fermion compound lacking localized f orbital states. We use angle-resolved photoemission spectroscopy and dynamical mean field theory to reveal a new kind of correlation-induced flat band with suppressed inter-atomic electron hopping arising from intra-atomic Hund coupling. The appearance of heavy quasiparticles is ascribed to a proximate orbital-selective Mott state characterized by fluctuating local moments as evidenced by complementary magnetotransport measurements. The spectroscopic fingerprints of long-lived quasiparticles and their disappearance with increasing temperature further support the emergence of a high-temperature bad metal state observed in transport data. This work resolves a long-standing puzzle on the origin of heavy fermion behavior and unconventional transport in LiV2O4. Simultaneously, it opens a new path to achieving flat bands through electronic interactions in d-orbital systems with geometrical frustration, potentially enabling the realization of exotic phases of matter such as the fractionalized Fermi liquids.

cond-mat.str-el

Pb-intercalated epitaxial graphene on SiC: Full insight into band structure and orbital character of interlayer Pb, and charge transfer into graphene

Intercalation is a robust approach for modulating the properties of epitaxial graphene on SiC and stabilizing two-dimensional (2D) intercalant layers at the graphene/SiC interface. In this work, we present synchrotron-based angle resolved photoelectron spectroscopy (ARPES) measurements focussing on the band structure of intercalated Pb under a single layer of epitaxial graphene. The interlayer Pb exhibits a metallic character, a $(1 \times 1)$ registry with respect to SiC, and free electron-like bands to a first order. Divergences from the free electron approximation include various band splittings and gaps throughout the Pb Brillouin zone. Light polarization dependent ARPES measurements indicate a predominant out-of-plane orbital character for the Pb bands, suggesting potential interactions between the interlayer Pb and graphene's $\pi$ orbitals that may induce proximity effects in graphene. Density functional theory (DFT) calculations for a $(1 \times 1)$ Pb monolayer on SiC show a reasonable qualitative agreement with the experimentally observed interlayer bands as well as the polarization dependent measurements. Finally, temperature dependent ARPES measurements reveal that the nearly charge-neutral graphene layer involves charge transfer from both the interlayer Pb and the substrate SiC.

cond-mat.mes-hall

Contrasting electron-phonon interaction between electron- and hole-doped cuprates

Spin- and charge-lattice interactions are potential key factors in the microscopic mechanism of high-temperature superconductivity in cuprates. Although both interactions can dramatically shape the low-energy electronic structure, their phenomenological roles in superconductivity are usually investigated independently. Employing angle-resolved photoemission spectroscopy, we reveal the spectroscopic fingerprint of short-range antiferromagnetic order in conjunction with enhanced electron-phonon interaction in the electron-doped cuprate superconductor $\mathrm{Nd_{1.85}Ce_{0.15}CuO_4}$. The observed mode coupling exhibits a strong momentum dependence that is in striking contrast to the node-antinode dichotomy previously observed in the hole-doped cuprates. Our results reveal an intimate relationship between electron-phonon coupling and antiferromagnetic fluctuations, which collectively sets the stage for unconventional superconductivity in the electron-doped cuprates.

cond-mat.supr-con

Duality and degeneracy lifting in two-dimensional electron liquids on SrTiO$_3$(001)

Two-dimensional electron liquids (2DELs) have increasing technological relevance for ultrafast electronics and spintronics, yet significant gaps in their fundamental understanding are exemplified on the prototypical SrTiO$_3$. We correlate the exact SrTiO$_3$(001) surface structure with distinct 2DELs through combined microscopic angle-resolved photoemission spectroscopy and non-contact atomic force microscopy on truly bulk-terminated surfaces that alleviate structural uncertainties inherent to this long-studied system. The SrO termination is shown to develop a 2DEL following the creation of oxygen vacancies, unlike the intrinsically metallic TiO$_2$ termination. Differences in degeneracy of the 2DELs, that share the same band filling and identical band bending, are assigned to polar distortions of the Ti atoms in combination with spin order, supported with the extraction of fundamental electron-phonon coupling strength. These results not only resolve the ambiguities regarding 2DELs on SrTiO$_3$ thus far, but also pave the way to manipulating band filling and spin order in oxide 2DELs in general.

cond-mat.mtrl-sci

Topological Weyl Altermagnetism in CrSb

Altermagnets constitute a novel, third fundamental class of collinear magnetic ordered materials, alongside with ferro- and antiferromagnets. They share with conventional antiferromagnets the feature of a vanishing net magnetization. At the same time they show a spin-splitting of electronic bands, just as in ferromagnets, caused by the atomic exchange interaction. On the other hand, topology has recently revolutionized our understanding of condensed matter physics, introducing new phases of matter classified by intrinsic topological order. Here we connect the worlds of altermagnetism and topology, showing that the electronic structure of the altermagnet CrSb is topological and hosts a novel Weyl semimetallic state. Using high-resolution and spin angleresolved photoemission spectroscopy, we observe a large momentum-dependent spin-splitting in CrSb, reaching up to 1 eV, that induces altermagnetic Weyl nodes with an associated magnetic quantum number. At the surface we observe their spin-polarized topological Fermi-arcs. This establishes that in altermagnets the large energy scale intrinsic to the spin-splitting - orders of magnitude larger than the relativistic spin-orbit coupling - creates its own realm of robust electronic topology.

cond-mat.mtrl-sci

Uniaxial strain tuning of charge modulation and singularity in a kagome superconductor

Tunable quantum materials hold great potential for applications. Of special interest are materials in which small lattice strain induces giant electronic responses. The kagome compounds AV3Sb5 (A = K, Rb, Cs) provide a testbed for such singular electronic states. In this study, through angle-resolved photoemission spectroscopy, we provide comprehensive spectroscopic measurements of the giant responses induced by compressive and tensile strains on the charge-density-wave (CDW) order parameter and high-order van Hove singularity (HO-VHS) in CsV3Sb5. We observe a tripling of the CDW gap magnitudes with ~1% strain, accompanied by the changes of both energy and mass of the saddle-point fermions. Our results reveal an anticorrelation between the unconventional CDW order parameter and the mass of a HO-VHS, and highlight the role of the latter in the superconducting pairing. The giant electronic responses uncover a rich strain tunability of the versatile kagome system in studying quantum interplays under lattice perturbations.

cond-mat.mtrl-sci

Non-Hermitian Boundary in a Surface Selective Reconstructed Magnetic Weyl Semimetal

Non-Hermitian physics, studying systems described by non-Hermitian Hamiltonians, reveals unique phenomena not present in Hermitian systems. Unlike Hermitian systems, non-Hermitian systems have complex eigenvalues, making their effects less directly observable. Recently, significant efforts have been devoted to incorporating the non-Hermitian effects into condensed matter physics. However, progress has been hindered by the absence of a viable experimental approach. Here, the discovery of surface-selectively spontaneous reconstructed Weyl semimetal NdAlSi provides a feasible experimental platform for studying non-Hermitian physics. Utilizing angle-resolved photoemission spectroscopy measurements, surface-projected density functional theory calculations, and scanning tunneling microscopy measurements, we demonstrate that surface reconstruction in NdAlSi alters surface Fermi arc connectivity and generates new isolated non-topological surface Fermi arcs. In the presence of a magnetic field, the surface-selective spontaneous reconstructed Weyl semimetal NdAlSi can be viewed as a Hermitian bulk--non-Hermitian boundary system. The isolated non-topological surface Fermi arcs on the reconstructed surface act as a loss mechanism and open boundary condition for the topological electrons and bulk states, serving as non-Hermitian boundary states. This discovery provides a good experimental platform for exploring new physical phenomena and potential applications based on boundary non-Hermitian effects, extending beyond purely mathematical concepts.

cond-mat.mtrl-sci

Disorder Driven Non-Anderson Transition in a Weyl Semimetal

For several decades, it was widely believed that a non-interacting disordered electronic system could only undergo an Anderson metal-insulator transition due to Anderson localization. However, numerous recent theoretical works have predicted the existence of a disorder-driven non-Anderson phase transition that differ from Anderson localization. The frustration lies in the fact that this non-Anderson disorder-driven transition has not yet been experimentally demonstrated in any system. Here, using angle-resolved photoemission spectroscopy, we present a case study of observing the non-Anderson disorder-driven transition by visualizing the electronic structure of the Weyl semimetal NdAlSi on surfaces with varying amounts of disorder. Our observations reveal that strong disorder can effectively suppress all surface states in the Weyl semimetal NdAlSi, including the topological surface Fermi arcs. This disappearance of surface Fermi arcs is associated with the vanishing of the bulk topological invariant, indicating a quantum phase transition from a Weyl semimetal to a diffusive metal. By analyzing the changes in the electronic structure of NdAlSi, as the surface degrades, we provide a physical picture of this non-Anderson transition from a Weyl semimetal to a diffuse metal. These observations provide the first direct experimental evidence of the non-Anderson disorder-driven transition, a discovery long anticipated by theoretical physicists. The finding dispels longstanding suspicions among researchers that non-Anderson transitions exist in real quantum systems.

cond-mat.mtrl-sci