arXiv subjects

Matthew D. Watson

Publications and source records attributed to Matthew D. Watson.

At least 37 records · Page 2Linked to original sources

arXiv2024

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↗

arXiv2024

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↗

arXiv2024

Avoided metallicity in a hole-doped Mott insulator on a triangular lattice

Doping of a Mott insulator gives rise to a wide variety of exotic emergent states, from high-temperature superconductivity to charge, spin, and orbital orders. The physics underpinning their evolution is, however, poorly understood. A major challenge is the chemical complexity associated with traditional routes to doping. Here, we study the Mott insulating CrO$_2$ layer of the delafossite PdCrO$_2$, where an intrinsic polar catastrophe provides a clean route to doping of the surface. From scanning tunnelling microscopy and angle-resolved photoemission, we find that the surface stays insulating accompanied by a short-range ordered state. From density functional theory, we demonstrate how the formation of charge disproportionation results in an insulating ground state of the surface that is disparate from the hidden Mott insulator in the bulk. We demonstrate that voltage pulses induce local modifications to this state which relax over tens of minutes, pointing to a glassy nature of the charge order.

cond-mat.str-el↗

arXiv2024

Giant exchange splitting in the electronic structure of A-type 2D antiferromagnet CrSBr

We present the evolution of the electronic structure of CrSBr from its antiferromagnetic ground state to the paramagnetic phase above T_N=132 K, in both experiment and theory. Low temperature angle-resolved photoemission spectroscopy (ARPES) results are obtained using a novel method to overcome sample charging issues, revealing quasi-2D valence bands in the ground state. The results are very well reproduced by our QSGŴ calculations, which further identify certain bands at the X points to be exchange-split pairs of states with mainly Br and S character. By tracing band positions as a function of temperature, we show the splitting disappears above T_N. The energy splitting is interpreted as an effective exchange splitting in individual layers in which the Cr moments all align, within the so-called A-type antiferromagnetic arrangement. Our results lay firm foundations for the interpretation of the many other intriguing physical and optical properties of CrSBr.

cond-mat.str-el↗

arXiv2024

Holstein polarons, Rashba-like spin splitting and Ising superconductivity in electron-doped MoSe2

Interaction between electrons and phonons in solids is a key effect defining physical properties of materials such as electrical and thermal conductivity. In transitional metal dichalcogenides (TMDCs) the electron-phonon coupling results in the creation of polarons, quasiparticles that manifest themselves as discrete features in the electronic spectral function. In this study, we report the formation of polarons at the alkali dosed MoSe2 surface, where Rashba-like spin splitting of the conduction band states is caused by an inversion-symmetry breaking electric field. In addition, we observe the crossover from phonon-like to plasmon-like polaronic spectral features at MoSe2 surface with increasing doping. Our findings support the concept of electron-phonon coupling mediated superconductivity in electron-doped layered TMDC materials, observed using ionic liquid gating technology. Furthermore, the discovered spin-splitting at the Fermi level could offer crucial experimental validation for theoretical models of Ising-type superconductivity in these materials.

cond-mat.supr-con↗

arXiv2024

Fermi Surface Nesting Driving the RKKY Interaction in the Centrosymmetric Skyrmion Magnet Gd2PdSi3

The magnetic skyrmions generated in a centrosymmetric crystal were recently first discovered in Gd2PdSi3. In light of this, we observe the electronic structure by angle-resolved photoemission spectroscopy (ARPES) and unveil its direct relationship with the magnetism in this compound. The Fermi surface and band dispersions are demonstrated to have a good agreement with the density functional theory (DFT) calculations carried out with careful consideration of the crystal superstructure. Most importantly, we find that the three-dimensional Fermi surface has extended nesting which matches well the q-vector of the magnetic order detected by recent scattering measurements. The consistency we find among ARPES, DFT, and the scattering measurements suggests the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction involving itinerant electrons to be the formation mechanism of skyrmions in Gd2PdSi3.

cond-mat.mtrl-sci↗

arXiv2024

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↗

arXiv2024

Lattice fluctuations, not excitonic correlations, mediated electronic localization in TiSe$_2$

TiSe$_2$ is thought to be an insulator with a bandgap of ~0.1eV. It has attracted a much interest because, among of a rich array of unique properties, many have thought TiSe$_2$ is a rare realisation of an excitonic insulator. Below 200 K, TiSe$_2$ undergoes a transition from a high-symmetry ({P-3m1}) phase to a low-symmetry ({P-3c1}) phase. Here we establish that TiSe$_2$ is indeed an insulator in both {P-3m1} and {P-3c1} phases. However, the insulating state is driven not by excitonic effects but by symmetry-breaking of the {P-3m1} phase. In the CDW phase the symmetry breaking is static. At high temperature, thermally driven instantaneous deviations from {P-3m1} break the symmetry on the characteristic time scale of a phonon. Even while the time-averaged \emph{lattice} structure assumes {P-3m1} symmetry, the time-averaged \emph{energy band} structure is closer to the CDW phase -- a rare instance of a metal-insulator transition induced by dynamical symmetry breaking. We establish these conclusions from a high-fidelity, self-consistent form of many body perturbation theory, in combination with molecular dynamics simulations to capture the effects of thermal disorder. The many-body theory includes explicitly ladder diagrams in the polarizability, which incorporates excitonic effects in an \emph{ab initio} manner. The excitonic modification to the potential is slight, ruling out the possibility that TiSe$_2$ is an excitonic insulator. Charge self-consistency is essential distinguish the metallic from insulating state.

cond-mat.mtrl-sci↗

arXiv2024

Resurgence of superconductivity and the role of $d_{xy}$ hole band in FeSe$_{1-x}$Te$_x$

Iron-chalcogenide superconductors display rich phenomena caused by orbital-dependent band shifts and electronic correlations. Additionally, they are potential candidates for topological superconductivity due to the band inversion between the Fe $d$ bands and the chalcogen $p_z$ band. Here we present a detailed study of the electronic structure of the nematic superconductors FeSe$_{1-x}$Te$_x$ ($0<x<0.4$) using angle-resolved photoemission spectroscopy to understand the role of orbital-dependent band shifts, electronic correlations and the chalcogen band. We assess the changes in the effective masses using a three-band low energy model, and the band renormalization via comparison with DFT band structure calculations. The effective masses decrease for all three-hole bands inside the nematic phase followed by a strong increase for the band with $d_{xy}$ orbital character. Interestingly, this nearly-flat $d_{xy}$ band becomes more correlated as it shifts towards the Fermi level with increasing Te concentrations and as the second superconducting dome emerges. Our findings suggests that the $d_{xy}$ hole band, which is very sensitive to the chalcogen height, could be involved in promoting an additional pairing channel and increasing the density of states to stabilize the second superconducting dome in FeSe$_{1-x}$Te$_x$. This simultaneous shift of the $d_{xy}$ hole band and enhanced superconductivity is in contrast with FeSe$_{1-x}$S$_x$.

cond-mat.supr-con↗

arXiv2023

The pseudochiral Fermi surface of $α$-RuI$_3$

In continuation of research into RuCl$_3$ and RuBr$_3$ as potential quantum spin liquids, a phase with unique magnetic order characterised by long-range quantum entanglement and fractionalised excitations, the compound RuI$_3$ has been recently synthesised. Here, we show RuI$_3$ is a moderately correlated metal with two bands crossing the Fermi level, implying the absence of any quantum spin liquids phase. We find that the Fermi surface as measured or calculated for a 2D ($k_\text{x},k_\text{y}$) slice at any $k_\text{z}$ lacks mirror symmetry, i.e. is pseudochiral. We link this phenomenon to the ABC stacking in the R$\bar{3}$ space group of $α$-RuI$_3$, which is achiral but lacks any mirror or glide symmetries. We further provide a formal framework for understanding when such a pseudochiral electronic structure may be observed.

cond-mat.str-el↗

arXiv2023

Charge doping into spin minority states mediates doubling of $T_\mathrm{C}$ in ferromagnetic CrGeTe$_3$

The recent discovery of the persistence of long-range magnetic order when van der Waals layered magnets are thinned towards the monolayer limit has provided a tunable platform for the engineering of novel magnetic structures and devices. Here, we study the evolution of the electronic structure of CrGeTe$_3$ as a function of electron doping in the surface layer. From angle-resolved photoemission spectroscopy, we observe spectroscopic fingerprints that this electron doping drives a marked increase in $T_\mathrm{C}$, reaching values more than double that of the undoped material, in agreement with recent studies using electrostatic gating. Together with density functional theory calculations and Monte Carlo simulations, we show that, surprisingly, the increased $T_\mathrm{C}$ is mediated by the population of spin-minority Cr $t_{2g}$ states, forming a half-metallic 2D electron gas at the surface. We show how this promotes a novel variant of double exchange, and unlocks a significant influence of the Ge -- which was previously thought to be electronically inert in this system -- in mediating Cr-Cr exchange.

cond-mat.mtrl-sci↗

arXiv2023

Observation of termination-dependent topological connectivity in a magnetic Weyl kagome-lattice

Engineering surfaces and interfaces of materials promises great potential in the field of heterostructures and quantum matter designer, with the opportunity of driving new many-body phases that are absent in the bulk compounds. Here, we focus on the magnetic Weyl kagome system Co$_3$Sn$_2$S$_2$ and show how for different sample's terminations the Weyl-points connect also differently, still preserving the bulk-boundary correspondence. Scanning-tunnelling microscopy has suggested such a scenario indirectly. Here, we demonstrate this directly for the fermiology of Co$_3$Sn$_2$S$_2$, by linking it to the system real space surfaces distribution. By a combination of micro-ARPES and first-principles calculations, we measure the energy-momentum spectra and the Fermi surfaces of Co$_3$Sn$_2$S$_2$ for different surface terminations and show the existence of topological features directly depending on the top-layer electronic environment. Our work helps to define a route to control bulk-derived topological properties by means of surface electrostatic potentials, creating a realistic and reliable methodology to use Weyl kagome metals in responsive magnetic spintronics.

cond-mat.str-el↗

arXiv2023

Unveiling phase diagram of the lightly doped high-Tc cuprate superconductors with disorder removed

The currently established electronic phase diagram of cuprates is based on a study of single- and double-layered compounds. These CuO$_2$ planes, however, are directly contacted with dopant layers, thus inevitably disordered with an inhomogeneous electronic state. Here, we solve this issue by investigating a 6-layered Ba$_2$Ca$_5$Cu$_6$O$_{12}$(F,O)$_2$ with inner CuO$_2$ layers, which are clean with the extremely low disorder, by angle-resolved photoemission spectroscopy (ARPES) and quantum oscillation measurements. We find a tiny Fermi pocket with a doping level less than 1% to exhibit well-defined quasiparticle peaks which surprisingly lack the polaronic feature. This provides the first evidence that the slightest amount of carriers is enough to turn a Mott insulating state into a metallic state with long-lived quasiparticles. By tuning hole carriers, we also find an unexpected phase transition from the superconducting to metallic states at 4%. Our results are distinct from the nodal liquid state with polaronic features proposed as an anomaly of the heavily underdoped cuprates.

cond-mat.supr-con↗

arXiv2023

Spectral signatures of a unique charge density wave in Ta$_2$NiSe$_7$

Charge Density Waves (CDW) are commonly associated with the presence of near-Fermi level states which are separated from others, or "nested", by a wavector of $\mathbf{q}$. Here we use Angle-Resolved Photo Emission Spectroscopy (ARPES) on the CDW material Ta$_2$NiSe$_7$ and identify a total absence of any plausible nesting of states at the primary CDW wavevector $\mathbf{q}$. Nevertheless we observe spectral intensity on replicas of the hole-like valence bands, shifted by a wavevector of $\mathbf{q}$, which appears with the CDW transition. In contrast, we find that there is a possible nesting at $\mathbf{2q}$, and associate the characters of these bands with the reported atomic modulations at $\mathbf{2q}$. Our comprehensive electronic structure perspective shows that the CDW-like transition of Ta$_2$NiSe$_7$ is unique, with the primary wavevector $\mathbf{q}$ being unrelated to any low-energy states, but suggests that the reported modulation at $\mathbf{2q}$, which would plausibly connect low-energy states, might be more important for the overall energetics of the problem.

cond-mat.str-el↗

arXiv2023

Hierarchy of Lifshitz transitions in the surface electronic structure of Sr$_2$RuO$_4$ under uniaxial compression

We report the evolution of the electronic structure at the surface of the layered perovskite Sr$_2$RuO$_4$ under large in-plane uniaxial compression, leading to anisotropic $B_{1g}$ strains of ${\varepsilon_{xx}-\varepsilon_{yy}=-0.9\pm0.1\%}$. From angle-resolved photoemission, we show how this drives a sequence of Lifshitz transitions, reshaping the low-energy electronic structure and the rich spectrum of van Hove singularities that the surface layer of Sr$_2$RuO$_4$ hosts. From comparison to tight-binding modelling, we find that the strain is accommodated predominantly by bond-length changes rather than modifications of octahedral tilt and rotation angles. Our study sheds new light on the nature of structural distortions at oxide surfaces, and how targeted control of these can be used to tune density of states singularities to the Fermi level, in turn paving the way to the possible realisation of rich collective states at the Sr$_2$RuO$_4$ surface.

cond-mat.str-el↗

arXiv2022

Observation of flat $Γ$ moiré bands in twisted bilayer WSe$_2$

The recent observation of correlated phases in transition metal dichalcogenide moiré systems at integer and fractional filling promises new insight into metal-insulator transitions and the unusual states of matter that can emerge near such transitions. Here, we combine real- and momentum-space mapping techniques to study moiré superlattice effects in 57.4$^{\circ}$ twisted WSe$_2$ (tWSe$_2$). Our data reveal a split-off flat band that derives from the monolayer $Γ$ states. Using advanced data analysis, we directly quantify the moiré potential from our data. We further demonstrate that the global valence band maximum in tWSe$_2$ is close in energy to this flat band but derives from the monolayer K-states which show weaker superlattice effects. These results constrain theoretical models and open the perspective that $Γ$-valley flat bands might be involved in the correlated physics of twisted WSe$_2$.

cond-mat.str-el↗

arXiv2022

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↗

arXiv2022

Strong surface termination dependence of the electronic structure of polar superconductor LaFeAsO revealed by nano-ARPES

The electronic structures of the iron-based superconductors have been intensively studied by using angleresolved photoemission spectroscopy (ARPES). A considerable amount of research has been focused on the LaFeAsO family, showing the highest transition temperatures, where previous ARPES studies have found much larger Fermi surfaces than bulk theoretical calculations would predict. The discrepancy has been attributed to the presence of termination-dependent surface states. Here, using photoemission spectroscopy with a sub-micron focused beam spot (nano-ARPES) we have successfully measured the electronic structures of both the LaO and FeAs terminations in LaFeAsO. Our data reveal very different band dispersions and core-level spectra for different surface terminations, showing that previous macro-focus ARPES measurements were incomplete. Our results give direct evidence for the surface-driven electronic structure reconstruction in LaFeAsO, including formation of the termination-dependent surface states at the Fermi level. This new experimental technique, which we have shown to be very powerful when applied to this prototypical compound, can now be used to study various materials with different surface terminations.

cond-mat.supr-con↗