Search

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., Comment: 10 pages including supplementary information

The Mott insulator Ca$_2$RuO$_4$ exhibits a rare insulator-to-metal transition (IMT) induced by DC current. While structural changes associated with this transition have been tracked by neutron diffraction, Raman scattering, and x-ray spectroscopy, work on elucidating the response of the electronic degrees of freedom is still in progress. Here we unveil the current-induced modifications of the electronic states of Ca$_2$RuO$_4$ by employing angle-resolved photoemission spectroscopy (ARPES) in conjunction with four-probe transport. Two main effects emerge: a clear reduction of the Mott gap and a modification in the dispersion of the Ru-bands. The changes in dispersion occur exclusively along the $XM$ high-symmetry direction, parallel to the $b$-axis where the greatest in-plane lattice change occurs. These experimental observations, together with dynamical mean-field theory (DMFT) calculations simulated from the current-induced structural distortions, indicate the intimate interplay of lattice and orbital-dependent electronic response in the current-driven IMT. Furthermore, based on a free energy analysis, we demonstrate that the current-induced phase, albeit thermodynamically equivalent, is electronically distinct from the high-temperature zero-current metallic phase. Our results provide insight into the elusive nature of the current-induced IMT of Ca$_2$RuO$_4$ and advance the challenging, yet powerful, technique of transport-ARPES., Comment: 10 pages, 5 figures

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.

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.

We apply an intense infrared laser pulse in order to perturb the electronic and vibrational states in the three-dimensional charge density wave material 1$T$-VSe$_2$. Ultrafast snapshots of the light-induced hot carrier dynamics and non-equilibrium quasiparticle spectral function are collected using time- and angle-resolved photoemission spectroscopy. The hot carrier temperature and time-dependent electronic self-energy are extracted from the time-dependent spectral function, revealing that incoherent electron-phonon interactions heat the lattice above the charge density wave critical temperature on a timescale of $(200 \pm 40)$~fs. Density functional perturbation theory calculations establish that the presence of hot carriers alters the overall phonon dispersion and quenches efficient low-energy acoustic phonon scattering channels, which results in a new quasi-equilibrium state that is experimentally observed., Comment: 24 pages including supplemental material, 4 figures in the main text and 4 figures in the supplemental material

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., Comment: 8 pages, 5 figures

Assembling transition metal dichalcogenides (TMDCs) at the two-dimensional (2D) limit is a promising approach for tailoring emerging states of matter such as superconductivity or charge density waves (CDWs). Single-layer (SL) VSe$_2$ stands out in this regard because it exhibits a strongly enhanced CDW transition with a higher transition temperature compared to the bulk in addition to an insulating phase with an anisotropic gap at the Fermi level, causing a suppression of anticipated 2D ferromagnetism in the material. Here, we investigate the interplay of electronic and lattice degrees of freedom that underpin these electronic phases in SL VSe$_2$ using ultrafast pump-probe photoemission spectroscopy. In the insulating state, we observe a light-induced closure of the energy gap on a timescale of 480 fs, which we disentangle from the ensuing hot carrier dynamics. Our work thereby reveals that the phase transition in SL VSe$_2$ is driven by electron-lattice coupling and demonstrates the potential for controlling electronic phases in 2D materials with light., Comment: 23 pages including supplementary information, 3 figures in the main text and 6 figures in the supplemental text

We investigate the temperature-dependent electronic structure of the van der Waals ferromagnet, CrGeTe$_3$. Using angle-resolved photoemission spectroscopy, we identify atomic- and orbital-specific band shifts upon cooling through ${T_\mathrm{C}}$. From these, together with x-ray absorption spectroscopy and x-ray magnetic circular dichroism measurements, we identify the states created by a covalent bond between the Te ${5p}$ and the Cr ${e_g}$ orbitals as the primary driver of the ferromagnetic ordering in this system, while it is the Cr ${t_{2g}}$ states that carry the majority of the spin moment. The ${t_{2g}}$ states furthermore exhibit a marked bandwidth increase and a remarkable lifetime enhancement upon entering the ordered phase, pointing to a delicate interplay between localized and itinerant states in this family of layered ferromagnets.

We present a combined study from angle-resolved photoemission and density-functional theory calculations of the temperature-dependent electronic structure in the excitonic insulator candidate Ta$_2$NiSe$_5$. Our experimental measurements unambiguously establish the normal state as a semimetal with a significant band overlap of $>$100~meV. Our temperature-dependent measurements indicate how these low-energy states hybridise when cooling through the well-known 327~K phase transition in this system. From our calculations and polarisation-dependent photoemission measurements, we demonstrate the importance of a loss of mirror symmetry in enabling the band hybridisation, driven by a shear-like structural distortion which reduces the crystal symmetry from orthorhombic to monoclinic. Our results thus point to the key role of the lattice distortion in enabling the phase transition of Ta$_2$NiSe$_5$., Comment: 6 pages, 4 figures

Inversion-symmetric crystals are optically isotropic and thus naively not expected to show dichroism effects in optical absorption and photoemission processes. Here, we find a strong linear dichroism effect (up to 42.4%) in the conduction band of inversion-symmetric bilayer MoS$_2$, when measuring energy- and momentum-resolved snapshots of excited electrons by time- and angle-resolved photoemission spectroscopy. We model the polarization-dependent photoemission intensity in the transiently-populated conduction band using the semiconductor Bloch equations and show that the observed dichroism emerges from intralayer single-particle effects within the isotropic part of the dispersion. This leads to optical excitations with an anisotropic momentum-dependence in an otherwise inversion symmetric material., Comment: 10 pages including supporting information, 3 figures in the main paper and 4 figures in the supporting information

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$_2$.

We present the observation of glass-like dynamic correlations of mobile mercury ions in the ionic conductor Cu2HgI4, detected in both NMR and nonlinear conductivity experiments. The results show that dynamic cooperativity appears in systems seemingly unrelated to glassy and soft arrested materials. A simple kinetic two-component model is proposed, which seems to provide a good description of the cooperative ionic dynamics., Comment: 5+2 pages (including supplemental material) This is final, accepted version