Controlling crystal cleavage in focused ion beam shaped specimens for surface spectroscopy.

Our understanding of quantum materials is commonly based on precise determinations of their electronic spectrum by spectroscopic means, most notably angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy. Both require atomically clean and flat crystal surfaces, which are traditionally prepared by in situ mechanical cleaving in ultrahigh vacuum chambers. We present a new approach that addresses three main issues of the current state-of-the-art methods: (1) Cleaving is a highly stochastic and, thus, inefficient process; (2) fracture processes are governed by the bonds in a bulk crystal, and many materials and surfaces simply do not cleave; and (3) the location of the cleave is random, preventing data collection at specified regions of interest. Our new workflow is based on focused ion beam machining of micro-strain lenses, in which shape (rather than crystalline) anisotropy dictates the plane of cleavage, which can be placed at a specific target layer. As proof-of-principle, we show ARPES results from micro-cleaves of Sr2RuO4 along the ac plane and from two surface orientations of SrTiO3, a notoriously difficult to cleave cubic perovskite.

Fate of Quasiparticles at High Temperature in the Correlated Metal Sr_{2}RuO_{4}.

We study the temperature evolution of quasiparticles in the correlated metal Sr_{2}RuO_{4}. Our angle resolved photoemission data show that quasiparticles persist up to temperatures above 200 K, far beyond the Fermi liquid regime. Extracting the quasiparticle self-energy, we demonstrate that the quasiparticle residue Z increases with increasing temperature. Quasiparticles eventually disappear on approaching the bad metal state of Sr_{2}RuO_{4} not by losing weight but via excessive broadening from super-Planckian scattering. We further show that the Fermi surface of Sr_{2}RuO_{4}-defined as the loci where the spectral function peaks-deflates with increasing temperature. These findings are in semiquantitative agreement with dynamical mean field theory calculations.

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° 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}.

Bulk and Surface Electronic Structure of the Dual-Topology Semimetal Pt_{2}HgSe_{3}.

We report high-resolution angle-resolved photoemission measurements on single crystals of Pt_{2}HgSe_{3} grown by high-pressure synthesis. Our data reveal a gapped Dirac nodal line whose (001) projection separates the surface Brillouin zone in topological and trivial areas. In the nontrivial k-space range, we find surface states with multiple saddle points in the dispersion, resulting in two van Hove singularities in the surface density of states. Based on density-functional theory calculations, we identify these surface states as signatures of a topological crystalline state, which coexists with a weak topological phase.

In situ strain tuning of the metal-insulator-transition of Ca2RuO4 in angle-resolved photoemission experiments.

Pressure plays a key role in the study of quantum materials. Its application in angle resolved photoemission (ARPES) studies, however, has so far been limited. Here, we report the evolution of the k-space electronic structure of bulk Ca2RuO4, lightly doped with Pr, under uniaxial strain. Using ultrathin plate-like crystals, we achieve uniaxial strain levels up to -4.1%, sufficient to suppress the insulating Mott phase and access the previously unexplored electronic structure of the metallic state at low temperature. ARPES experiments performed while tuning the uniaxial strain reveal that metallicity emerges from a marked redistribution of charge within the Ru t2g shell, accompanied by a sudden collapse of the spectral weight in the lower Hubbard band and the emergence of a well-defined Fermi surface which is devoid of pseudogaps. Our results highlight the profound roles of lattice energetics and of the multiorbital nature of Ca2RuO4 in this archetypal Mott transition and open new perspectives for spectroscopic measurements.

Observation of Out-of-Plane Spin Texture in a SrTiO_{3}(111) Two-Dimensional Electron Gas.

We explore the second order bilinear magnetoelectric resistance (BMER) effect in the d-electron-based two-dimensional electron gas (2DEG) at the SrTiO_{3}(111) surface. We find evidence of a spin-split band structure with the archetypal spin-momentum locking of the Rashba effect for the in-plane component. Under an out-of-plane magnetic field, we find a BMER signal that breaks the sixfold symmetry of the electronic dispersion, which is a fingerprint for the presence of a momentum-dependent out-of-plane spin component. Relativistic electronic structure calculations reproduce this spin texture and indicate that the out-of-plane component is a ubiquitous property of oxide 2DEGs arising from strong crystal field effects. We further show that the BMER response of the SrTiO_{3}(111) 2DEG is tunable and unexpectedly large.

Atomically Precise Lateral Modulation of a Two-Dimensional Electron Liquid in Anatase TiO2 Thin Films.

Engineering the electronic band structure of two-dimensional electron liquids (2DELs) confined at the surface or interface of transition metal oxides is key to unlocking their full potential. Here we describe a new approach to tailoring the electronic structure of an oxide surface 2DEL demonstrating the lateral modulation of electronic states with atomic scale precision on an unprecedented length scale comparable to the Fermi wavelength. To this end, we use pulsed laser deposition to grow anatase TiO2 films terminated by a (1 × 4) in-plane surface reconstruction. Employing photostimulated chemical surface doping we induce 2DELs with tunable carrier densities that are confined within a few TiO2 layers below the surface. Subsequent in situ angle-resolved photoemission experiments demonstrate that the (1 × 4) surface reconstruction provides a periodic lateral perturbation of the electron liquid. This causes strong backfolding of the electronic bands, opening of unidirectional gaps and a saddle point singularity in the density of states near the chemical potential.

A facility for the analysis of the electronic structures of solids and their surfaces by synchrotron radiation photoelectron spectroscopy.

A synchrotron radiation beamline in the photon energy range of 18-240 eV and an electron spectroscopy end station have been constructed at the 3 GeV Diamond Light Source storage ring. The instrument features a variable polarisation undulator, a high resolution monochromator, a re-focussing system to form a beam spot of 50 × 50 µm2, and an end station for angle-resolved photoelectron spectroscopy (ARPES) including a 6-degrees-of-freedom cryogenic sample manipulator. The beamline design and its performance allow for a highly productive and precise use of the ARPES technique at an energy resolution of 10-15 meV for fast k-space mapping studies with a photon flux up to 2 ⋅ 1013 ph/s and well below 3 meV for high resolution spectra.

Tailoring the nature and strength of electron-phonon interactions in the SrTiO3(001) 2D electron liquid.

Surfaces and interfaces offer new possibilities for tailoring the many-body interactions that dominate the electrical and thermal properties of transition metal oxides. Here, we use the prototypical two-dimensional electron liquid (2DEL) at the SrTiO3(001) surface to reveal a remarkably complex evolution of electron-phonon coupling with the tunable carrier density of this system. At low density, where superconductivity is found in the analogous 2DEL at the LaAlO3/SrTiO3 interface, our angle-resolved photoemission data show replica bands separated by 100 meV from the main bands. This is a hallmark of a coherent polaronic liquid and implies long-range coupling to a single longitudinal optical phonon branch. In the overdoped regime the preferential coupling to this branch decreases and the 2DEL undergoes a crossover to a more conventional metallic state with weaker short-range electron-phonon interaction. These results place constraints on the theoretical description of superconductivity and allow a unified understanding of the transport properties in SrTiO3-based 2DELs.

Collapse of the Mott Gap and Emergence of a Nodal Liquid in Lightly Doped Sr(2)IrO(4).

We report angle resolved photoemission experiments on the electron doped Heisenberg antiferromagnet (Sr(1-x)La(x))(2)IrO(4). For a doping level of x=0.05, we find an unusual metallic state with coherent nodal excitations and an antinodal pseudogap bearing strong similarities with underdoped cuprates. This state emerges from a rapid collapse of the Mott gap with doping resulting in a large underlying Fermi surface that is backfolded by a (π,π) reciprocal lattice vector which we attribute to the intrinsic structural distortion of Sr(2)IrO(4).

Control of a two-dimensional electron gas on SrTiO3(111) by atomic oxygen.

We report on the formation of a two-dimensional electron gas (2DEG) at the bare surface of (111) oriented SrTiO3. Angle resolved photoemission experiments reveal highly itinerant carriers with a sixfold symmetric Fermi surface and strongly anisotropic effective masses. The electronic structure of the 2DEG is in good agreement with self-consistent tight-binding supercell calculations that incorporate a confinement potential due to surface band bending. We further demonstrate that alternate exposure of the surface to ultraviolet light and atomic oxygen allows tuning of the carrier density and the complete suppression of the 2DEG.

Quasiparticle dynamics and spin-orbital texture of the SrTiO3 two-dimensional electron gas.

Two-dimensional electron gases (2DEGs) in SrTiO3 have become model systems for engineering emergent behaviour in complex transition metal oxides. Understanding the collective interactions that enable this, however, has thus far proved elusive. Here we demonstrate that angle-resolved photoemission can directly image the quasiparticle dynamics of the d-electron subband ladder of this complex-oxide 2DEG. Combined with realistic tight-binding supercell calculations, we uncover how quantum confinement and inversion symmetry breaking collectively tune the delicate interplay of charge, spin, orbital and lattice degrees of freedom in this system. We reveal how they lead to pronounced orbital ordering, mediate an orbitally enhanced Rashba splitting with complex subband-dependent spin-orbital textures and markedly change the character of electron-phonon coupling, co-operatively shaping the low-energy electronic structure of the 2DEG. Our results allow for a unified understanding of spectroscopic and transport measurements across different classes of SrTiO3-based 2DEGs, and yield new microscopic insights on their functional properties.

Electronic structure of a quasi-freestanding MoS2 monolayer.

Several transition-metal dichalcogenides exhibit a striking crossover from indirect to direct band gap semiconductors as they are thinned down to a single monolayer. Here, we demonstrate how an electronic structure characteristic of the isolated monolayer can be created at the surface of a bulk MoS2 crystal. This is achieved by intercalating potassium in the interlayer van der Waals gap, expanding its size while simultaneously doping electrons into the conduction band. Our angle-resolved photoemission measurements reveal resulting electron pockets centered at the K̅ and K' points of the Brillouin zone, providing the first momentum-resolved measurements of how the conduction band dispersions evolve to yield an approximately direct band gap of ∼1.8 eV in quasi-freestanding monolayer MoS2. As well as validating previous theoretical proposals, this establishes a novel methodology for manipulating electronic structure in transition-metal dichalcogenides, opening a new route for the generation of large-area quasi-freestanding monolayers for future fundamental study and use in practical applications.

Coherent quasiparticles with a small fermi surface in lightly doped Sr(3)Ir(2)O(7).

We characterize the electron doping evolution of (Sr_{1-x}La_{x})_{3}Ir_{2}O_{7} by means of angle-resolved photoemission. Concomitant with the metal insulator transition around x≈0.05 we find the emergence of coherent quasiparticle states forming a closed small Fermi surface of volume 3x/2, where x is the independently measured La concentration. The quasiparticle weight Z remains large along the entire Fermi surface, consistent with the moderate renormalization of the low-energy dispersion, and no pseudogap is observed. This indicates a conventional, weakly correlated Fermi liquid state with a momentum independent residue Z≈0.5 in lightly doped Sr_{3}Ir_{2}O_{7}.

Emergent quantum confinement at topological insulator surfaces.

Bismuth-chalchogenides are model examples of three-dimensional topological insulators. Their ideal bulk-truncated surface hosts a single spin-helical surface state, which is the simplest possible surface electronic structure allowed by their non-trivial Z(2) topology. However, real surfaces of such compounds, even if kept in ultra-high vacuum, rapidly develop a much more complex electronic structure whose origin and properties have proved controversial. Here we demonstrate that a conceptually simple model, implementing a semiconductor-like band bending in a parameter-free tight-binding supercell calculation, can quantitatively explain the entire measured hierarchy of electronic states. In combination with circular dichroism in angle-resolved photoemission experiments, we further uncover a rich three-dimensional spin texture of this surface electronic system, resulting from the non-trivial topology of the bulk band structure. Moreover, our study sheds new light on the surface-bulk connectivity in topological insulators, and reveals how this is modified by quantum confinement.

Subband structure of a two-dimensional electron gas formed at the polar surface of the strong spin-orbit perovskite KTaO3.

We demonstrate the formation of a two-dimensional electron gas (2DEG) at the (100) surface of the 5d transition-metal oxide KTaO3. From angle-resolved photoemission, we find that quantum confinement lifts the orbital degeneracy of the bulk band structure and leads to a 2DEG composed of ladders of subband states of both light and heavy carriers. Despite the strong spin-orbit coupling, our measurements provide a direct upper bound for the potential Rashba spin splitting of only Δk(parallel)}~0.02 Å(-1) at the Fermi level. The polar nature of the KTaO3(100) surface appears to help mediate the formation of the 2DEG as compared to nonpolar SrTiO3(100).

Controlling bulk conductivity in topological insulators: key role of anti-site defects.

Intrinsic topological insulators are realized by alloying Bi(2)Te(3) with Bi(2)Se(3). Angle-resolved photoemission and bulk transport measurements reveal that the Fermi level is readily tuned into the bulk bandgap. First-principles calculations of the native defect landscape highlight the key role of anti-site defects for achieving this, and predict optimal growth conditions to realize maximally resistive topological insulators.

Large tunable Rashba spin splitting of a two-dimensional electron gas in Bi2Se3.

We report a Rashba spin splitting of a two-dimensional electron gas in the topological insulator Bi(2)Se(3) from angle-resolved photoemission spectroscopy. We further demonstrate its electrostatic control, and show that spin splittings can be achieved which are at least an order-of-magnitude larger than in other semiconductors. Together these results show promise for the miniaturization of spintronic devices to the nanoscale and their operation at room temperature.

Structural origin of apparent Fermi surface pockets in angle-resolved photoemission of Bi2Sr(2-x)La(x)CuO(6+δ).

We observe apparent hole pockets in the Fermi surfaces of single-layer Bi-based cuprate superconductors from angle-resolved photoemission. From detailed low-energy electron diffraction measurements and an analysis of the angle-resolved photoemission polarization dependence, we show that these pockets are not intrinsic but arise from multiple overlapping superstructure replicas of the main and shadow bands. We further demonstrate that the hole pockets reported recently from angle-resolved photoemission [Meng et al., Nature (London) 462, 335 (2009)] have a similar structural origin and are inconsistent with an intrinsic hole pocket associated with the electronic structure of a doped CuO2 plane.

Creation and control of a two-dimensional electron liquid at the bare SrTiO3 surface.

Many-body interactions in transition-metal oxides give rise to a wide range of functional properties, such as high-temperature superconductivity, colossal magnetoresistance or multiferroicity . The seminal recent discovery of a two-dimensional electron gas (2DEG) at the interface of the insulating oxides LaAlO(3) and SrTiO(3) (ref. 4) represents an important milestone towards exploiting such properties in all-oxide devices. This conducting interface shows a number of appealing properties, including a high electron mobility, superconductivity and large magnetoresistance, and can be patterned on the few-nanometre length scale. However, the microscopic origin of the interface 2DEG is poorly understood. Here, we show that a similar 2DEG, with an electron density as large as 8×10(13) cm(-2), can be formed at the bare SrTiO(3) surface. Furthermore, we find that the 2DEG density can be controlled through exposure of the surface to intense ultraviolet light. Subsequent angle-resolved photoemission spectroscopy measurements reveal an unusual coexistence of a light quasiparticle mass and signatures of strong many-body interactions.