Resistive switching in diamondoid thin films.

The electrical transport properties of a thin film of the diamondoid adamantane, deposited on an Au/W substrate, were investigated experimentally. The current I, in applied potential V, from the admantane-thiol/metal heterstructure to a wire lead on its surface exhibited non-symmetric (diode-like) characteristics and a signature of resistive switching (RS), an effect that is valuable to non-volatile memory applications. I(V) follows a hysteresis curve that passes twice through [Formula: see text] linearly, indicating RS between two states with significantly different conductances, possibly due to an exotic mechanism.

Spectral weight reduction of two-dimensional electron gases at oxide surfaces across the ferroelectric transition.

The discovery of a two-dimensional electron gas (2DEG) at the [Formula: see text] interface has set a new platform for all-oxide electronics which could potentially exhibit the interplay among charge, spin, orbital, superconductivity, ferromagnetism and ferroelectricity. In this work, by using angle-resolved photoemission spectroscopy and conductivity measurement, we found the reduction of 2DEGs and the changes of the conductivity nature of some ferroelectric oxides including insulating Nb-lightly-substituted [Formula: see text], [Formula: see text] (BTO) and (Ca,Zr)-doped BTO across paraelectric-ferroelectric transition. We propose that these behaviours could be due to the increase of space-charge screening potential at the 2DEG/ferroelectric regions which is a result of the realignment of ferroelectric polarisation upon light irradiation. This finding suggests an opportunity for controlling the 2DEG at a bare oxide surface (instead of interfacial system) by using both light and ferroelectricity.

Interplay of negative electronic compressibility and capacitance enhancement in lightly-doped metal oxide Bi0.95La0.05FeO3 by quantum capacitance model.

Light-sensitive capacitance variation of Bi0.95La0.05FeO3 (BLFO) ceramics has been studied under violet to UV irradiation. The reversible capacitance enhancement up to 21% under 405 nm violet laser irradiation has been observed, suggesting a possible degree of freedom to dynamically control this in high dielectric materials for light-sensitive capacitance applications. By using ultraviolet photoemission spectroscopy (UPS), we show here that exposure of BLFO surfaces to UV light induces a counterintuitive shift of the O2p valence state to lower binding energy of up to 243 meV which is a direct signature of negative electronic compressibility (NEC). A decrease of BLFO electrical resistance agrees strongly with the UPS data suggesting the creation of a thin conductive layer on its insulating bulk under light irradiation. By exploiting the quantum capacitance model, we find that the negative quantum capacitance due to this NEC effect plays an important role in this capacitance enhancement.

Fermiology and Superconductivity of Topological Surface States in PdTe_{2}.

We study the low-energy surface electronic structure of the transition-metal dichalcogenide superconductor PdTe_{2} by spin- and angle-resolved photoemission, scanning tunneling microscopy, and density-functional theory-based supercell calculations. Comparing PdTe_{2} with its sister compound PtSe_{2}, we demonstrate how enhanced interlayer hopping in the Te-based material drives a band inversion within the antibonding p-orbital manifold well above the Fermi level. We show how this mediates spin-polarized topological surface states which form rich multivalley Fermi surfaces with complex spin textures. Scanning tunneling spectroscopy reveals type-II superconductivity at the surface, and moreover shows no evidence for an unconventional component of its superconducting order parameter, despite the presence of topological surface states.

Ubiquitous formation of bulk Dirac cones and topological surface states from a single orbital manifold in transition-metal dichalcogenides.

Transition-metal dichalcogenides (TMDs) are renowned for their rich and varied bulk properties, while their single-layer variants have become one of the most prominent examples of two-dimensional materials beyond graphene. Their disparate ground states largely depend on transition metal d-electron-derived electronic states, on which the vast majority of attention has been concentrated to date. Here, we focus on the chalcogen-derived states. From density-functional theory calculations together with spin- and angle-resolved photoemission, we find that these generically host a co-existence of type-I and type-II three-dimensional bulk Dirac fermions as well as ladders of topological surface states and surface resonances. We demonstrate how these naturally arise within a single p-orbital manifold as a general consequence of a trigonal crystal field, and as such can be expected across a large number of compounds. Already, we demonstrate their existence in six separate TMDs, opening routes to tune, and ultimately exploit, their topological physics.

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.

Negative electronic compressibility and tunable spin splitting in WSe2.

Tunable bandgaps, extraordinarily large exciton-binding energies, strong light-matter coupling and a locking of the electron spin with layer and valley pseudospins have established transition-metal dichalcogenides (TMDs) as a unique class of two-dimensional (2D) semiconductors with wide-ranging practical applications. Using angle-resolved photoemission (ARPES), we show here that doping electrons at the surface of the prototypical strong spin-orbit TMD WSe2, akin to applying a gate voltage in a transistor-type device, induces a counterintuitive lowering of the surface chemical potential concomitant with the formation of a multivalley 2D electron gas (2DEG). These measurements provide a direct spectroscopic signature of negative electronic compressibility (NEC), a result of electron-electron interactions, which we find persists to carrier densities approximately three orders of magnitude higher than in typical semiconductor 2DEGs that exhibit this effect. An accompanying tunable spin splitting of the valence bands further reveals a complex interplay between single-particle band-structure evolution and many-body interactions in electrostatically doped TMDs. Understanding and exploiting this will open up new opportunities for advanced electronic and quantum-logic devices.

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.

Phase competition in trisected superconducting dome.

A detailed phenomenology of low energy excitations is a crucial starting point for microscopic understanding of complex materials, such as the cuprate high-temperature superconductors. Because of its unique momentum-space discrimination, angle-resolved photoemission spectroscopy (ARPES) is ideally suited for this task in the cuprates, where emergent phases, particularly superconductivity and the pseudogap, have anisotropic gap structure in momentum space. We present a comprehensive doping- and temperature-dependence ARPES study of spectral gaps in Bi(2)Sr(2)CaCu(2)O(8+δ), covering much of the superconducting portion of the phase diagram. In the ground state, abrupt changes in near-nodal gap phenomenology give spectroscopic evidence for two potential quantum critical points, p = 0.19 for the pseudogap phase and p = 0.076 for another competing phase. Temperature dependence reveals that the pseudogap is not static below T(c) and exists p > 0.19 at higher temperatures. Our data imply a revised phase diagram that reconciles conflicting reports about the endpoint of the pseudogap in the literature, incorporates phase competition between the superconducting gap and pseudogap, and highlights distinct physics at the edge of the superconducting dome.

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).

Reaffirming the d(x2-y2) superconducting gap using the autocorrelation angle-resolved photoemission spectroscopy of Bi1.5Pb0.55Sr1.6La0.4CuO(6+δ).

Knowledge of the gap function is important to understand the pairing mechanism for high-temperature (T(c)) superconductivity. However, Fourier transform scanning tunneling spectroscopy (FT STS) and angle-resolved photoemission spectroscopy (ARPES) in the cuprates have reported contradictory gap functions, with FT-STS results deviating strongly from a canonical d(x2-y2) form. By applying an "octet model" analysis to autocorrelation ARPES, we reveal that a contradiction occurs because the octet model does not consider the effects of matrix elements and the pseudogap. This reaffirms the canonical d(x2-y2) superconducting gap around the node, which can be directly determined from ARPES. Further, our study suggests that the FT-STS reported fluctuating superconductivity around the node at far above T(c) is not necessary to explain the existence of the quasiparticle interference at low energy.

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.

From a single-band metal to a high-temperature superconductor via two thermal phase transitions.

The nature of the pseudogap phase of cuprate high-temperature superconductors is a major unsolved problem in condensed matter physics. We studied the commencement of the pseudogap state at temperature T* using three different techniques (angle-resolved photoemission spectroscopy, polar Kerr effect, and time-resolved reflectivity) on the same optimally doped Bi2201 crystals. We observed the coincident, abrupt onset at T* of a particle-hole asymmetric antinodal gap in the electronic spectrum, a Kerr rotation in the reflected light polarization, and a change in the ultrafast relaxational dynamics, consistent with a phase transition. Upon further cooling, spectroscopic signatures of superconductivity begin to grow close to the superconducting transition temperature (T(c)), entangled in an energy-momentum-dependent manner with the preexisting pseudogap features, ushering in a ground state with coexisting orders.

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.

Strong electron correlations in the normal state of the iron-based FeSe0.42Te0.58 superconductor observed by angle-resolved photoemission spectroscopy.

We investigate the normal state of the "11" iron-based superconductor FeSe0.42Te0.58 by angle-resolved photoemission. Our data reveal a highly renormalized quasiparticle dispersion characteristic of a strongly correlated metal. We find sheet dependent effective carrier masses between approximately 3 and 16m{e} corresponding to a mass enhancement over band structure values of m{*}/m{band} approximately 6-20. This is nearly an order of magnitude higher than the renormalization reported previously for iron-arsenide superconductors of the "1111" and "122" families but fully consistent with the bulk specific heat.

Fermi surface and van Hove singularities in the itinerant Metamagnet Sr3Ru2O7.

The low-energy electronic structure of the itinerant metamagnet Sr3Ru2O7 is investigated by angle-resolved photoemission and density-functional calculations. We find well-defined quasiparticle bands with resolution-limited linewidths and Fermi velocities up to an order of magnitude lower than in single layer Sr2RuO4. The complete topography, the cyclotron masses, and the orbital character of the Fermi surface are determined, in agreement with bulk sensitive de Haas-van Alphen measurements. An analysis of the dxy band dispersion reveals a complex density of states with van Hove singularities near the Fermi level, a situation which is favorable for magnetic instabilities.

Evolution of the Fermi surface and quasiparticle renormalization through a van Hove singularity in Sr2-yLayRuO4.

We employ a combination of chemical substitution and angle resolved photoemission spectroscopy to prove that the Fermi level in the gamma band of Sr(2-y)La(y)RuO(4) can be made to traverse a van Hove singularity. Remarkably, the large mass renormalization has little dependence on either k or doping. By combining the results from photoemission with thermodynamic measurements on the same batches of crystals, we deduce a parametrization of the full many-body quasiparticle dispersion in Sr(2)RuO(4) which extends from the Fermi level to approximately 20 meV above it.

Monochromatic electron photoemission from diamondoid monolayers.

We found monochromatic electron photoemission from large-area self-assembled monolayers of a functionalized diamondoid, [121]tetramantane-6-thiol. Photoelectron spectra of the diamondoid monolayers exhibited a peak at the low-kinetic energy threshold; up to 68% of all emitted electrons were emitted within this single energy peak. The intensity of the emission peak is indicative of diamondoids being negative electron affinity materials. With an energy distribution width of less than 0.5 electron volts, this source of monochromatic electrons may find application in technologies such as electron microscopy, electron beam lithography, and field-emission flat-panel displays.

Fermi surface and quasiparticle excitations of Sr2RhO4.

The electronic structure of the layered 4d transition metal oxide Sr2RhO4 is investigated by angle resolved photoemission. We find well-defined quasiparticle excitations with a highly anisotropic dispersion, suggesting a quasi-two-dimensional Fermi-liquid-like ground state. Markedly different from the isostructural Sr2RuO4, only two bands with dominant Rh 4dxz,zy character contribute to the Fermi surface. A quantitative analysis of the photoemission quasiparticle band structure is in excellent agreement with bulk data. In contrast, it is found that state-of-the-art density functional calculations in the local density approximation differ significantly from the experimental findings.