P. D. C. King

Creation and control of a two-dimensional electron liquid at the bare SrTiO 3 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.

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.

Conductivity in transparent oxide semiconductors

Despite an extensive research effort for over 60 years, an understanding of the origins of conductivity in wide band gap transparent conducting oxide (TCO) semiconductors remains elusive. While TCOs have already found widespread use in device applications requiring a transparent contact, there are currently enormous efforts to (i) increase the conductivity of existing materials, (ii) identify suitable alternatives, and (iii) attempt to gain semiconductor-engineering levels of control over their carrier density, essential for the incorporation of TCOs into a new generation of multifunctional transparent electronic devices. These efforts, however, are dependent on a microscopic identification of the defects and impurities leading to the high unintentional carrier densities present in these materials. Here, we review recent developments towards such an understanding. While oxygen vacancies are commonly assumed to be the source of the conductivity, there is increasing evidence that this is not a sufficient mechanism to explain the total measured carrier concentrations. In fact, many studies suggest that oxygen vacancies are deep, rather than shallow, donors, and their abundance in as-grown material is also debated. We discuss other potential contributions to the conductivity in TCOs, including other native defects, their complexes, and in particular hydrogen impurities. Convincing theoretical and experimental evidence is presented for the donor nature of hydrogen across a range of TCO materials, and while its stability and the role of interstitial versus substitutional species are still somewhat open questions, it is one of the leading contenders for yielding unintentional conductivity in TCOs. We also review recent work indicating that the surfaces of TCOs can support very high carrier densities, opposite to the case for conventional semiconductors. In thin-film materials/devices and, in particular, nanostructures, the surface can have a large impact on the total conductivity in TCOs. We discuss models that attempt to explain both the bulk and surface conductivity on the basis of bulk band structure features common across the TCOs, and compare these materials to other semiconductors. Finally, we briefly consider transparency in these materials, and its interplay with conductivity. Understanding this interplay, as well as the microscopic contenders for providing the conductivity of these materials, will prove essential to the future design and control of TCO semiconductors, and their implementation into novel multifunctional devices.

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.

Strong Electron Correlations in the Normal State of the Iron-Based FeSe0.42Te0.58 Superconductor Observed by Angle-Resolved Photoemission Spectroscopy

A. Tamai, A.Y. Ganin, E. Rozbicki, J. Bacsa, W. Meevasana, P.D.C. King, M. Caffio, R. Schaub, S. Margadonna, K. Prassides, M.J. Rosseinsky, and F. Baumberger School of Physics and Astronomy, University of St. Andrews, St. Andrews, Fife KY16 9SS, United Kingdom Department of Chemistry, University of Liverpool, Liverpool L69 7ZD, United Kingdom School of Chemistry, University of St. Andrews, St. Andrews, Fife KY16 9ST, United Kingdom School of Chemistry, University of Edinburgh, Edinburgh EH9 3JJ, United Kingdom Department of Chemistry, Durham University, Durham DH1 3LE, United Kingdom (Dated: February 10, 2010)

Direct observation of spin-polarized bulk bands in an inversion-symmetric semiconductor

The coupling between spin, valley and layer degrees of freedom in transition-metal dichalcogenides is shown to give rise to spin-polarized electron states, providing opportunities to create and manipulate spin and valley polarizations in bulk solids. Methods to generate spin-polarized electronic states in non-magnetic solids are strongly desired to enable all-electrical manipulation of electron spins for new quantum devices1. This is generally accepted to require breaking global structural inversion symmetry1,2,3,4,5. In contrast, here we report the observation from spin- and angle-resolved photoemission spectroscopy of spin-polarized bulk states in the centrosymmetric transition-metal dichalcogenide WSe2. Mediated by a lack of inversion symmetry in constituent structural units of the bulk crystal where the electronic states are localized6, we show how spin splittings up to ∼0.5 eV result, with a spin texture that is strongly modulated in both real and momentum space. Through this, our study provides direct experimental evidence for a putative locking of the spin with the layer and valley pseudospins in transition-metal dichalcogenides7,8, of key importance for using these compounds in proposed valleytronic devices.

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.

Atomic-scale control of competing electronic phases in ultrathin LaNiO3

In an effort to scale down electronic devices to atomic dimensions, the use of transition-metal oxides may provide advantages over conventional semiconductors. Their high carrier densities and short electronic length scales are desirable for miniaturization, while strong interactions that mediate exotic phase diagrams open new avenues for engineering emergent properties. Nevertheless, understanding how their correlated electronic states can be manipulated at the nanoscale remains challenging. Here, we use angle-resolved photoemission spectroscopy to uncover an abrupt destruction of Fermi liquid-like quasiparticles in the correlated metal LaNiO₃ when confined to a critical film thickness of two unit cells. This is accompanied by the onset of an insulating phase as measured by electrical transport. We show how this is driven by an instability to an incipient order of the underlying quantum many-body system, demonstrating the power of artificial confinement to harness control over competing phases in complex oxides with atomic-scale precision.

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).

Interplay of spin-orbit interactions, dimensionality, and octahedral rotations in semimetallic SrIrO(3).

We employ reactive molecular-beam epitaxy to synthesize the metastable perovskite SrIrO(3) and utilize in situ angle-resolved photoemission to reveal its electronic structure as an exotic narrow-band semimetal. We discover remarkably narrow bands which originate from a confluence of strong spin-orbit interactions, dimensionality, and both in- and out-of-plane IrO(6) octahedral rotations. The partial occupation of numerous bands with strongly mixed orbital characters signals the breakdown of the single-band Mott picture that characterizes its insulating two-dimensional counterpart, Sr(2)IrO(4), illustrating the power of structure-property relations for manipulating the subtle balance between spin-orbit interactions and electron-electron interactions.