J. M. Riley

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.

Observation of Ultrafast Free Carrier Dynamics in Single Layer MoS2

The dynamics of excited electrons and holes in single layer (SL) MoS2 have so far been difficult to disentangle from the excitons that dominate the optical response of this material. Here, we use time- and angle-resolved photoemission spectroscopy for a SL of MoS2 on a metallic substrate to directly measure the excited free carriers. This allows us to ascertain a direct quasiparticle band gap of 1.95 eV and determine an ultrafast (50 fs) extraction of excited free carriers via the metal in contact with the SL MoS2. This process is of key importance for optoelectronic applications that rely on separated free carriers rather than excitons.

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.

Ultrafast Band Structure Control of a Two-Dimensional Heterostructure

The electronic structure of two-dimensional (2D) semiconductors can be significantly altered by screening effects, either from free charge carriers in the material or by environmental screening from the surrounding medium. The physical properties of 2D semiconductors placed in a heterostructure with other 2D materials are therefore governed by a complex interplay of both intra- and interlayer interactions. Here, using time- and angle-resolved photoemission, we are able to isolate both the layer-resolved band structure and, more importantly, the transient band structure evolution of a model 2D heterostructure formed of a single layer of MoS2 on graphene. Our results reveal a pronounced renormalization of the quasiparticle gap of the MoS2 layer. Following optical excitation, the band gap is reduced by up to ∼400 meV on femtosecond time scales due to a persistence of strong electronic interactions despite the environmental screening by the n-doped graphene. This points to a large degree of tunability of both the electronic structure and the electron dynamics for 2D semiconductors embedded in a van der Waals-bonded heterostructure.

Nearly free electrons in a 5d delafossite oxide metal.

Transport and ARPES reveal extremely good metallicity arising from almost free-electron behavior in single-crystal PtCoO2. Understanding the role of electron correlations in strong spin-orbit transition-metal oxides is key to the realization of numerous exotic phases including spin-orbit–assisted Mott insulators, correlated topological solids, and prospective new high-temperature superconductors. To date, most attention has been focused on the 5d iridium-based oxides. We instead consider the Pt-based delafossite oxide PtCoO2. Our transport measurements, performed on single-crystal samples etched to well-defined geometries using focused ion beam techniques, yield a room temperature resistivity of only 2.1 microhm·cm (μΩ-cm), establishing PtCoO2 as the most conductive oxide known. From angle-resolved photoemission and density functional theory, we show that the underlying Fermi surface is a single cylinder of nearly hexagonal cross-section, with very weak dispersion along kz. Despite being predominantly composed of d-orbital character, the conduction band is remarkably steep, with an average effective mass of only 1.14me. Moreover, the sharp spectral features observed in photoemission remain well defined with little additional broadening for more than 500 meV below EF, pointing to suppressed electron-electron scattering. Together, our findings establish PtCoO2 as a model nearly-free–electron system in a 5d delafossite transition-metal oxide.

Spin-valley locking in the normal state of a transition-metal dichalcogenide superconductor

Metallic transition-metal dichalcogenides (TMDCs) are benchmark systems for studying and controlling intertwined electronic orders in solids, with superconductivity developing from a charge-density wave state. The interplay between such phases is thought to play a critical role in the unconventional superconductivity of cuprates, Fe-based and heavy-fermion systems, yet even for the more moderately-correlated TMDCs, their nature and origins have proved controversial. Here, we study a prototypical example, 2H-NbSe2, by spin- and angle-resolved photoemission and first-principles theory. We find that the normal state, from which its hallmark collective phases emerge, is characterized by quasiparticles whose spin is locked to their valley pseudospin. This results from a combination of strong spin–orbit interactions and local inversion symmetry breaking, while interlayer coupling further drives a rich three-dimensional momentum dependence of the underlying Fermi-surface spin texture. These findings necessitate a re-investigation of the nature of charge order and superconducting pairing in NbSe2 and related TMDCs.

Spin and valley control of free carriers in single-layer WS2

The semiconducting single-layer transition metal dichalcogenides have been identified as ideal materials for accessing and manipulating spin- and valley-quantum numbers due to a set of favorable optical selection rules in these materials. Here, we apply time- and angle-resolved photoemission spectroscopy to directly probe optically excited free carriers in the electronic band structure of a high quality single layer of WS

Narrow-band anisotropic electronic structure of ReS2

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Maximal Rashba-like spin splitting via kinetic energy-coupled inversion symmetry breaking

. We observe that the optically generated free hole density in a single valley can be increased by a factor of 2 using a circularly polarized optical excitation. Moreover, we find that by varying the photon energy of the excitation we can tune the free carrier density in a given spin-split state around the valence band maximum of the material. The control of the photon energy and polarization of the excitation thus permits us to selectively excite free electron-hole pairs with a given spin and within a single valley.

Crossover from lattice to plasmonic polarons of a spin-polarised electron gas in ferromagnetic EuO

We have used angle-resolved photoemission spectroscopy to investigate the band structure of