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Register a new userDirect observation of local Rashba spin polarization and spin-layer locking in centrosymmetric monolayer PtSe$_2$
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The generally accepted view that spin polarization is induced by the asymmetry of the global crystal space group has limited the search for spintronics [1] materials to non-centrosymmetric materials. Recently it has been suggested that spin polarization originates fundamentally from local atomic site asymmetries [2], and therefore centrosymmetric materials may exhibit previously overlooked spin polarizations. Here by using spin- and angle-resolved photoemission spectroscopy (spin-ARPES), we report helical spin texture induced by local Rashba effect (R-2) in centrosymmetric monolayer PtSe$_2$ film. First-principles calculations and effective analytical model support the spin-layer locking picture: in contrast to the spin splitting in conventional Rashba effect (R-1), the opposite spin polarizations induced by R-2 are degenerate in energy while spatially separated in the top and bottom Se layers. These results not only enrich our understanding of spin polarization physics, but also may find applications in electrically tunable spintronics.
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Spin polarization effects in nonmagnetic materials are generally believed as an outcome of spin-orbit coupling provided that the global inversion symmetry is lacking, also known as spin-momentum locking. The recently discovered hidden spin polarization indicates that specific atomic site asymmetry could also induce measurable spin polarization, leading to a paradigm shift to centrosymmetric crystals for potential spintronic applications. Here, combining spin- and angle-resolved photoemission spectroscopy and theoretical calculations, we report distinct spin-layer locking phenomena surrounding different high-symmetry momenta in a centrosymmetric, layered material BiOI. The measured spin is highly polarized along the Brillouin zone boundary, while is almost vanishing around the zone center due to its nonsymmorphic crystal structure. Our work not only demonstrates the existence of hidden spin polarization, but also uncovers the microscopic mechanism of the way spin, momentum and layer locking to each other, shedding lights on the design metrics for future spintronic devices.
In monolayer Transition Metal Dichalcogenides (TMDs) the valence and conduction bands are spin split because of the strong spin-orbit interaction. In tungsten-based TMDs the spin-ordering of the conduction band is such that the so-called dark exciton, consisting of an electron and a hole with opposite spin orientation, has lower energy than the A exciton. A possible mechanism leading to the transition from bright to dark excitons involves the scattering of the electrons from the upper to the lower conduction band state in K. Here we exploit the valley selective optical selection rules and use two-color helicity-resolved pump-probe spectroscopy to directly measure the intravalley spin-flip relaxation dynamics of electrons in the conduction band of single-layer WS$_2$. This process occurs on a sub-ps time scale and it is significantly dependent on the temperature, indicative of a phonon-assisted relaxation. These experimental results are supported by time-dependent ab-initio calculations which show that the intra-valley spin-flip scattering occurs on significantly longer time scales only exactly at the K point. In a realistic situation the occupation of states away from the minimum of the conduction band leads to a dramatic reduction of the scattering time.
A recent 2D spinFET concept proposes to switch electrostatically between two separate sublayers with strong and opposite intrinsic Rashba effects. This concept exploits the spin-layer locking mechanism present in centrosymmetric materials with local dipole fields, where a weak electric field can easily manipulate just one of the spin channels. Here, we propose a novel monolayer material within this family, lutetium oxide iodide (LuIO). It displays one of the largest Rashba effects among 2D materials (up to $k_R = 0.08$ {AA}$^{-1}$), leading to a $pi/2$ rotation of the spins over just 1 nm. The monolayer had been predicted to be exfoliable from its experimentally-known 3D bulk counterpart, with a binding energy even lower than graphene. We characterize and model with first-principles simulations the interplay of the two gate-controlled parameters for such devices: doping and spin channel selection. We show that the ability to split the spin channels in energy diminishes with doping, leading to specific gate-operation guidelines that can apply to all devices based on spin-layer locking.
Valley pseudospin in two-dimensional (2D) transition-metal dichalcogenides (TMDs) allows optical control of spin-valley polarization and intervalley quantum coherence. Defect states in TMDs give rise to new exciton features and theoretically exhibit spin-valley polarization; however, experimental achievement of this phenomenon remains challenges. Here, we report unambiguous valley pseudospin of defect-bound localized excitons in CVD-grown monolayer MoS2; enhanced valley Zeeman splitting with an effective g-factor of -6.2 is observed. Our results reveal that all five d-orbitals and the increased effective electron mass contribute to the band shift of defect states, demonstrating a new physics of the magnetic responses of defect-bound localized excitons, strikingly different from that of A excitons. Our work paves the way for the manipulation of the spin-valley degrees of freedom through defects toward valleytronic devices.
We report scanning tunneling microscopy (STM) and spectroscopy (STS) measurements of monolayer and bilayer WSe$_2$. We measure a band gap of 2.21 $pm$ 0.08 eV in monolayer WSe$_2$, which is much larger than the energy of the photoluminescence peak indicating a large excitonic binding energy. We additionally observe significant electronic scattering arising from atomic-scale defects. Using Fourier transform STS (FT-STS), we map the energy versus momentum dispersion relations for monolayer and bilayer WSe$_2$. Further, by tracking allowed and forbidden scattering channels as a function of energy we infer the spin texture of both the conduction and valence bands. We observe a large spin-splitting of the valence band due to strong spin-orbit coupling, and additionally observe spin-valley-layer coupling in the conduction band of bilayer WSe$_2$.
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