A comprehensive mapping of the spin polarization of the electronic bands in ferroelectric a-GeTe(111) films has been performed using a time-of-flight momentum microscope equipped with an imaging spin filter that enables a simultaneous measurement of more than 10.000 data points (voxels). A Rashba type splitting of both surface and bulk bands with opposite spin helicity of the inner and outer Rashba bands is found revealing a complex spin texture at the Fermi energy. The switchable inner electric field of GeTe implies new functionalities for spintronic devices.
In systems with broken inversion symmetry spin-orbit coupling (SOC) yields a Rashba-type spin splitting of electronic states, manifested in a k-dependent splitting of the bands. While most research had previously focused on 2D electron systems, recently a three-dimensional (3D) form of such Rashba-effect was found in a series of bismuth tellurohalides. Whereas these materials exhibit a very large spin-splitting, they lack an important property concerning functionalization, namely the possibility to switch or tune the spin texture. This limitation can be overcome in a new class of functional materials displaying Rashba-splitting coupled to ferroelectricity: the ferroelectric Rashba semiconductors (FERS). Using spin- and angle-resolved photoemission spectroscopy (SARPES) we show that GeTe(111) forms a prime member of this class, displaying a complex spin-texture for the Rashba-split surface and bulk bands arising from the intrinsic inversion symmetry breaking caused by the ferroelectric polarization of the bulk (FE). Apart from pure surface and bulk states we find surface-bulk resonant states (SBR) whose wavefunctions entangle the spinors from the bulk and surface contributions. At the Fermi level their hybridization results in unconventional spin topologies with cochiral helicities and concomitant gap opening. The GeTe(111) surface and SBR states make the semiconductor surface conducting. At the same time our SARPES data confirm that GeTe is a narrow-gap semiconductor, suggesting that GeTe(111) electronic states are endowed with spin properties that are theoretically challenging to anticipate. As the helicity of the spins in Rashba bands is connected to the direction of the FE polarization, this work paves the way to all-electric non-volatile control of spin-transport properties in semiconductors.
$alpha$-GeTe(111) is a non-centrosymmetric ferroelectric material, for which a strong spin-orbit interaction gives rise to giant Rashba split states in the bulk and at the surface. The detailed dispersions of the surface states inside the bulk band gap remains an open question because they are located in the unoccupied part of the electronic structure, making them inaccessible to static angle-resolved photoemission spectroscopy. We show that this difficulty can be overcome via in-situ potassium doping of the surface, leading to a rigid shift of 80 meV of the surface states into the occupied states. Thus, we resolve in great detail their dispersion and highlight their crossing at the $bar{Gamma}$ point, which, in comparison with density functional theory calculations, definitively confirms the Rashba mechanism.
We use spin- and angle-resolved photoemission spectroscopy (SARPES) combined with polarization-variable laser and investigate the spin-orbit coupling effect under interband hybridization of Rashba spin-split states for the surface alloys Bi/Ag(111) and Bi/Cu(111). In addition to the conventional band mapping of photoemission for Rashba spin-splitting, the different orbital and spin parts of the surface wavefucntion are directly imaged into energy-momentum space. It is unambiguously revealed that the interband spin-orbit coupling modifies the spin and orbital character of the Rashba surface states leading to the enriched spin-orbital entanglement and the pronounced momentum dependence of the spin-polarization. The hybridization thus strongly deviates the spin and orbital characters from the standard Rashba model. The complex spin texture under interband spin-orbit hybridyzation proposed by first-principles calculation is experimentally unraveled by SARPES with a combination of p- and s-polarized light.
Ferroelectric Rashba semiconductors (FERSC) have recently emerged as a promising class of spintronics materials. The peculiar coupling between spin and polar degrees of freedom responsible for several exceptional properties, including ferroelectric switching of Rashba spin texture, suggests that the electrons spin could be controlled by using only electric fields. In this regard, recent experimental studies revealing charge-to-spin interconversion phenomena in two prototypical FERSC, GeTe and SnTe, appear extremely relevant. Here, by employing density functional theory calculations, we investigate spin Hall effect (SHE) in these materials and show that it can be large either in ferroelectric or paraelectric structure. We further explore the compatibility between doping required for the practical realization of SHE in semiconductors and polar distortions which determine Rashba-related phenomena in FERSC, but which could be suppressed by free charge carriers. Based on the analysis of the lone pairs which drive ferroelectricity in these materials, we have found that the polar displacements in GeTe can be sustained up to a critical hole concentration of over $sim 10^{21}$/cm$^{3}$, while the tiny distortions in SnTe vanish at a minimal level of doping. Finally, we have estimated spin Hall angles for doped structures and demonstrated that the spin Hall effect could be indeed achieved in a polar phase. We believe that the confirmation of spin Hall effect, Rashba spin textures and ferroelectricity coexisting in one material will be helpful for design of novel multifunctional spintronics devices operating without magnetic fields.
GeTe has been proposed as the father compound of a new class of functional materials displaying bulk Rashba effects coupled to ferroelectricity: ferroelectric Rashba semiconductors. In nice agreement with first principle calculations, we show by angular resolved photoemission and piezo-force microscopy that GeTe displays surface and bulk Rashba bands arising from the intrinsic inversion symmetry breaking provided by the remanent ferroelectric polarization. This work points to the possibility to control the spin chirality of bands in GeTe by acting on its ferroelectric polarization.
H. J. Elmers
,R. Wallauer
,M. Liebmann
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(2015)
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"Spin Mapping of Surface and Bulk Rashba States in Ferroelectric a-GeTe(111) Films"
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Hans-Joachim Elmers
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