We have found that surface superstructures made of "monolayer alloys" of Tl and Pb on Si(111), having giant Rashba effect, produce non-reciprocal spin-polarized photocurrent via circular photogalvanic effect (CPGE) by obliquely shining circularly polarized near-infrared (IR) light. CPGE is here caused by injection of in-plane spin into spin-split surface-state bands, which is observed only on Tl-Pb alloy layers, but not on single-element Tl nor Pb layers. In the Tl-Pb monolayer alloys, despite their monatomic thickness, the magnitude of CPGE is comparable to or even larger than the cases of many other spin-split thin-film materials. The data analysis has provided the relative permittivity $ε^{\ast}$ of the monolayer alloys to be $\sim$ 1.0, which is because the monolayer exists at a transition region between the vacuum and the substrate. The present result opens the possibility that we can optically manipulate spins of electrons even on monolayer materials.
Although most theoretical calculations of quantum wells with non-square profiles assume that material composition is varied continuously, it is more common in experiment to grow digital alloys. We compare the Rashba spin-orbit interaction of triangular wells using continuous, discrete, and digital alloying profiles in (001)-grown triangular InSb/Al_f(z)In_(1-f(z))Sb, finding a very large difference between digital alloying and the others, including a sign change in the Rashba spin-orbit coupling. We find that the interface contribution to the Rashba spin-orbit coupling is much larger in the co…
The Bi/Ag(111), Pb/Ag(111), and Sb/Ag(111) surface alloys exhibit a two-dimensional band structure with a strongly enhanced Rashba-type spin-splitting, which is in part attributed to the structural asymmetry resulting from an outward relaxation of the alloy atoms. In order to gain further insight into the spin-splitting mechanism, we have experimentally determined the outward relaxation of the alloy atoms in these surface alloys using quantitative low-energy electron diffraction (LEED). The structure plays an important role in the size of the spinsplitting as it dictates the potential landscap…
Atomically thin two-dimensional (2D) layered semiconductors such as transition metal dichalcogenides (TMDs) have attracted considerable attention due to their tunable band gap, intriguing spin-valley physics, piezoelectric effects and potential device applications. Here we study the electronic properties of a single layer WS$_{1.4}$Se$_{0.6}$ alloys. The electronic structure of this alloy, explored using angle resolved photoemission spectroscopy, shows a clear valence band structure anisotropy characterized by two paraboloids shifted in one direction of the k-space by a constant in-plane vecto…
We study the circular photogalvanic effect in the organometal halide perovskite solar cell absorber CH$_3$NH$_3$PbI$_3$. For crystal structures which lack inversion symmetry, the calculated photocurrent density is about $10^{-9}$ A/W, comparable to the previously studied quantum well and bulk Rashba systems. Because of the dependence of the circular photogalvanic effect on inversion symmetry breaking, the degree of inversion asymmetry at different depths from the surface can be probed by tuning the photon energy and associated penetration depth. We propose that measurements of this effect may …
We have studied the circular photogalvanic effect (CPGE) in Cu/Bi bilayers. When a circularly polarized light in the visible range is irradiated to the bilayer from an oblique incidence, we find a photocurrent that depends on the helicity of light. Such photocurrent appears in a direction perpendicular to the light plane of incidence but is absent in the parallel configuration. The helicity dependent photocurrent is significantly reduced for a Bi single layer film and the effect is nearly absent for a Cu single layer film. Conventional interpretation of the CPGE suggests the existence of spin-…
By detailed first-principles calculations we show that the Fermi energy and the Rashba splitting in disordered ternary surface alloys (BiPbSb)/Ag(111) can be independently tuned by choosing the concentrations of Bi and Pb. The findings are explained by three fundamental mechanisms, namely the relaxation of the adatoms, the strength of the atomic spin-orbit coupling, and band filling. By mapping the Rashba characteristics,i.e.the splitting and the Rashba energy, and the Fermi energy of the surface states in the complete range of concentrations. Our results suggest to investigate experimentally …
We performed density functional calculations for ultra-thin bismuth surface alloys: surface alloys of bismuth and face-centered cubic metals Bi/$M$(111)-$(\sqrt{3}\times\sqrt{3})R30°$ ($M$=Cu, Ag, Au, Ni, Co, and Fe). Our calculated Rashba parameters for the Bi/Ag are consistent with the previous experimental and theoretical results. We predicted a trend in the Rashba coefficients $α_R$ of bands around the Fermi energy for noble metals as follows: Bi/Ag > Bi/Cu > Bi/Au. As for the transition metals, there is a trend in $α_R$: Bi/Ni > Bi/Co > Bi/Fe. Our finding may lead to design efficient spin…
Spin-split Rashba bands have been exploited to efficiently control the spin degree of freedom of moving electrons, which possesses a great potential in frontier applications of designing spintronic devices and processing spin-based information. Given that intrinsic breaking of inversion symmetry and sizeable spin-orbit interaction, two-dimensional (2D) surface alloys formed by heavy metal elements exhibit a pronounced Rashba-type spin splitting of the surface states. Here, we have revealed the essential role of atomic orbital symmetry in the hexagonally warped Rashba spin-split surface state o…
A large and ideal Rashba-type spin-orbit splitting is desired for the applications of materials in spintronic devices and the detection of Majorana Fermions in solids. Here, we propose an approach to achieve giant and ideal spin-orbit splittings through a combination of ordered surface alloying and interface engineering, that is, growing alloy monolayers on an insulating polar surface. We illustrate this unique strategy by means of first-principles calculations of buckled hexagonal monolayers of SbBi and PbBi supported on Al$_2$O$_3$(0001). Both systems display ideal Rashba-type states with gi…
Interest in substitutional disordered alloys has recently reemerged with focus on the symmetry-sensitive properties in the alloy such as topological insulation and Rashba effect. A substitutional random alloy manifests a distribution of local environments, creating a polymorphous network. While the macroscopic average (monomorphous) structure may have the original high symmetry of the constituent compounds, many observable physical properties are sensitive to local symmetry, and are hence $<P(S_i)>$ rather than $P(S_0)$=$P(<S_i>)$. The fundamental difference between polymorphous $<P(S_i)>$ and…
In spintronic devices, the two main approaches to actively control the electrons' spin degree of freedom involve either static magnetic or electric fields. An alternative avenue relies on the application of optical fields to generate spin currents, which promises to bolster spin-device performance allowing for significantly faster and more efficient spin logic. To date, research has mainly focused on the optical injection of spin currents through the photogalvanic effect, and little is known about the direct optical control of the intrinsic spin splitting. Here, to explore the all-optical mani…
We have studied the BiCu$_2$/Cu(111) surface alloy using low-temperature scanning tunneling microscopy and spectroscopy. We observed standing waves caused by scattering off defects and step edges. Different from previous studies on similar Rashba-type surfaces, we identified multiple scattering vectors that originate from various intraband as well as interband scattering processes. A detailed energy-dependent analysis of the standing-wave patterns enables a quantitative determination of band dispersions, including the Rashba splitting. The results are in good agreement with ARPES data and demo…
Spin-orbit splitting of surface states is analyzed within and beyond the Rashba model using as examples the (111) surfaces of noble metals, Ag2Bi surface alloy, and topological insulator Bi2Se3. The ab initio analysis of relativistic velocity proves the Rashba model to be fundamentally inapplicable to real crystals. The splitting is found to be primarily due to a spin-orbit induced in-plane modification of the wave function, namely to its effect on the nonrelativistic Hamiltonian. The usual Rashba splitting -- given by charge distribution asymmetry -- is an order of magnitude smaller.
We report the preparation of the interface between graphene and the strong Rashba-split BiAg$_2$ surface alloy and investigatigation of its structure as well as the electronic properties by means of scanning tunneling microscopy/spectroscopy and density functional theory calculations. Upon evaluation of the quasiparticle interference patterns the unpertrubated linear dispersion for the $π$ band of $n$-doped graphene is observed. Our results also reveal the intact nature of the giant Rashba-split surface states of the BiAg$_2$ alloy, which demonstrate only a moderate downward energy shift upon …
Spin polarized two-dimensional electronic states have been previously observed on metallic surface alloys with giant Rashba splitting and on the surface of topological insulators. We study the surface band structure of these systems, in a unified manner, by exploiting recent results of k.p theory. The model suggests a different way to address the effect of anisotropy in Rashba systems. Changes in the surface band structure of various Rashba compounds can be captured by a single effective parameter which quantifies the competition between the Rashba effect and the hexagonal warping of the const…
Deploying an analytical atomistic model of the bulk band structure of the IV-VI semiconductors we connect the spin structure of the topological surface state to the crystal field and spin orbit coupling parameters of the bulk material. While the Dirac-Weyl (or equivalently, Rashba) type topological surface state is often assumed universal, we show that the physics of the surface state is strikingly non-universal. To see this explicitly we calculate the RKKY interaction, which may be viewed as a probe of this surface state spin structure, finding its \emph{qualitative form} depends on the value…
By means of density functional theory based calculations, we study the role of spin-orbit coupling in the new family of ABC hyperferroelectrics [Phys. Rev. Lett. 112, 127601 (2014)]. We unveil an extremely rich physics strongly linked to ferroelectric properties, ranging from the electric control of bulk Rashba effect to the existence of a three dimensional topological insulator phase, with concomitant topological surface states even in the ultrathin film limit. Moreover, we predict that the topological transition, as induced by alloying, is followed by a Weyl semi-metal phase of finite concen…
The Fermi and Rashba energies of surface states in the Bi_xPb_{1-x}/Ag(111) alloy can be tuned simultaneously by changing the composition parameter x. We report on unconventional Fermi surface spin textures observed by spin and angle-resolved photoemission spectroscopy {that are correlated with a topological transition of the Fermi surface occurring at x=0.5. We show that the surface states remain fully spin polarized upon alloying and that the spin polarization vectors are approximately tangential to the constant energy contours. We discuss the implications of the topological transition for t…
Here, we report first principles calculations and analysis of laser-induced photocurrents at the surface of a prototype Rashba system. By referring to Keldysh non-equilibrium formalism combined with the Wannier interpolation scheme we perform first-principles electronic structure calculations of a prototype BiAg$_2$ surface alloy, which is a well-known material realization of the Rashba model. In addition to non-magnetic ground state situation we also study the case of in-plane magnetized BiAg$_2$. We calculate the laser-induced charge photocurrents for the ferromagnetic case and the laser-ind…
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 sta…
The effective linear coupling coefficient and the total spin-splitting are calculated in Ga- and N- face InGaN quantum wells. Alloy content, geometry, and gate voltage affect an internal field and an electron density distribution in the growth direction that has direct effect on a spin-splitting. The sign of structural inversion asymmetry (SIA) spin-orbit coupling coefficient depends on an internal electric field in the well that results in different signs for Ga-face and N-face III-Nitride structures. The effective linear coupling coefficient is always positive because of the Dresselhaus-type…
We have investigated the atomic and electronic structure of the ($\sqrt{3}\times \sqrt{3}$)$R30^{\circ}$ SnAu$_2$/Au(111) surface alloy. Low energy electron diffraction and scanning tunneling microscopy measurements show that the native herringbone reconstruction of bare Au(111) surface remains intact after formation of a long range ordered ($\sqrt{3}\times \sqrt{3}$)$R30^{\circ}$ SnAu$_2$2/Au(111) surface alloy. Angle-resolved photoemission and two-photon photoemission spectroscopy techniques reveal Rashba-type spin-split bands in the occupied valence band with comparable momentum space split…
In order to carefully address the interplay between substitutional disorder and spin-orbit-coupling in IV-VI alloys, we propose a novel theoretical approach that integrates the reliability of plane-wave based density-functional theory beyond the local-density approximation with the Coherent Potential Approximation. By applying the proposed method to ternary chalcogenide alloys, we predict a substantial robustness of spectral features close to the Fermi energy against substitutional disorder. Supplementing our first-principles calculations with the analysis of the $k \cdot p$ model for rock-sal…
We have studied theoretically the Weyl semimetals the point symmetry group of which has reflection planes and which contain equivalent valleys with opposite chiralities. These include the most frequently studied compounds, namely the transition metals monopnictides TaAs, NbAs, TaP, NbP, and also Bi$_{1-x}$Sb$_x$ alloys. The circular photogalvanic current, which inverts its direction under reversal of the light circular polarization, has been calculated for the light absorption under direct optical transitions near the Weyl points. In the studied materials, the total contribution of all the val…
We report on a novel material, namely two-dimensional (2D) V$_{1-x}$Pt$_x$Se$_2$ alloy, exhibiting simultaneously ferromagnetic order and Rashba spin-orbit coupling. While ferromagnetism is absent in 1T-VSe$_2$ due to the competition with the charge density wave phase, we demonstrate theoretically and experimentally that the substitution of vanadium by platinum in VSe$_2$ (10-50 %) to form an homogeneous 2D alloy restores ferromagnetic order with Curie temperatures of 6 K for 5 monolayers and 25 K for one monolayer of V$_{0.65}$Pt$_{0.35}$Se$_2$. Moreover, the presence of platinum atoms gives …
The quantum mechanical screening of a spin via conduction electrons depends sensitively on the environment seen by the magnetic impurity. A high degree of responsiveness can be obtained with metal complexes, as the embedding of a metal ion into an organic molecule prevents intercalation or alloying and allows for a good control by an appropriate choice of the ligands. There are therefore hopes to reach an "on demand" control of the spin state of single molecules adsorbed on substrates. Hitherto one route was to rely on "switchable" molecules with intrinsic bistabilities triggered by external s…
Conventional spin-degenerated surface electrons have been effectively manipulated by using organic and inorganic self-assembled nanoarrays as resonators. Step superlattices naturally assembled in vicinal surfaces are a particularly interesting case since they represent simple one-dimensional (1D) models for fundamental studies, and can imprint strong anisotropies in surface electron transport in real devices. Here we present the first realization of periodic resonator arrays on the BiAg2 atom-thick surface alloy with unprecedented atomic precision, and demonstrate their potential ability for t…
Nanostructured composites and nanowire arrays of traditional thermoelectrics like Bi, Bi(1-x)Sb(x) and Bi(2)Te(3) have metallic Rashba surface spin-orbit bands featuring high mobilities rivaling that of the bulk for which topological insulator behavior has been proposed. Nearly pure surface electronic transport has been observed at low temperatures in Bi nanowires with diameter around the critical diameter, 50 nm, for the semimetal-to semiconductor transition. The surface contributes strongly to the thermopower, actually dominating for temperatures T < 100 K in these nanowires. The surface the…
Spin polarization enhancement in a single-layer Bi(1-x)Sb(x) alloy on Ag(111) via isovalent substitution
Centro Atómico Bariloche, CNEA y CONICET（巴里洛切原子中心，国家原子能委员会和阿根廷科学研究委员会）；Consiglio Nazionale delle Ricerche, Istituto di Struttura della Materia (CNR-ISM)（意大利国家研究委员会，物质结构研究所）；Instituto de Nanociencia y Nanotecnología (CNEA - CONICET)（纳米科学与纳米技术研究所（国家原子能委员会-阿根廷科学研究委员会））
Electrical manipulation of magnetization by spin-orbit torque (SOT) has shown promise for realizing reliable magnetic memories and oscillators. To date, the generation of transverse spin current and SOT, whether it is of spin Hall effect (SHE), Rashba-Edelstein effect or spin-momentum locking origin, relies primarily on materials or heterostructures containing 5$d$ or 6$p$ heavy elements with strong spin-orbit coupling. Here we show that a paramagnetic CoGa compound possesses large enough spin Hall angle to allow robust SOT switching of perpendicularly-magnetized ferrimagnetic MnGa films in Co…
