Spin-split States Research Articles

Structural fluctuations cause spin-split states in tetragonal (CH3NH3)PbI3 as evidenced by the circular photogalvanic effect

Lead halide perovskites are used in thin-film solar cells, which owe their high efficiency to the long lifetimes of photocarriers. Various calculations find that a dynamical Rashba effect could significantly contribute to these long lifetimes. This effect is predicted to cause a spin splitting of the electronic bands of inversion-symmetric crystalline materials at finite temperatures, resulting in a slightly indirect band gap. Direct experimental evidence of the existence or the strength of the spin splitting is lacking. Here, we resonantly excite photocurrents in single crystalline ([Formula: see text])[Formula: see text] with circularly polarized light to clarify the existence of spin splittings in the band structure. We observe a circular photogalvanic effect, i.e., the photocurrent depends on the light helicity, in both orthorhombic and tetragonal ([Formula: see text])[Formula: see text] At room temperature, the effect peaks for excitation photon energies [Formula: see text] meV below the direct optical band gap. Temperature-dependent measurements reveal a sign change of the effect at the orthorhombic-tetragonal phase transition, indicating different microscopic origins in the two phases. Within the tetragonal phase, both [Formula: see text] and the amplitude of the circular photogalvanic effect increase with temperature. Our findings support a dynamical Rashba effect in this phase, i.e., a spin splitting caused by thermally induced structural fluctuations which break inversion symmetry.

Giant Rashba splitting of quasi-one-dimensional surface states on Bi/InAs(110)- (2×1)

Electronic states on the Bi/InAs(110)-(2$\times$1) surface and its spin-polarized structure are revealed by angle-resolved photoelectron spectroscopy (ARPES), spin-resolved ARPES, and density-functional-theory calculation. The surface state showed quasi-one-dimensional (Q1D) dispersion and a nearly metallic character; the top of the hole-like surface band is just below the Fermi level. The size of the Rashba parameter ($\alpha_{\rm R}$) reached quite a large value ($\sim$5.5 eV\AA). The present result would provide a fertile playground for further studies of the exotic electronic phenomena in 1D or Q1D systems with the spin-split electronic states as well as for advanced spintronic devices.

Dynamic spin injection into a quantum well coupled to a spin-split bound state

We present a theoretical analysis of dynamic spin injection due to spin-dependent tunneling between a quantum well (QW) and a bound state split in spin projection due to an exchange interaction or external magnetic field. We focus on the impact of Coulomb correlations at the bound state on spin polarization and sheet density kinetics of the charge carriers in the QW. The theoretical approach is based on kinetic equations for the electron occupation numbers taking into account high order correlation functions for the bound state electrons. It is shown that the on-site Coulomb repulsion leads to an enhanced dynamic spin polarization of the electrons in the QW and a delay in the carriers tunneling into the bound state. The interplay of these two effects leads to non-trivial dependence of the spin polarization degree, which can be probed experimentally using time-resolved photoluminescence experiments. It is demonstrated that the influence of the Coulomb interactions can be controlled by adjusting the relaxation rates. These findings open a new way of studying the Hubbard-like electron interactions experimentally.

Peculiar Rashba spin texture induced by C3v symmetry on the Bi(111) surface revisited

The spin texture of the spin-split surface states on Bi(111) has been comprehensively investigated by high energy and angular resolution spin- and angle-resolved photoelectron spectroscopy. A large out-of-plane spin component that alternately changes its sign is clearly observed. There is no evidence for peculiar polarization oscillation of the in-plane spin component, which was suggested to be due to breaking of the time-reversal symmetry in a previous report [A. Takayama et al., Phys. Rev. Lett. 106, 166401 (2011)]. The observed band structure and spin polarization are well reproduced by the $kp$ model Hamiltonian considering the ${C}_{3v}$ crystal symmetry, and the in-plane polarization variation at the different $k$ points can be understood by the photoemission final-state effect.

A Two-Dimensional Manganese Gallium Nitride Surface Structure Showing Ferromagnetism at Room Temperature

Practical applications of semiconductor spintronic devices necessitate ferromagnetic behavior at or above room temperature. In this paper, we demonstrate a two-dimensional manganese gallium nitride surface structure (MnGaN-2D) which is atomically thin and shows ferromagnetic domain structure at room temperature as measured by spin-resolved scanning tunneling microscopy and spectroscopy. Application of small magnetic fields proves that the observed magnetic domains follow a hysteretic behavior. Two initially oppositely oriented MnGaN-2D domains are rotated into alignment with only 120 mT and remain mostly in alignment at remanence. The measurements are further supported by first-principles theoretical calculations which reveal highly spin-polarized and spin-split surface states with spin polarization of up to 95% for manganese local density of states.

Direct evidence of hidden local spin polarization in a centrosymmetric superconductor LaO0.55 F0.45BiS2

Conventional Rashba spin polarization is caused by the combination of strong spin–orbit interaction and spatial inversion asymmetry. However, Rashba–Dresselhaus-type spin-split states are predicted in the centrosymmetric LaOBiS2 system by recent theory, which stem from the local inversion asymmetry of active BiS2 layer. By performing high-resolution spin- and angle-resolved photoemission spectroscopy, we have investigated the electronic band structure and spin texture of superconductor LaO0.55F0.45BiS2. Here we present direct spectroscopic evidence for the local spin polarization of both the valence band and the conduction band. In particular, the coexistence of Rashba-like and Dresselhaus-like spin textures has been observed in the conduction band. The finding is of key importance for fabrication of proposed dual-gated spin-field effect transistor. Moreover, the spin-split band leads to a spin–momentum locking Fermi surface from which superconductivity emerges. Our demonstration not only expands the scope of spintronic materials but also enhances the understanding of spin–orbit interaction-related superconductivity.

La interstitial defect-induced insulator-metal transition in the oxide heterostructures LaAlO3/SrTiO3

Perovskite oxide interfaces have attracted tremendous research interest for their fundamental physics and promising all-oxide electronics applications. Here, based on first-principles calculations, we propose a novel surface La interstitial promoted interface insulator-metal transition in LaAlO3/SrTiO3 (110). Compared with surface oxygen vacancies, which play a determining role on the insulator-metal transition of LaAlO3/SrTiO3 (001) interfaces, we find that surface La interstitials can be more experimentally realistic and accessible for manipulation and more stable in ambient atmospheric environment. Interestingly, these surface La interstitials also induce significant spin-splitting states with Ti dyz/dxz character at conducting LaAlO3/SrTiO3 (110) interface. On the other hand, for insulating LaAlO3/SrTiO3 (110) (<4 unit cells LaAlO3 thickness), a distortion between La (Al) and O atoms is found at the LaAlO3 side, partially compensating the polarization divergence. Our results reveal the origin of metal-insulator transition in LaAlO3/SrTiO3 (110) heterostructures, and also shed light on the manipulation of the superior properties of LaAlO3/SrTiO3 (110) for new possibilities of electronic and magnetic applications.

Superior Electronic Structure in Two-Dimensional MnPSe3/MoS2 van der Waals Heterostructures

We explore the electronic structure of two-dimensional (2D) MnPSe3/MoS2 van der Waals (vdW) heterostructures based on density functional theory. A novel spin splitting at the valance band maximum of MnPSe3 appears in some specific stacking models due to Mn d orbital hybridization. The simultaneous spin and valley splitting can be achieved by interfacial coupling, which is attractive for manipulation of the valley and spin degrees of freedom. More importantly, due to the antiferromagnetic ordering of manganese, the opposite spin moments at K and K′ valleys can be observed by transforming configurations, which realizes the tunable spin splitting states. Our theoretical work opens up the opportunities of valley and spin related applications of MnPSe3/MoS2 vdW heterostructures and offers a practical avenue for exploring novel devices based on the spin and valley degrees of freedom.

Creating anisotropic spin-split surface states in momentum space by molecular adsorption

In this ab initio study we demonstrate that molecular adsorption on a surface Rashba system can be used to modulate the surface electronic structure in different momentum space directions, i.e., to create anisotropic spin splittings in $\mathbf{k}$ space. This effect is rooted in the asymmetric adsorption of the molecules on the surface in a hollow site which breaks the surface symmetry. More specifically, we demonstrate that the physisorbed ${\mathrm{NH}}_{3}$ has a small influence on the surface Rashba states and only gives rise to variations of the surface state Rashba parameters up to a factor of 1.4 over the surface Brillouin zone. In contrast, the chemisorption of ${\mathrm{BH}}_{3}$ leads to variations of the Rashba parameter by more than a factor of 2.5. Consequently, the anisotropy of the Rashba-split-surface states induced by molecular adsorption also gives rise to a modulation of the surface state spin texture, i.e., the out-of-plane spin polarization varies along different $\mathbf{k}$ directions by up to 70% for the occupied states. This offers the possibility to change the spin direction from in-plane to predominantly out-of-plane by modifying the electronic momentum by 90\ifmmode^\circ\else\textdegree\fi{}.

Rashba spin-orbit coupling in graphene monolayer coated by periodic magnetic stripes

We investigate theoretically the effects of a modulated periodic perpendicular magnetic fields and the Rashba spin-orbit coupling (RSOC) on the electronic states and optical absorption spectrum in a graphene monolayer. The magnetic fields and supperlattice geometry give rise to distinct Dirac cone shift and open a finite bandgap at the Dirac point. In contrast to the energy spectrum without the RSOC interaction, we find that the RSOC term will develop a spin-splitting energy-momentum dispersion relation in this graphene magnetic supperlattice. Anisotropic and spin-split group velocities, effective masses and the momentum-dependent carrier distributions along the magnetic strips are demonstrated. And the manipulations of these exotic properties by tuning the magnetic fields and the RSOC are addressed systematically. Accordingly, we find bright-to-dark transitions in the electron-hole pairs transition rate spectrum and absorption peak splitting in the optical absorption spectrum tuned by the RSOC interaction. This feature offers us a practical way to detect these band engineering effects especially the exotic spin splitting states by using the conductance and optical technique.

Molecular and electronic structures and magnetic properties of multilayer graphene nanoclusters and their changes under the influence of adsorbed molecules

The results of investigations of the structures and properties of multilayer graphene nano-clusters (nanographites), structural blocks of activated carbon fibers, and their changes under the influence of adsorbed molecules are presented. The presence of specific edge p-electron-ic states in the nanographites and a reversible decrease in their density at the Fermi level upon the interaction of the graphite nanoparticles with adsorbed molecules of oxygen, chlorine, and water were found. The explanation of the discovered effect was proposed in the terms of the model of spin splitting of edge p-electronic states initiated by the transfer of a small fraction of the electron density from the nanographites to adsorbed molecules. The change in the sign of the temperature coefficient of current carrier spin relaxation rate in the presence of adsorbates can be accounted for by their interaction with edge spin-split (magnetically ordered) states. The preservation of peripheral p-electronic states of the nanographites of free (dangling) s-orbitals of edge carbon atoms at saturation with chlorine was substantiated.

Growth-Controlled Engineering of Magnetic Exchange Interactions in Single Crystalline GaCoZnO1-v Epitaxial Films with High Co Concentration

While semiconductor spintronics promises lower switching energy and faster speed, a major limitation on its development as a viable technology is the lack of room temperature ferromagnetic semiconductor materials. The material challenge is great, because not only magnetic and electronic doping but also thermally robust coupling between them are required for a room temperature ferromagnetic semiconductor. Here, we report the growth-controlled engineering of magnetic exchange interactions in single crystalline GaCoZnO1-v epitaxial films with high Co concentrations (0.3 ≤ x ≤ 0.45) by controlling oxygen vacancy and carrier density through Ga3+ doping. Strong ferromagnetism, spin-split impurity states, and spin-polarized electrical transport are realized and well controlled at room temperature by tailoring the s,p–d exchange coupling. This room temperature ferromagnetic semiconductor, which offers the ability to individually control carrier density and magnetic doping, will lay a solid foundation for the deve...

Persistence of a surface state arc in the topologically trivial phase of MoTe2

The prediction of Weyl fermions in the low-temperature noncentrosymmetric $1{T}^{\ensuremath{'}}$ phase of ${\mathrm{MoTe}}_{2}$ still awaits clear experimental confirmation. Here, we report angle-resolved photoemission (ARPES) data and ab initio calculations that reveal a surface state arc dispersing between the valence and the conduction band, as expected for a Weyl semimetal. However, we find that the arc survives in the high-temperature centrosymmetric $1{T}^{\ensuremath{'}\ensuremath{'}}$ phase. Therefore, a surface Fermi arc is not an unambiguous fingerprint of a topologically nontrivial phase. We have also investigated the surface state spin texture of the $1{T}^{\ensuremath{'}}$ phase by spin-resolved ARPES, and identified additional topologically trivial spin-split states within the projected band gap at higher binding energies.

The Effect of Exchange Magnetic Field on Spin Magnetic Susceptibility of Monolayer and AB-Stacked Bilayer MoS2

In this work, the spin-dependent electronic band structure and magnetic susceptibility (MS) of two graphene’s analogue, monolayer and AB-stacked bilayer MoS 2, are investigated in the presence of induced magnetization by magnetic insulators. Here, we have assumed that the type of magnetic insulators can change the magnetization strength. By focusing on the Dirac points of Brillouin zone and using the Dirac theory within the Green’s function approach, band structures and MSs of two systems are compared. In the bilayer case, gate voltage produces an electric field in order to have spin-orbit coupling (SOC) for spintronic applications. Our results represent the Stark and Zeeman effects because of the spin splitting states by electric and magnetic fields. We have found that the MS has marvelous behaviors before and after a critical magnetization in the monolayer MoS 2 while it increases slightly in bilayer lattice. Up (down) spin band gaps in bilayer MoS 2 decreases (increases) at both Dirac points due to the combined SOC and interlayer hopping potentials.

Direct mapping of spin and orbital entangled wave functions under interband spin-orbit coupling of giant Rashba spin-split surface states

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.

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$_2$. 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.

Impurity screening and stability of Fermi arcs against Coulomb and magnetic scattering in a Weyl monopnictide

We present a quasiparticle interference study of clean and Mn surface-doped TaAs, a prototypical Weyl semimetal, to test the screening properties as well as the stability of Fermi arcs against Coulomb and magnetic scattering. Contrary to topological insulators, the impurities are effectively screened in Weyl semimetals. The adatoms significantly enhance the strength of the signal such that theoretical predictions on the potential impact of Fermi arcs can be unambiguously scrutinized. Our analysis reveals the existence of three extremely short, previously unknown scattering vectors. Comparison with theory traces them back to scattering events between large parallel segments of spin-split trivial states, strongly limiting their coherence. In sharp contrast to previous work [R. Batabyal et al., Sci. Adv. 2, e1600709 (2016)], where similar but weaker subtle modulations were interpreted as evidence of quasiparticle interference originating from Femi arcs, we can safely exclude this being the case. Overall, our results indicate that intra- as well as inter-Fermi arc scattering are strongly suppressed and may explain why-in spite of their complex multiband structure-transport measurements show signatures of topological states in Weyl monopnictides.

Hidden Rashba spin-split states in a quasi-one-dimensional Au atomic chain on ferromagnetic Ni(110)

An electronic structure of a Au atomic chain on Ni(110), which was investigated decades ago, has been reinvestigated by high-resolution spin- and angle-resolved photoemission spectroscopy. Clear evidence of a Rashba spin split, i.e., spin-polarization reversal between positive and negative wave vectors with respect to the symmetry point, has been observed in the electronic bands possessing quasi-one-dimensional character. The observed spin-split state caused by spin-orbit interaction (SOI) was overlooked in the previous spin-resolved photoemission study probably due to the dominant effect of exchange splitting of the Ni substrate than the Rashba effect and poorer resolution of the previous measurement. The system containing both the Rashba-type SOI and the exchange interaction with one-dimensional character will provide a platform to investigate the effect of exchange interaction on the spin-split states caused by SOI with low dimensionality.

Direct evidence of interaction-induced Dirac cones in a monolayer silicene/Ag(111) system

Silicene, analogous to graphene, is a one-atom-thick 2D crystal of silicon, which is expected to share many of the remarkable properties of graphene. The buckled honeycomb structure of silicene, along with enhanced spin-orbit coupling, endows silicene with considerable advantages over graphene in that the spin-split states in silicene are tunable with external fields. Although the low-energy Dirac cone states lie at the heart of all novel quantum phenomena in a pristine sheet of silicene, a hotly debated question is whether these key states can survive when silicene is grown or supported on a substrate. Here we report our direct observation of Dirac cones in monolayer silicene grown on a Ag(111) substrate. By performing angle-resolved photoemission measurements on silicene(3 × 3)/Ag(111), we reveal the presence of six pairs of Dirac cones located on the edges of the first Brillouin zone of Ag(111), which is in sharp contrast to the expected six Dirac cones centered at the K points of the primary silicene(1 × 1) Brillouin zone. Our analysis shows clearly that the unusual Dirac cone structure we have observed is not tied to pristine silicene alone but originates from the combined effects of silicene(3 × 3) and the Ag(111) substrate. Our study thus identifies the case of a unique type of Dirac cone generated through the interaction of two different constituents. The observation of Dirac cones in silicene/Ag(111) opens a unique materials platform for investigating unusual quantum phenomena and for applications based on 2D silicon systems.

Accessing Rashba states in electrostatically gated topological insulator devices

We study the low temperature electrical transport in gated BiSbTe1.25Se1.75/hexagonal-Boron Nitride van der Waals heterostructure devices. Our experiments indicate the presence of Rashba spin-split states confined to the sample surface. While such states have been observed previously in photo-emission spectroscopy and STM experiments, it has not been possible to unambiguously detect them by electrical means and their transport properties remain mostly unknown. We show that these states support high mobility conduction with Hall effect mobilities ∼2000 to 3000 cm2/V-s that are paradoxically much larger than the mobilities of the topological surface states ∼300 cm2/V-s at T = 2 K. The spin-split nature of these states is confirmed by magneto-resistance measurements that reveal multi-channel weak anti-localization. Our work shows that Rashba spin split states can be electrically accessed in Topological insulators paving the way for future spintronic applications.