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1.
Article in English | MEDLINE | ID: mdl-39167777

ABSTRACT

Ferroelectric Rashba semiconductors (FRS) are highly demanded for their potential capability for nonvolatile electric control of electron spins. An ideal FRS is characterized by a combination of room temperature ferroelectricity and a strong Rashba effect, which has, however, been rarely reported. Herein, we designed a room-temperature FRS by vertically stacking a Sb monolayer on a room-temperature ferroelectric In2Se3 monolayer. Our first-principles calculations reveal that the Sb/In2Se3 heterostructure exhibits a clean Rashba splitting band near the Fermi level and a strong Rashba effect coupled to the ferroelectric order. Switching the electric polarization direction enhances the Rashba effect, and the flipping is feasible with a low energy barrier of 22 meV. This Rashba-ferroelectricity coupling effect is robust against changes of the heterostructure interfacial distance and external electric fields. Such a nonvolatile electrically tunable Rashba effect at room temperature enables potential applications in next-generation data storage and logic devices operated under small electrical currents.

2.
Article in English | MEDLINE | ID: mdl-39162076

ABSTRACT

Magnetoresistance effects are crucial for understanding the charge-spin transport as well as propelling the advancement of spintronic applications. Here, we report the coexistence of magnetic-moment-dependent (MD) and magnetic-field-driven (FD) unidirectional magnetoresistance (UMR) effects in CoFeB/InSb/CdTe heterostructures. The strong spin-orbital coupling of InSb and the matched impedance at the CoFeB/InSb interface warrant a distinct MD-UMR effect at room temperature, while the interaction between the in-plane magnetic field and the Rashba effect at the InSb/CdTe interface induces the marked FD-UMR signal that dominates the high-field region. Moreover, owning to different spin scattering mechanisms, these two types of non-reciprocal charge transports show opposite polarities with respect to the magnetic field direction, which further enables an effective phase modulation of the angular-dependent magnetoresistance. The demonstration of the tunable UMR response validates our CoFeB/InSb/CdTe system as a suitable integrated building block for multifunctional spintronic memory and sensor designs.

3.
ACS Nano ; 18(28): 18405-18411, 2024 Jul 16.
Article in English | MEDLINE | ID: mdl-38970487

ABSTRACT

The unique spin texture of quantum states in topological materials underpins many proposed spintronic applications. However, realizations of such great potential are stymied by perturbations, such as temperature and local fields imposed by impurities and defects, that can render a promising quantum state uncontrollable. Here, we report room-temperature scanning tunneling microscopy/spectroscopy observation of interaction between Rashba states and topological surface states, which manifests local electronic structure along step edges controllable by the layer thickness of thin films. The first-principles theoretical calculation elucidates the robust Rashba states coexisting with topological surface states along the surface steps with characteristic spin textures in momentum space. Furthermore, the Rashba edge states can be switched off by reducing the thickness of a topological insulator Bi2Se3 to bolster their interaction with the hybridized topological surface states. The study unveils a manipulating mechanism of the spin textures at room temperature, reinforcing the necessity of thin film technology in controlling the quantum states.

4.
ACS Nano ; 18(28): 18299-18306, 2024 Jul 16.
Article in English | MEDLINE | ID: mdl-38951488

ABSTRACT

Two-dimensional (2D) hybrid organic/inorganic perovskites are an emerging materials class for optoelectronic and spintronic applications due to strong excitonic absorption and emission, large spin-orbit coupling, and Rashba spin-splitting effects. For many of the envisioned applications, tuning the majority charge carrier (electron or hole) concentration is desirable, but electronic doping of metal-halide perovskites has proven to be challenging. Here, we demonstrate electron injection into the lower-energy branch of the Rashba-split conduction band of 2D phenethylammonium lead iodide by means of n-type molecular doping at room temperature. The molecular dopant, benzyl viologen (BV), is shown to compensate adventitious p-type impurities and can lead to a tunable Fermi level above the conduction band minimum and increased conductivity in intrinsic samples. The doping-induced carrier concentration is monitored by the observation of free-carrier absorption and intraband optical transitions in the infrared spectral range. These optical measurements allow for an estimation of the Rashba splitting energy ER ≈38 ± 4 meV. Photoinduced quantum beating measurements demonstrate that the excess electron density reduces the electron spin g-factor by ca. 6%. This work demonstrates controllable carrier concentrations in hybrid organic/inorganic perovskites and yields potential for room temperature spin control through the Rashba effect.

5.
J Phys Condens Matter ; 36(41)2024 Jul 15.
Article in English | MEDLINE | ID: mdl-38959901

ABSTRACT

While the recent prediction and observation of magnetic skyrmions bears inspiring promise for next-generation spintronic devices, how to detect and track their position becomes an important issue. In this work, we investigate the spin transport in a two-dimensional magnetic nanoribbon with the Hall-bar geometry in the presence of Rashba spin-orbit coupling and magnetic skyrmions. We employ the Kwant tight-binding code to compute the Hall conductance and local spin-polarized current density. We consider two versions of the model: One with single skyrmion and one with two separate skyrmions. It is found that the size and position of the skyrmions strongly modulate the Hall conductance near the Hall-bar position. The geometry of the Hall bar also has a strong influence on the Hall conductance of the system. With the decreasing of the width of Hall leads, the peak of Hall conductance becomes sharper. We also show the spatial distribution of the spin-polarized current density around a skyrmion located at different positions. We extend this study toward two separate skyrmions, where the Hall conductance also reveals a sizable dependence on the position of the skyrmions and their distance. Our numerical analysis offers the possibility of electrically detecting the skyrmion position, which could have potential applications in ultrahigh-density storage design.

6.
J Phys Condens Matter ; 36(40)2024 Jul 09.
Article in English | MEDLINE | ID: mdl-38979851

ABSTRACT

In this study, we employ density functional theory based first-principles calculations to investigate the spin-orbit effects in the electronic structure of a polar-nonpolar sandwich heterostructure namelyLaAlO3/SrTiO3/LaAlO3. Our focus on theTi-3dbands reveals an inverted ordering of theSrTiO3-t2gorbital near the n-type interface, which is consistent with earlier experimental work. In contrast, toward the p-type interface, the orbital ordering aligns with the natural ordering ofSrTiO3orbitals, influenced by crystal field splitting. In the presence of SOC, a notable inter-orbital coupling betweent2gandegorbitals is observed within the tetragonal slab, a phenomenon not reported before in theSrTiO3-based 2D systems. Additionally, our observations highlight that the cubic Rashba splitting in this system surpasses the linear Rashba splitting, contrary to experimental findings. This comprehensive analysis contributes to a refined understanding of the role of orbital mixing in Rashba splitting in the sandwich oxide heterostructures.

7.
ACS Nano ; 2024 Jul 22.
Article in English | MEDLINE | ID: mdl-39037050

ABSTRACT

While semiconductor nanocrystals provide versatile fluorescent materials for light-emitting devices, their brightness suffers from the "dark exciton"─an optically inactive electronic state into which nanocrystals relax before emitting. Recently, a theoretical mechanism, the Rashba effect, was discovered that can overcome this limitation by inverting the lowest-lying levels and creating a bright excitonic ground state. However, no methodology is available to systematically identify materials that exhibit this inversion, hindering the development of superbright nanocrystals and their devices. Here, based on a detailed understanding of the Rashba mechanism, we demonstrate a procedure that reveals previously unknown "bright-exciton" nanocrystals. We first define physical criteria to reduce over 500,000 known solids to 173 targets. Higher-level first-principles calculations then refine this list to 28 candidates. From these, we select five with high oscillator strength and develop effective-mass models to determine the nature of their lowest excitonic state. We confirm that four of the five solids yield bright ground-state excitons in nanocrystals. Thus, our results provide a badly needed roadmap for experimental investigation of bright-exciton nanomaterials.

8.
Article in English | MEDLINE | ID: mdl-39013007

ABSTRACT

In this study, we investigate the spin-momentum locking phenomenon on Rashba states of antimony (Sb) films. Utilizing spin pumping in conjunction with an external charge current, we uncover the topological properties of Sb surface states. Our key finding is the precise manipulation of the direction and magnitude of the charge current generated by the inverse Rashba-Edelstein effect. This control is achieved through the dynamic interaction between out-of-equilibrium pumped spins and spin-momentum-locked flowing spins, which are perpendicular to the charge current. Our results highlight Sb as a promising material for both fundamental and applied spintronics research. The studied Sb nanostructures demonstrate potential for the development of low-power logic gates operating with currents in the microampere range, paving the way for advanced spintronic applications.

9.
Small ; : e2402604, 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38898739

ABSTRACT

Dzyaloshinskii-Moriya interaction (DMI) is shown to induce a topologically protected chiral spin texture in magnetic/nonmagnetic heterostructures. In the context of van der Waals spintronic devices, graphene emerges as an excellent candidate material. However, due to its negligible spin-orbit interaction, inducing DMI to stabilize topological spins when coupled to 3d-ferromagnets remains challenging. Here, it is demonstrated that, despite these challenges, a sizeable Rashba-type spin splitting followed by significant DMI is induced in graphene/Fe3GeTe2. This is made possible due to an interfacial electric field driven by charge asymmetry together with the broken inversion symmetry of the heterostructure. These findings reveal that the enhanced DMI energy parameter, resulting from a large effective electron mass in Fe3GeTe2, remarkably contributes to stabilizing non-collinear spins below the Curie temperature, overcoming the magnetic anisotropy energy. These results are supported by the topological Hall effect, which coexists with the non-trivial breakdown of Fermi liquid behavior, confirming the interplay between spins and non-trivial topology. This work paves the way toward the design and control of interface-driven skyrmion-based devices.

10.
ACS Nano ; 18(26): 17218-17227, 2024 Jul 02.
Article in English | MEDLINE | ID: mdl-38904261

ABSTRACT

Lead halide perovskite quantum dots (QDs), the latest generation of the colloidal QD family, exhibit outstanding optical properties, which are now exploited as both classical and quantum light sources. Most of their rather exceptional properties are related to the peculiar exciton fine-structure of band-edge states, which can support unique bright triplet excitons. The degeneracy of the bright triplet excitons is lifted with energetic splitting in the order of millielectronvolts, which can be resolved by the photoluminescence (PL) measurements of single QDs at cryogenic temperatures. Each bright exciton fine-structure-state (FSS) exhibits a dominantly linear polarization, in line with several theoretical models based on the sole crystal field, exchange interaction, and shape anisotropy. Here, we show that in addition to a high degree of linear polarization, the individual exciton FSS can exhibit a non-negligible degree of circular polarization even without external magnetic fields by investigating the four Stokes parameters of the exciton fine-structure in individual CsPbBr3 QDs through Stokes polarimetric measurements. We observe a degree of circular polarization up to ∼38%, which could not be detected by using the conventional polarimetric technique. In addition, we found a consistent transition from left- to right-hand circular polarization within the fine-structure triplet manifold, which was observed in magnetic-field-dependent experiments. Our optical investigation provides deeper insights into the nature of the exciton fine structures and thereby drives the yet-incomplete understanding of the unique photophysical properties of this class of QDs for the benefit of future applications in chiral quantum optics.

11.
ACS Appl Mater Interfaces ; 16(24): 31247-31253, 2024 Jun 19.
Article in English | MEDLINE | ID: mdl-38844450

ABSTRACT

As Coulomb drag near charge neutrality (CN) is driven by fluctuations or inhomogeneity in charge density, the topology should play an extremely important role. Interlinking Coulomb drag and topology could reveal how the system's nontrivial topology influences the electron-electron interactions at the quantum level. However, such an aspect is overlooked as most studies focus on symmetric drag systems without topology. To understand this topological aspect, we need to study Coulomb drag in an asymmetric system with a broken inversion symmetry and strong spin-orbit coupling (SOC). Here we experimentally demonstrate the energy-driven Coulomb drag in an asymmetric van der Waals heterostructure composed of black phosphorus and rhenium disulfide characterized by broken inversion symmetry. Temperature-dependent transport measurements near CN provide compelling evidence for the energy-driven Coulomb drag due to electron-hole coupling that is energetically favored in a broken-gap heterojunction, as confirmed by Hall coefficient sign reversal with temperature. Moreover, contrary to the symmetric devices, our results exhibit magnetic-field-free, i.e., topology-driven, Hall drag, revealing an intrinsic coupling between energy and charge modes. This is the manifestation of nonzero Berry curvature, akin to a magnetic field in momentum space, in a Rashba system, which arises from the SOC and broken inversion symmetry of the heterostructure.

12.
Nano Lett ; 2024 Jun 06.
Article in English | MEDLINE | ID: mdl-38842923

ABSTRACT

Epitaxial heterostructures with topological insulators enable novel quantum phases and practical device applications. Their topological electronic states are sensitive to the microscopic parameters, including structural inversion asymmetry (SIA), which is an inherent feature of many real heterostructures. Controlling SIA is challenging, because it requires the ability to tune the displacement field across the topological film. Here, using nanopatterned gates, we demonstrate a tunable displacement field in a heterostructure of the two-dimensional topological insulator cadmium arsenide. Transport studies in magnetic fields reveal an extreme sensitivity of the band inversion to SIA. We show that a relatively small displacement field (∼50 mV/nm) converts the crossing of the two zeroth Landau levels in magnetic field to an avoided crossing, signaling a change to trivial band order. This work demonstrates a universal methodology for tuning electronic states in topological thin films.

13.
ACS Nano ; 18(24): 15716-15728, 2024 Jun 18.
Article in English | MEDLINE | ID: mdl-38847339

ABSTRACT

Epitaxial graphene/ferromagnetic metal (Gr/FM) heterostructures deposited onto heavy metals have been proposed for the realization of spintronic devices because of their perpendicular magnetic anisotropy and sizable Dzyaloshinskii-Moriya interaction (DMI), allowing for both enhanced thermal stability and stabilization of chiral spin textures. However, establishing routes toward this goal requires the fundamental understanding of the microscopic origin of their unusual properties. Here, we elucidate the nature of the induced spin-orbit coupling (SOC) at Gr/Co interfaces on Ir. Through spin- and angle-resolved photoemission spectroscopy along with density functional theory, we show that the interaction of the heavy metals with the Gr layer via hybridization with the FM is the source of strong SOC in the Gr layer. Furthermore, our studies on ultrathin Co films underneath Gr reveal an energy splitting of ∼100 meV for in-plane and negligible for out-of-plane spin polarized Gr π-bands, consistent with a Rashba-SOC at the Gr/Co interface, which is either the fingerprint or the origin of the DMI. This mechanism vanishes at large Co thicknesses, where neither in-plane nor out-of-plane spin-orbit splitting is observed, indicating that Gr π-states are electronically decoupled from the heavy metal. The present findings are important for future applications of Gr-based heterostructures in spintronic devices.

14.
J Phys Condens Matter ; 36(33)2024 May 23.
Article in English | MEDLINE | ID: mdl-38780062

ABSTRACT

Bloch oscillations (BOs) in Rashba systems, taking into account the effects of hexagonal warping and proximity-induced band gap, are reported. We find that in addition to real-space trajectories, the group and Berry velocities of Bloch electrons exhibit novel BOs which strongly depend on the crystal momentum. This oscillatory motion is affected significantly by variations in the strength of hexagonal warping and the proximity-induced band gap, originating from the substantial changes in the energy spectrum induced by these factors. In addition, it is shown that the Bloch oscillations are modified considerably under the influence of applied uniform in-plane electric and transverse magnetic fields, which allow for a geometric visualization of the Bloch dynamics. Interestingly, when the system is subjected to these fields simultaneously, it undergoes a dynamic phase transition between confined and de-confined states. This phase transition is tuned by the relative strength of the applied fields and is further influenced by variations in the strength of hexagonal warping and proximity-induced band gap. The appearance of such a transition is attributed to the interplay between the external fields and the intrinsic properties of the crystal lattice. Moreover, we find that the direct-current drift velocity shows negative differential conductivity, which is a characteristic feature of the BO regime.

15.
ACS Appl Mater Interfaces ; 16(20): 26915-26921, 2024 May 22.
Article in English | MEDLINE | ID: mdl-38717847

ABSTRACT

Multifunctional integration in a single device has always been a hot research topic, especially for contradictory phenomena, one of which is the coexistence of ferroelectricity and metallicity. The complex oxide heterostructures, as symmetric breaking systems, provide a great possibility to incorporate different properties. Moreover, finding a series of oxide heterostructures to achieve this goal remains as a challenge. Here, taking the advantage of different physical phenomena, we use H2 plasma to pretreat the SrTiO3 (STO) substrate and then fabricate HfO2/STO heterostructures with it. The novel, well-repeatable metallic two-dimensional electron gas (2DEG) is directly obtained at the heterointerfaces without any further complex procedures, while the obvious ferroelectric-like behavior and Rashba spin-orbit coupling are also observed. The understanding of the mechanism, as well as the modified facile preparation procedure, would be meaningful for further development of ferroelectric metal in complex oxide heterostructures.

16.
ACS Nano ; 18(21): 13506-13516, 2024 May 28.
Article in English | MEDLINE | ID: mdl-38748456

ABSTRACT

Spin-orbit torques (SOT) allow ultrafast, energy-efficient toggling of magnetization state by an in-plane charge current for applications such as magnetic random-access memory (SOT-MRAM). Tailoring the SOT vector comprising of antidamping (TAD) and fieldlike (TFL) torques could lead to faster, more reliable, and low-power SOT-MRAM. Here, we establish a method to quantify the longitudinal (TAD) and transverse (TFL) components of the SOT vector and its efficiency χAD and χFL, respectively, in nanoscale three-terminal SOT magnetic tunnel junctions (SOT-MTJ). Modulation of nucleation or switching field (BSF) for magnetization reversal by SOT effective fields (BSOT) leads to the modification of SOT-MTJ hysteresis loop behavior from which χAD and χFL are quantified. Surprisingly, in nanoscale W/CoFeB SOT-MTJ, we find χFL to be (i) twice as large as χAD and (ii) 6 times as large as χFL in micrometer-sized W/CoFeB Hall-bar devices. Our quantification is supported by micromagnetic and macrospin simulations which reproduce experimental SOT-MTJ Stoner-Wohlfarth astroid behavior only for χFL > χAD. Additionally, from the threshold current for current-induced magnetization switching with a transverse magnetic field, we show that in SOT-MTJ, TFL plays a more prominent role in magnetization dynamics than TAD. Due to SOT-MRAM geometry and nanodimensionality, the potential role of nonlocal spin Hall spin current accumulated adjacent to the SOT-MTJ in the mediation of TFL and χFL amplification merits to be explored.

17.
Nanomaterials (Basel) ; 14(8)2024 Apr 16.
Article in English | MEDLINE | ID: mdl-38668177

ABSTRACT

The Rashba effect appears in the semiconductors with an inversion-asymmetric structure and strong spin-orbit coupling, which splits the spin-degenerated band into two sub-bands with opposite spin states. The Rashba effect can not only be used to regulate carrier relaxations, thereby improving the performance of photoelectric devices, but also used to expand the applications of semiconductors in spintronics. In this mini-review, recent research progress on the Rashba effect of two-dimensional (2D) organic-inorganic hybrid perovskites is summarized. The origin and magnitude of Rashba spin splitting, layer-dependent Rashba band splitting of 2D perovskites, the Rashba effect in 2D perovskite quantum dots, a 2D/3D perovskite composite, and 2D-perovskites-based van der Waals heterostructures are discussed. Moreover, applications of the 2D Rashba effect in circularly polarized light detection are reviewed. Finally, future research to modulate the Rashba strength in 2D perovskites is prospected, which is conceived to promote the optoelectronic and spintronic applications of 2D perovskites.

18.
Materials (Basel) ; 17(8)2024 Apr 16.
Article in English | MEDLINE | ID: mdl-38673177

ABSTRACT

Lead halide perovskites (LHPs) containing organic parts are emerging optoelectronic materials with a wide range of applications thanks to their high optical absorption, carrier mobility, and easy preparation methods. They possess spin-dependent properties, such as strong spin-orbit coupling (SOC), and are promising for spintronics. The Rashba effect in LHPs can be manipulated by a magnetic field and a polarized light field. Considering the surfaces and interfaces of LHPs, light polarization-dependent optoelectronics of LHPs has attracted attention, especially in terms of spin-dependent photocurrents (SDPs). Currently, there are intense efforts being made in the identification and separation of SDPs and spin-to-charge interconversion in LHP. Here, we provide a comprehensive review of second-order nonlinear photocurrents in LHP in regard to spintronics. First, a detailed background on Rashba SOC and its related effects (including the inverse Rashba-Edelstein effect) is given. Subsequently, nonlinear photo-induced effects leading to SDPs are presented. Then, SDPs due to the photo-induced inverse spin Hall effect and the circular photogalvanic effect, together with photocurrent due to the photon drag effect, are compared. This is followed by the main focus of nonlinear photocurrents in LHPs containing organic parts, starting from fundamentals related to spin-dependent optoelectronics. Finally, we conclude with a brief summary and future prospects.

19.
J Phys Condens Matter ; 36(31)2024 May 08.
Article in English | MEDLINE | ID: mdl-38663418

ABSTRACT

Topological insulator (TI) surface states exert strong spin-orbit torques. When the magnetization is in the plane its interaction with the TI conduction electrons is non-trivial, and is influenced by extrinsic spin-orbit scattering. This is expected to be strong in TIs but is difficult to calculate and to measure unambiguously. Here we show that extrinsic spin-orbit scattering sizably renormalizes the surface state spin-orbit torque resulting in a strong density dependence. The magnitude of the renormalization of the spin torque and the effect of spin-orbit scattering on the relative sizes of the in-plane and out-of-plane field-like torques have strong implications for experiment: We propose two separate experimental signatures for the measurement of its presence.

20.
Nano Lett ; 24(10): 3089-3096, 2024 Mar 13.
Article in English | MEDLINE | ID: mdl-38426455

ABSTRACT

Exploration of two-dimensional (2D) sliding ferroelectric (FE) materials with experimentally detectable ferroelectricity and value-added novel functionalities is highly sought for the development of 2D "slidetronics". Herein, based on first-principles calculations, we identify the synthesizable van der Waals (vdW) layered crystals HgX2 (X = Br and I) as a new class of 2D sliding ferroelectrics. Both HgBr2 and HgI2 in 2D multilayered forms adopt the preferential stacking sequence, leading to room temperature stable out-of-plane (vertical) ferroelectricity that can be reversed via the sliding of adjacent monolayers. Owing to strong interlayer coupling and interfacial charge rearrangement, 2D HgI2 layers possess strong sliding ferroelectricity up to 0.16 µC/cm2, readily detectable in experiment. Moreover, robust sliding ferroelectricity and interlayer sliding controllable Rashba spin texture of FE-HgI2 layers enable potential applications as 2D spintronic devices such that the electric control of electron spin detection can be realized at the 2D regime.

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