Manipulation of Helicity-Dependent Photocurrent and Stokes Parameter Detection in Topological Insulator Bi2Te3 Nanowires.

Helicity-dependent photocurrent (HDPC) and its modulation in topological insulator Bi2Te3 nanowires have been investigated. It is revealed that when the incident plane of a laser is perpendicular to the nanowire, the HDPC is an odd function of the incident angle, which is mainly contributed by the circular photogalvanic effect originating from the surface states of Bi2Te3 nanowire. When the incident plane of a laser is parallel to the nanowire, the HDPC is approximately an even function of the incident angle, which is due to the circular photon drag effect coming from the surface states. It is found that the HDPC can be effectively tuned by the back gate and the ionic liquid top gate. By analyzing the substrate dependence of the HDPC, we find that the HDPC of the Bi2Te3 nanowire on the Si substrate is an order of magnitude larger than that on SiO2, which may be due to the spin injection from the Si substrate to the Bi2Te3 nanowire. In addition, by applying different biases, the Stokes parameters of a polarized light can be extracted by arithmetic operation of the photocurrents measured in the Bi2Te3 nanowire. This work suggests that topological insulator Bi2Te3 nanowires may provide a good platform for opto-spintronic devices, especially in chirality and polarimtry detection.

Ferromagnetic Insulating Ground-State Resolved in Mixed Protons and Oxygen Vacancies-Doped La0.67Sr0.33CoO3 Thin Films via Ionic Liquid Gating.

The realization of ferromagnetic insulating ground state is a critical prerequisite for spintronic applications. By applying electric field-controlled ionic liquid gating (ILG) to stoichiometry La0.67Sr0.33CoO3 thin films, the doping of protons (H+) has been achieved for the first time. Furthermore, a hitherto-unreported ferromagnetic insulating phase with a remarkably high Tc up to 180 K has been observed which can be attributed to the doping of H+ and the formation of oxygen vacancies (VO). The chemical formula of the dual-ion migrated film has been identified as La2/3Sr1/3CoO8/3H2/3 based on combined Co L23-edge absorption spectra and configuration interaction cluster calculations, from which we are able to explain the ferromagnetic ground state in terms of the distinct magnetic moment contributions from Co ions with octahedral (Oh) and tetrahedral (Td) symmetries following antiparallel spin alignments. Further density functional theory calculations have been performed to verify the functionality of H+ as the transfer ion and the origin of the novel ferromagnetic insulating ground state. Our results provide a fundamental understanding of the ILG regulation mechanism and shed light on the manipulating of more functionalities in other correlated compounds through dual-ion manipulation.

Hundred-Fold Enhancement in the Anomalous Hall Effect Induced by Hydrogenation.

The anomalous Hall effect (AHE) is one of the most fascinating transport properties in condensed matter physics. However, the AHE magnitude, which mainly depends on net spin polarization and band topology, is generally small in oxides and thus limits potential applications. Here, we demonstrate a giant enhancement of AHE in a LaCoO3-induced 5d itinerant ferromagnet SrIrO3 by hydrogenation. The anomalous Hall resistivity and anomalous Hall angle, which are two of the most critical parameters in AHE-based devices, are found to increase to 62.2 µΩ·cm and 3%, respectively, showing an unprecedentedly large enhancement ratio of ∼10000%. Theoretical analysis suggests the key roles of Berry curvature in enhancing AHE. Furthermore, the hydrogenation concomitantly induces the significant elevation of Curie temperature from 75 to 160 K and 40-fold reinforcement of coercivity. Such giant regulation and very large AHE magnitude observed in SrIrO3 could pave the path for 5d oxide devices.

Protonation-Induced Colossal Lattice Expansion in La2/3Sr1/3MnO3.

Ion injection controlled by an electric field is a powerful method to manipulate the diverse physical and chemical properties of metal oxides. However, the dynamic control of ion concentrations and their correlations with lattices in perovskite systems have not been fully understood. In this study, we systematically demonstrate the electric-field-controlled protonation of La2/3Sr1/3MnO3 (LSMO) films. The rapid and room-temperature protonation induces a colossal lattice expansion of 9.35% in tensile-strained LSMO, which is crucial for tailoring material properties and enabling a wide range of applications in advanced electronics, energy storage, and sensing technologies. This large expansion in the lattice is attributed to the higher degree of proton diffusion, resulting in a significant elongation in the Mn-O bond and octahedral tilting, which is supported by results from density functional theory calculations. Interestingly, such a colossal expansion is not observed in LSMO under compressive strain, indicating the close dependence of ion-electron-lattice coupling on strain states. These efficient modulations of the lattice and magnetoelectric functionalities of LSMO via proton diffusion offer a promising avenue for developing multifunctional iontronic devices.

Formation of Highly Conductive Interfaces in Crystalline Ionic Liquid-Gated Unipolar MoTe2/h-BN Field-Effect Transistor.

2H MoTe2 (molybdenum ditelluride) has generated significant interest because of its superconducting, nonvolatile memory, and semiconducting of new materials, and it has a large range of electrical properties. The combination of transition metal dichalcogenides (TMDCs) and two dimensional (2D) materials like hexagonal boron nitride (h-BN) in lateral heterostructures offers a unique platform for designing and engineering novel electronic devices. We report the fabrication of highly conductive interfaces in crystalline ionic liquid-gated (ILG) field-effect transistors (FETs) consisting of a few layers of MoTe2/h-BN heterojunctions. In our initial exploration of tellurium-based semiconducting TMDs, we directed our attention to MoTe2 crystals with thicknesses exceeding 12 nm. Our primary focus centered on investigating the transport characteristics and quantitatively assessing the surface interface heterostructure. Our transconductance (gm) measurements indicate that the very efficient carrier modulation with an ILG FET is two times larger than standard back gating, and it demonstrates unipolarity of the device. The ILG FET exhibited highly unipolar p-type behavior with a high on/off ratio, and it significantly increased the mobility in MoTe2/h-BN heterochannels, achieving improvement as one of the highest recorded mobility increments. Specifically, we observed hole and electron mobility values ranging from 345 cm2 V-1 s-1 to 285 cm2 V-1 s-1 at 80 K. We predict that our ability to observe the intrinsic, heterointerface conduction in the channels was due to a drastic reduction of the Schottky barriers, and electrostatic gating is suggested as a method for controlling the phase transitions in the few layers of TMDC FETs. Moreover, the simultaneous structural phase transitions throughout the sample, achieved through electrostatic doping control, presents new opportunities for developing phase change devices using atomically thin membranes.

Electrical Control of Spin Hall Efficiency and Field-Free Magnetization Switching in W/Pt/Co/Pt Heterostructures with Competing Spin Currents.

Reversal of magnetization via current-induced spin-orbit torque (SOT) is one of the core issues in spintronics. However, an in-plane assistant field is usually required for the deterministic switching of a perpendicularly magnetized system. Additionally, the efficiency of SOT is low, which is detrimental to device applications. This study achieved a reversible and non-volatile control of the critical current for magnetization switching and spin Hall efficiency in the TaN/W/Pt/Co/Pt/TaN heterostructures by ionic liquid (IL) gating-induced hydrogen ion adsorption and desorption in the upper Pt layer. Furthermore, the thinning of the Pt and TaN capping layers activated the oxygen ion migration toward the Co layer under IL gating, resulting in an exchange bias field and allowing field-free magnetization switching and Boolean logic operation. The results of this study offer an intriguing opportunity to promote the development of SOT-based spintronic devices from the perspective of iontronics with low energy dissipation.

Strain-driven formation of epitaxial nanostructures in brownmillerite strontium cobaltite thin films.

Nanostructured materials can display unique physical properties and are of particular interest for their new functionalities. Epitaxial growth is a promising approach for the controlled synthesis of nanostructures with desired structures and crystallinity. SrCoOx is a particularly intriguing material owing to a topotactic phase transition between an antiferromagnetic insulating brownmillerite SrCoO2.5 (BM-SCO) phase and a ferromagnetic metallic perovskite SrCoO3-δ (P-SCO) phase depending on the oxygen concentration. Here, we present the formation and control of epitaxial BM-SCO nanostructures by substrate-induced anisotropic strain. Perovskite substrates with a (110)-orientation and which allow for compressive strain result in the creation of BM-SCO nanobars, while (111)-oriented substrates give rise to the formation of BM-SCO nanoislands. We have found that substrate-induced anisotropic strain coupled with the orientation of crystalline domains determines the shape and facet of the nanostructures, while their size can be tuned by the degree of strain. Moreover, the nanostructures can be transformed between antiferromagnetic BM-SCO and ferromagnetic P-SCO via ionic liquid gating. Thus, this study provides insights into the design of epitaxial nanostructures whose structure and physical properties can be readily controlled.

Electric Control of 2D Van Hove Singularity in Oxide Ultra-Thin Films.

Divergent density of states (DOS) can induce extraordinary phenomena such as significant enhancement of superconductivity and unexpected phase transitions. Moreover, van Hove singularities (VHSs) lead to divergent DOS in 2D systems. Despite recent interest in VHSs, only a few controllable cases have been reported to date. In this work, by utilizing an atomically ultra-thin SrRuO3 film, the electronic structure of a 2D VHS is investigated with angle-resolved photoemission spectroscopy and transport properties are controlled. By applying electric fields with alkali metal deposition and ionic-liquid gating methods, the 2D VHS and the sign of the charge carrier are precisely controlled. Use of a tunable 2D VHS in an atomically flat oxide film could serve as a new strategy to realize infinite DOS near the Fermi level, thereby allowing efficient tuning of electric properties.

Emergent quantum phenomena in atomically engineered iridate heterostructures.

Over the last few years, researches in iridates have developed into an exciting field with the discovery of numerous emergent phenomena, interesting physics, and intriguing functionalities. Among the studies, iridate-based artificial structures play a crucial role owing to their extreme flexibility and tunability in lattice symmetry, chemical composition, and crystal dimensionality. In this article, we present an overview of the recent progress regarding iridate-based artificial structures. We first explicitly introduce several essential concepts in iridates. Then, we illustrate important findings on representative SrIrO3/SrTiO3 superlattices, heterostructures comprised of SrIrO3 and magnetic oxides, and their response to external electric-field stimuli. Finally, we comment on existing problems and promising future directions in this exciting field.

Nonvolatile n-Type Doping and Metallic State in Multilayer-MoS2 Induced by Hydrogenation Using Ionic-Liquid Gating.

Manipulation of the carrier density of layered transition-metal dichalcogenides (TMDs) is of fundamental significance for a wide range of electronic and optoelectronic applications. Herein, we applied the ionic-liquid-gating (ILG) method to inject the smallest ions, H+, into layered MoS2 to manipulate its carrier concentration. The measurements demonstrate that the injection of H+ realizes a nonvolatile n-type doping and metallic state in multilayer-MoS2 with a concentration of injection electron of ∼1.08 × 1013 cm-2 but has no effect on monolayer-MoS2, which clearly reveals that the H+ is injected into the interlayer of MoS2, not in the crystal lattice. The H+-injected multilayer-MoS2 was then used as the contact electrodes of a monolayer-MoS2 field effect transistor to improve the contact quality, and its performance has been enhanced. Our work deepens the understanding of the ILG technology and extends its application in TMDs.

Indirect Band Gap in Scrolled MoS2 Monolayers.

MoS2 nanoscrolls that have inner core radii of ∼250 nm are generated from MoS2 monolayers, and the optical and transport band gaps of the nanoscrolls are investigated. Photoluminescence spectroscopy reveals that a MoS2 monolayer, originally a direct gap semiconductor (∼1.85 eV (optical)), changes into an indirect gap semiconductor (∼1.6 eV) upon scrolling. The size of the indirect gap for the MoS2 nanoscroll is larger than that of a MoS2 bilayer (∼1.54 eV), implying a weaker interlayer interaction between concentric layers of the MoS2 nanoscroll compared to Bernal-stacked MoS2 few-layers. Transport measurements on MoS2 nanoscrolls incorporated into ambipolar ionic-liquid-gated transistors yielded a band gap of ∼1.9 eV. The difference between the transport and optical gaps indicates an exciton binding energy of 0.3 eV for the MoS2 nanoscrolls. The rolling up of 2D atomic layers into nanoscrolls introduces a new type of quasi-1D nanostructure and provides another way to modify the band gap of 2D materials.

Electric-Field Control of Spin Diffusion Length and Electric-Assisted D'yakonov-Perel' Mechanism in Ultrathin Heavy Metal and Ferromagnetic Insulator Heterostructure.

Electric-field control of spin dynamics is significant for spintronic device applications. Thus far, effectively electric-field control of magnetic order, magnetic damping factor and spin-orbit torque (SOT) has been studied in magnetic materials, but the electric field control of spin relaxation still remains unexplored. Here, we use ionic liquid gating to control spin-related property in the ultra-thin (4 nm) heavy metal (HM) platinum (Pt) and ferromagnetic insulator (FMI) yttrium iron garnet (Y3Fe5O12, YIG) heterostructure. It is found that the anomalous Hall effect (AHE), spin relaxation time and spin diffusion length can be effectively controlled by the electric field. The anomalous Hall resistance is almost twice as large as at 0 voltage after applying a small voltage of 5.5 V. The spin relaxation time can vary by more than 50 percent with the electric field, from 41.6 to 64.5 fs. In addition, spin relaxation time at different gate voltage follows the reciprocal law of the electron momentum scattering time, which indicates that the D'yakonov-Perel' mechanism is dominant in the Pt/YIG system. Furthermore, the spin diffusion length can be effectively controlled by an ionic gate, which can be well explained by voltage-modulated interfacial spin scattering. These results help us to improve the interface spin transport properties in magnetic materials, with great contributions to the exploration of new physical mechanisms and spintronics device.

Electrical Control of Spin Hall Effect in Pt by Hydrogen Ion Adsorption and Desorption.

The manipulation of charge-to-spin current conversion and spin-orbit torque (SOT) is of great interest due to its profound physics and potential applications. Controlling the spin current through the electric field provides a perspective for highly efficient SOT devices. Here, we use H2O-doped ionic liquid gating to realize the reversible and nonvolatile manipulation of the spin Hall effect of Pt, and the spin Hall angle can be modulated by 48% within an accessible gate voltage range. The increase in the spin Hall angle is demonstrated to be caused by the adsorption of hydrogen ions on the Pt surface and the consequent enhancement of the spin Hall conductivity under positive voltage. Furthermore, the enhancement of the spin Hall angle is beneficial to reduce the critical current density for driving the domain wall motion. These results supply a method for the dynamic control of the charge-to-spin current conversion, which will promote the development of spintronic devices driven by electric fields.

Multivalley Superconductivity in Monolayer Transition Metal Dichalcogenides.

In transition metal dichalcogenides (TMDs), Ising superconductivity with an antisymmetric spin texture on the Fermi surface has attracted wide interest due to the exotic pairing and topological properties. However, it is not clear whether the Q valley with a giant spin splitting is involved in the superconductivity of heavily doped semiconducting 2H-TMDs. Here by taking advantage of a high-quality monolayer WS2 on hexagonal boron nitride flakes, we report an ionic-gating induced superconducting dome with a record high critical temperature of ∼6 K, accompanied by an emergent nonlinear Hall effect. The nonlinearity indicates the development of an additional high-mobility channel, which (corroborated by first principle calculations) can be ascribed to the population of Q valleys. Thus, multivalley population at K and Q is suggested to be a prerequisite for developing superconductivity. The involvement of Q valleys also provides insights to the spin textured Fermi surface of Ising superconductivity in the large family of transition metal dichalcogenides.

Protonation enhanced superconductivity in PdTe2.

Electrochemical ionic liquid gating is an effective way to intercalate ions into layered materials and modulate the properties. Here we report an enhanced superconductivity in a topological superconductor candidate PdTe2through electrochemical gating procedure. The superconducting transition temperature was increased to approximately 3.2 K by ionic gating induced protonation at room temperature. Moreover, a further enhanced superconductivity of both superconducting transition temperature and superconducting volume fraction was observed after the gated samples were placed in a glove box for 2 months. This may be caused by the diffusion of protons in the gated single crystals, which is rarely reported in electrochemical ionic liquid gating experiments. Our results further the superconducting study of PdTe2and may reveal a common phenomenon in the electrochemical gating procedure.

Ionic Liquid Gating of SrTiO3 Lamellas Fabricated with a Focused Ion Beam.

In this work, we combine two previously incompatible techniques for defining electronic devices: shaping three-dimensional crystals by focused ion beam (FIB), and two-dimensional electrostatic accumulation of charge carriers. The principal challenge for this integration is nanometer-scale surface damage inherent to any FIB-based fabrication. We address this by using a sacrificial protective layer to preserve a selected pristine surface. The test case presented here is accumulation of 2D carriers by ionic liquid gating at the surface of a micron-scale SrTiO3 lamella. Preservation of surface quality is reflected in superconductivity of the accumulated carriers. This technique opens new avenues for realizing electrostatic charge tuning in materials that are not available as large or exfoliatable single crystals, and for patterning the geometry of the accumulated carriers.

Chemical Potential Switching of the Anomalous Hall Effect in an Ultrathin Noncollinear Antiferromagnetic Metal.

The discovery of the anomalous Hall effect in noncollinear antiferromagnetic metals represents one of the most important breakthroughs for the emergent antiferromagnetic spintronics. The tuning of chemical potential has been an important theoretical approach to varying the anomalous Hall conductivity, but the direct experimental demonstration has been challenging owing to the large carrier density of metals. In this work, an ultrathin noncollinear antiferromagnetic Mn3 Ge film is fabricated and its carrier density is modulated by ionic liquid gating. Via a small voltage of ≈3 V, its carrier density is altered by ≈90% and, accordingly, the anomalous Hall effect is completely switched off. This work thus creates an attractive new way to steering the anomalous Hall effect in noncollinear antiferromagnets.

Control of Oxygen Vacancy Ordering in Brownmillerite Thin Films via Ionic Liquid Gating.

Oxygen defects and their atomic arrangements play a significant role in the physical properties of many transition metal oxides. The exemplary perovskite SrCoO3-δ (P-SCO) is metallic and ferromagnetic. However, its daughter phase, the brownmillerite SrCoO2.5 (BM-SCO), is insulating and an antiferromagnet. Moreover, BM-SCO exhibits oxygen vacancy channels (OVCs) that in thin films can be oriented either horizontally (H-SCO) or vertically (V-SCO) to the film's surface. To date, the orientation of these OVCs has been manipulated by control of the thin film deposition parameters or by using a substrate-induced strain. Here, we present a method to electrically control the OVC ordering in thin layers via ionic liquid gating (ILG). We show that H-SCO (antiferromagnetic insulator, AFI) can be converted to P-SCO (ferromagnetic metal, FM) and subsequently to V-SCO (AFI) by the insertion and subtraction of oxygen throughout thick films via ILG. Moreover, these processes are independent of substrate-induced strain which favors formation of H-SCO in the as-deposited film. The electric-field control of the OVC channels is a path toward the creation of oxitronic devices.

Ionic-Liquid Gating in Two-Dimensional TMDs: The Operation Principles and Spectroscopic Capabilities.

Ionic-liquid gating (ILG) is able to enhance carrier densities well above the achievable values in traditional field-effect transistors (FETs), revealing it to be a promising technique for exploring the electronic phases of materials in extreme doping regimes. Due to their chemical stability, transition metal dichalcogenides (TMDs) are ideal candidates to produce ionic-liquid-gated FETs. Furthermore, as recently discovered, ILG can be used to obtain the band gap of two-dimensional semiconductors directly from the simple transfer characteristics. In this work, we present an overview of the operation principles of ionic liquid gating in TMD-based transistors, establishing the importance of the reference voltage to obtain hysteresis-free transfer characteristics, and hence, precisely determine the band gap. We produced ILG-based bilayer WSe2 FETs and demonstrated their ambipolar behavior. We estimated the band gap directly from the transfer characteristics, demonstrating the potential of ILG as a spectroscopy technique.

Light Controllable Electronic Phase Transition in Ionic Liquid Gated Monolayer Transition Metal Dichalcogenides.

Ionic liquid gating has proved to be effective in inducing emergent quantum phenomena such as superconductivity, ferromagnetism, and topological states. The electrostatic doping at two-dimensional interfaces relies on ionic motion, which thus is operated at sufficiently high temperature. Here, we report the in situ tuning of quantum phases by shining light on an ionic liquid-gated interface at cryogenic temperatures. The light illumination enables flexible switching of the quantum transition in monolayer WS2 from an insulator to a superconductor. In contrast to the prevailing picture of photoinduced carriers, we find that in the presence of a strong interfacial electric field conducting electrons could escape from the surface confinement by absorbing photons, mimicking the field emission. Such an optical tuning tool in conjunction with ionic liquid gating greatly facilitates continuous modulation of carrier densities and hence electronic phases, which would help to unveil novel quantum phenomena and device functionality in various materials.