Ionic Liquid Gating Research Articles

Electrically Tunable Nonlinearity at 3.2 Terahertz in Single-Layer Graphene.

Graphene is a nonlinear material in the terahertz (THz) frequency range, with χ(3) ∼ 10-9 m2/V2 ∼ 15 orders of magnitude higher than that of other materials used in the THz range, such as GaAs or lithium niobate. This nonlinear behavior, combined with ultrafast dynamic for excited carriers, proved to be essential for third harmonic generation in the sub-THz and low (<2.5 THz) THz range, using moderate (60 kV/cm) fields and at room temperature. Here, we show that, for monochromatic high peak power (1.8 W) input THz signals, emitted by a quantum cascade laser, the nonlinearity can be controlled using an ionic liquid gate that tunes the graphene Fermi energy up to >1.2 eV. Pump and probe experiments reveal an intense absorption nonlinearity at 3.2 THz, with a dominant 3rd-order contribution at EF > 0.7 eV, hence opening intriguing perspectives per engineering novel architectures for light generation at frequencies > 9 THz.

Mechanistic Insights into Synaptic Plasticity Behaviors of Electrolyte-Gated Flexible Transistor Devices.

Biological synaptic function simulation using flexible electronic devices based on low-dimensional semiconductor materials is an emerging and rapidly evolving research field with promising applications in brain-like computers and artificial intelligence systems. In this work, we present the fabrication of solution compatible MoS2 thin-film transistors on the ultrathin polymethyl methacrylate substrates via layer-by-layer assembly followed by a one-step transfer printing method. The MoS2 transport channel is controlled by ionic liquid gating with 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide, resulting in excellent synaptic performances for emulating memory and perception synapse functions. To investigate the synaptic behaviors, we conduct a series of synaptic spike-dependent experiments and propose an advanced model that delineates the long-term plasticity and short-term plasticity with separate characteristic factors. These findings provide insights into the fundamental mechanisms of synaptic plasticity in electric double-layer devices and contribute to a better understanding of their synaptic performances. In addition, we examine the effects of bending conditions on synaptic plasticity and synaptic weights, unveiling the synergistic interplay between mechanical deformation and synaptic behaviors. Our experimental results, combined with the developed model, are in good agreement and shed light on the influence of mechanical flexibility on the synaptic properties of the devices. In summary, this study establishes a solid foundation for further development of flexible synaptic devices from both practical and theoretical perspectives.

Electric Control of Helicity-Dependent Photocurrent and Surface Polarity Detection on Two-Dimensional Bi2O2Se Nanosheets.

Bismuth oxyselenide (Bi2O2Se) is a two-dimensional (2D) layered semiconductor material with high electron Hall mobility and excellent environmental stability as well as strong spin-orbit interaction (SOI), which has attracted intense attention for application in spintronic and spin optoelectronic devices. However, a comprehensive study of spin photocurrent and its microscopic origin in Bi2O2Se is still missing. Here, the helicity-dependent photocurrent (HDPC) was investigated in Bi2O2Se nanosheets. By analyzing the dependence of HDPC on the angle of incidence, we find that the HDPC originates from surface states with Cs symmetry in Bi2O2Se, which can be attributed to the circular photogalvanic effect (CPGE) and circular photon drag effect (CPDE). It is revealed that the HDPC current almost changes linearly with the source-drain voltage. Furthermore, we demonstrate effective tuning of HDPC in Bi2O2Se by ionic liquid gating, indicating that the spin splitting of the surface electronic structure is effectively tuned. By analyzing the gate voltage dependence of HDPC, we can unambiguously identify the surface polarity and the surface electronic structure of Bi2O2Se. The large HDPC in Bi2O2Se nanosheets and its efficient electrical tuning demonstrate that 2D Bi2O2Se nanosheets may provide a good platform for opto-spintronics devices.

Electric-field control of reversible electronic and magnetic transitions in two-dimensional oxide monolayer magnets

Atomically thin oxide magnetic materials are highly desirable due to the promising potential to integrate two-dimensional (2D) magnets into next-generation spintronics. Therefore, 2D oxide magnetism is expected to be effectively tuned by the magnetic and electrical fields, holding prospective for future low-dissipation electronic devices. However, the electric-field control of 2D oxide monolayer magnetism has rarely been reported. Here, we present the realization of 2D monolayer magnetism in oxide (SrRuO3)1/(SrTiO3)N (N = 1, 3) superlattices that shows an efficient and reversible phase transition through electric-field controlled proton (H+) evolution. By using ionic liquid gating to modulate the proton concentration in (SrRuO3)1/(SrTiO3)1 superlattice, an electric-field induced metal-insulator transition was observed, along with gradually suppressed magnetic ordering and modulated magnetic anisotropy. Theoretical analysis reveals that proton intercalation plays a crucial role in both electronic and magnetic phase transitions. Strikingly, SrTiO3 layers can act as a proton sieve, which have a significant influence on proton evolution. Our work stimulates the tuning functionality of 2D oxide monolayer magnetism by voltage control, providing potential for future energy-efficient electronics.

Control of Compensation Temperature in CoGd Films through Hydrogen and Oxygen Migration under Gate Voltage.

Electrical control of magnetic properties is crucial for low-energy memory and logic spintronic devices. We find that the magnetic properties of ferrimagnetic CoGd can be altered through ionic liquid gating. Gate voltages manipulate the opposite magnetic moments in Co and Gd sublattices and induce a giant magnetic compensation temperature change of more than 200 K in Pt/CoGd/Pt heterostructures. The electrically controlled dominant magnetic sublattice allows voltage-induced magnetization switching. Both experiments and theoretical calculations demonstrate that the significant modulations of compensation temperature are relevant to the reduced Gd moments due to the presence of hydrogen ions at positive voltages as well as the enhanced Co moments and reduced Gd moments due to the injection of oxygen ions at negative voltages. These findings expand the possibilities for all-electric and reversible magnetization control in the field of spintronics.

Optical grade bromide-based thin film electrolytes

Controlling the charge density in low-dimensional materials with an electrostatic potential is a powerful tool to explore and influence their electronic and optical properties. Conventional solid gates impose strict geometrical constraints to the devices and often absorb electromagnetic radiation in the infrared (IR) region. A powerful alternative is ionic liquid (IL) gating. This technique only needs a metallic electrode in contact with the IL, and the highest achievable electric field is limited by the electrochemical interactions of the IL with the environment. Despite the excellent gating properties, a large number of ILs are hardly exploitable for optical experiments in the mid-IR region because they typically suffer from low optical transparency and degradation in ambient conditions. Here, we report the realization of two electrolytes based on bromide ILs dissolved in polymethyl methacrylate (PMMA). We demonstrate that such electrolytes in the form of thin films can induce state-of-the-art charge densities as high as 20×1015 cm−2 with an electrochemical window of [−1V, 1V] in vacuum. Thanks to the low water absorption of PMMA, they work both in vacuum and in ambient atmosphere after a simple vacuum curing. Furthermore, our electrolytes can be spin-coated into flat thin films with optical transparency in the range from 600 to 4000 cm–1. Thanks to these properties, these electrolytes are excellent candidates to fill the gap as versatile gating layers for electronic and mid-IR optoelectronic devices.

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.

Reversible metal-insulator transition in SrIrO3 ultrathin layers by field effect control of inversion symmetry breaking

SrIrO3 is a correlated semimetal with narrow t2g d-bands of strong mixed orbital character resulting from the interplay of the spin-orbit interaction due to heavy iridium atoms and the band folding induced by the lattice structure. In ultrathin layers, inversion symmetry breaking, occurring naturally due to the presence of the substrate, opens new orbital hopping channels, which in presence of spin-orbit interaction causes deep modifications in the electronic structure. Here, we show that in SrIrO3 ultrathin films the effect of inversion symmetry breaking on the band structure can be externally manipulated in a field effect experiment. We further prove that the electric field toggles the system reversibly between a metallic and an insulating state with canted antiferromagnetism and an emergent anomalous Hall effect. This is achieved through the spin-orbit driven coupling of the electric field generated in an ionic liquid gate to the electronic structure, where the electric field controls the band structure rather than the usual band filling, thereby enabling electrical control of the effective role of electron correlations. The externally tunable antiferromagnetic insulator, rooted in the strong spin-orbit interaction of iridium, may inspire interesting applications in spintronics.

Self-Powered Phase Transition Driven by Triboelectric Nanogenerator

The phase transition of SrCoO2.5 (BM-SCO) is very popular in recent reports based on its special structure. The oxygen vacancy channel of BM-SCO provides a convenient condition for phase transformation to SrCoO3-δ (PV-SCO), with prospects in smart windows, memristive devices, and magnetic recording. The traditional method for phase transition is thermal annealing, while the electric-field-controlled ionic liquid (IL) gating is also a convenient method. Herein, we use a triboelectric nanogenerator as a self-powered system, which can provide a constant voltage for the IL and achieve ion injection to induce phase transition, and this procedure proved to be reversible. X-ray diffraction scanning and high-resolution transmission electron microscope observation showed that the crystal structures of the two phases are significantly different. Besides, BM-SCO is antiferromagnetic, PV-SCO is ferromagnetic, and the optical transmittance also changes during the phase transition. As for the applications of this film, we used IL gating to modulate the resistive switching behavior, which shows a change between high-resistance state and low-resistance state during the phase transition and can be used in resistive random access memory devices.

Electrical Manipulation of Orbital Current Via Oxygen Migration in Ni81 fe19 /Cuox /Tan Heterostructure.

The orbital Hall effect and the interfacial Rashba effect provide new approaches to generate orbital current and spin-orbit torque (SOT) efficiently without the use of heavy metals. However, achieving efficient dynamic control of orbital current and SOT in light metal oxides has proven challenging. In this study, we demonstrate that a sizable magnetoresistance effect related to orbital current and SOT can be observed in Ni81 Fe19 /CuOx /TaN heterostructures with various CuOx oxidisation concentrations. The ionic liquid gating induces migration of oxygen ions, which modulates the oxygen concentration at the Ni81 Fe19 /CuOx interface, leading to reversible manipulation of the magnetoresistance effect and SOT. The existence of a thick TaN capping layer allows for sophisticated internal oxygen ion reconstruction in the CuOx layer, rather than conventional external ion exchange. These results provide a method for the reversible and dynamic manipulation of the orbital current and SOT generation efficiency, thereby advancing the development of spin-orbitronics devices through ionic engineering. This article is protected by copyright. All rights reserved.

Tunable resonance Raman scattering of quantum dots in a nonlinear excitation regime.

Controllable tuning of electron-phonon coupling strength and excited state dynamics is important for the understanding of resonance Raman scattering in low-dimensional semiconductors. Here, we report a significant and reversible field-induced modulation in absolute resonance Raman intensity of quantum dots using ionic liquid gating. Meanwhile, a potential-dependent nonlinear relationship is present between Raman intensity and excitation power density. By exploring the parameter space within a time domain model, we find that the Raman intensity variation is mainly determined by the homogeneous linewidth. We further propose that the Fermi level positions and exciton species play key roles in the excited state decay rates.

Electrochemical thinning of Co kagome-lattice layers in ferromagnetic Co3Sn2S2 thin films by bias-induced Co dissolution

Solid–liquid interfaces made of functional inorganic materials and liquid electrolytes exhibit various interesting responses by applying an electric bias across the interface. Using an electric-double-layer device fabricated on a thin-film channel of magnetic Weyl semimetal Co3Sn2S2 with an ionic liquid gate electrolyte, we show that the conducting channel thickness can be effectively decreased by applying a negative gate voltage. The application of a gate voltage of −6 V at 250 K gives rise to an irreversible increase in the channel resistance. Transmission electron microscopy reveals that the thickness of the crystallized Co3Sn2S2 region is decreased by applying the negative bias, leaving a Co-poor disordered region on top of the Co3Sn2S2 layer. These results suggest that the preferential dissolution of Co is driven under the application of the negative bias, which leads to the disconnection of Co kagome-lattice layer that is mainly responsible for electrical conduction in Co3Sn2S2. Distinct from conventional bottom-up film growth approaches, this top-down thickness control enables us to examine the thickness dependence of the anomalous transport properties of Co3Sn2S2 in a single sample. The present finding will be useful for experimentally verifying the theoretically discussed ultrathin-film properties of the magnetic Weyl semimetal Co3Sn2S2.

In situ electrical and thermal transport properties of FeySe1−xTex films with ionic liquid gating

We combine in-situ electrical transport and Seebeck coefficient measurements with the ionic liquid gating technique to investigate superconductivity and the normal state of FeySe1-xTex (FST) films. We find that the pristine FST films feature a non-Fermi liquid temperature dependence of the Seebeck coefficient, i.e., S/T ~ AS lnT, and AS is strongly correlated with the superconducting transition temperature (Tc). Ionic liquid gating significantly raises Tc of FST films, for which the Seebeck coefficient displays a novel scaling behavior and retains the logarithmic temperature dependence. Moreover, a quantitative relationship between the slope of T-linear resistivity (A\r{ho}) and Tc for gated films is observed, i.e., (A\r{ho})1/2 ~ Tc, consistent with previous reports on cuprates and FeSe. The scaling behaviors of AS and A\r{ho} point to a spin-fluctuation-associated transport mechanism in gated FeySe1-xTex superconductors.

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.

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.

A novel CVD graphene-based synaptic transistors with ionic liquid gate

The synaptic devices based on various electronic materials have been widely investigated to realize functions of artificial information processing with low power consumption. In this work, a novel CVD graphene field-effect transistor is fabricated with ionic liquid gate to study the synaptic behaviors based on the electrical-double-layer mechanism. It is found that the excitative current is enhanced with the pulse width, voltage amplitude and frequency. With different situations of the applied pulse voltage, the inhibitory and excitatory behaviors are successfully simulated, at the same time the short-term memory is also realized. The corresponding ions migration and charge density variation are analyzed in the different time segments. This work provides the guidance for the design of artificial synaptic electronics with ionic liquid gate for low-power computing application.

Electromagnetic evolution in proton-containing spinel NiCo2O4 thin films via ionic liquid gating

Proton incorporation through ionic liquid gating (ILG) has become an efficient strategy to manipulate the novel ground-state properties in complex oxides. However, the mechanisms of proton evolution and their correlations with other degrees of freedom in quantum material systems are still unclear. Herein, we provide insights into the correlated interactions among different lattice-spin-orbital-spin degrees of freedom in spinel ${\mathrm{NiCo}}_{2}{\mathrm{O}}_{4}$ (NCO) films with a complex local electronic configuration and coordination environments. Our results reveal that the Ni ions near the Fermi level show the prior ${\mathrm{Ni}}^{3+}\ensuremath{\rightarrow}{\mathrm{Ni}}^{2+}$ response, whereas the Co ions at different octahedral and tetrahedral sites exhibit a stepwise ${\mathrm{Co}}^{3+}\ensuremath{\rightarrow}{\mathrm{Co}}^{2+}$ evolution. The gradual evolutions reflected in both structure and electronic configuration aspects determine the different electronic conducting mechanisms as well as the variation of the magnetic ground states in the protonated NCO films. Our systematic structure-property investigations shed light on the fundamental understanding of the strongly correlated nature in quantum materials and the manipulation of quantum materials with desired functionalities through the ILG approach.

Hysteresis and training effect in the electric control of spin current in Pt/Y3Fe5O12 heterostructures

We have reported on the hysteresis and training effect of spin current in $\mathrm{Pt}/{\mathrm{Y}}_{3}{\mathrm{Fe}}_{5}{\mathrm{O}}_{12}$ heterostructures during subsequent cycles of ionic liquid gate voltage ${V}_{g}$. The inverse spin Hall effect voltage in spin pumping and spin Hall magnetoresistance exhibit diode-like behaviors in the first half cycle of ${V}_{g}$ and also show hysteresis in the first cycle of ${V}_{g}$. Both the diode-like behavior and the hysteresis become weak and even vanish in the second cycle of ${V}_{g}$ due to the training effect. The above experimental results can be well explained by the screening charge doping model, in which the charge and the local magnetic moment are asymmetrically distributed in the Pt layer. The applicability of this model is further confirmed by measurements of anisotropic magnetoresistance and ferromagnetic resonance. The diode-like behavior is attributed to interplay between the asymmetrically distributed local magnetic moment and the spin current relaxation in the Pt layer. The hysteresis and the training effect arise from the incompletely reversible process between oxidation and reduction of Pt atoms and the evolution of the surface morphology at the ionic liquid/Pt interface under electric gating. This work provides new insights to improve the functional performance of electrically controlled spin current devices.

Enhanced Magnetization in CoFe2O4 Through Hydrogen Doping

AbstractMagnetic spinel oxides have attracted extensive research interest due to their rich physics and wide range of applications. However, these materials invariably suffer suppressed magnetization, due to structural imperfections (e.g., disorder, anti‐site defects, etc.). Herein, a dramatic enhanced magnetization is obtained with an increasement of 5 µB/u.c in CoFe2O4 (CFO) through ionic liquid gating induced hydrogen doping. The intercalated hydrogen ions lead to both distinct lattice expansion of ≈0.7% and notable Fe valence state reduction through electron doping, in which ≈17% Fe3+ is reduced into Fe2+. These facts collectively trigger a site‐specific spin‐flip on tetrahedrally coordinated Co2+ sites that enhances the net ferrimagnetic moment nearly to its theoretical maximum for perfect CFO.

Junctionless Electric-Double-Layer MoS2 Field-Effect Transistor with a Sub-5 nm Thick Electrostatically Highly Doped Channel.

Junctionless transistors are suitable for sub-3 nm applications because of their extremely simple structure and high electrical performance, which compensate for short-channel effects. Two-dimensional semiconductor transition-metal dichalcogenide materials, such as MoS2, may also resolve technical and fundamental issues for Si-based technology. Here, we present the first junctionless electric-double-layer field-effect transistor with an electrostatically highly doped 5 nm thick MoS2 channel. A double-gated MoS2 transistor with an ionic-liquid top gate and a conventional bottom gate demonstrated good transfer characteristics with a 104 on-off current ratio, a 70 mV dec-1 subthreshold swing at a 0 V bottom-gate bias, and drain-current versus top-gate-voltage characteristics were shifted left significantly with increasing bottom-gate bias due to an electrostatically increased overall charge carrier concentration in the MoS2 channel. When a bottom-gate bias of 80 V was applied, a shoulder and two clear peak features were identified in the transconductance and its derivative, respectively; this outcome is typical of Si-based junctionless transistors. Furthermore, the decrease in electron mobility induced by a transverse electric field was reduced with increasing bottom-gate bias. Numerical simulations and analytical models were used to support these findings, which clarify the operation of junctionless MoS2 transistors with an electrostatically highly doped channel.