Electrostatic Gating Research Articles

Renewable Energy from Livestock Waste Valorization: Amyloid-Based Feather Keratin Fuel Cells.

Increasing carbon emissions have accelerated climate change, resulting in devastating effects that are now tangible on an everyday basis. This is mirrored by a projected increase in global energy demand of approximately 50% within a single generation, urging a shift from fossil-fuel-derived materials toward greener materials and more sustainable manufacturing processes. Biobased industrial byproducts, such as side streams from the food industry, are attractive alternatives with strong potential for valorization due to their large volume, low cost, renewability, biodegradability, and intrinsic material properties. Here, we demonstrate the reutilization of industrial chicken feather waste into proton-conductive membranes for fuel cells, protonic transistors, and water-splitting devices. Keratin was isolated from chicken feathers via a fast and economical process, converted into amyloid fibrils through heat treatment, and further processed into membranes with an imparted proton conductivity of 6.3 mS cm-1 using a simple oxidative method. The functionality of the membranes is demonstrated by assembling them into a hydrogen fuel cell capable of generating 25 mW cm-2 of power density to operate various types of devices using hydrogen and air as fuel. Additionally, these membranes were used to generate hydrogen through water splitting and in protonic field-effect transistors as thin-film modulators of protonic conductivity via the electrostatic gating effect. We believe that by converting industrial waste into renewable energy materials at low cost and high scalability, our green manufacturing process can contribute to a fully circular economy with a neutral carbon footprint.

Magneto-ionic and electrostatic gating of magnetism: Phenomena and devices

Magneto-ionic and electrostatic gating of magnetism: Phenomena and devices

Revealing flat bands and hybridization gaps in a twisted bilayer graphene device with microARPES

Controlling the electronic structure of two-dimensional materials using the combination of twist angle and electrostatic doping is an effective means to induce emergent phenomena. In bilayer graphene with an interlayer twist angle near the magic angle, the electronic dispersion is strongly modified by a manifold of hybridizing moiré Dirac cones leading to flat band segments with strong electronic correlations. Numerous technical challenges arising from spatial inhomogeneity of interlayer interactions, twist angle and device functionality have so far limited momentum-resolved electronic structure measurements of these systems to static conditions. Here, we present a detailed characterization of the electronic structure exhibiting miniband dispersions for twisted bilayer graphene, near the magic angle, integrated in a functional device architecture using micro-focused angle-resolved photoemission spectroscopy. The optimum conditions for visualizing the miniband dispersion are determined by exploiting the spatial resolution and photon energy tunability of the light source and applied to extract a hybridization gap size of eV and flat band segments extending across a moiré mini Brillouin zone. In situ electrostatic gating of the sample enables significant electron-doping, causing the conduction band states to shift below the Fermi energy. Our work emphasizes key challenges in probing the electronic structure of magic angle bilayer graphene devices and outlines conditions for exploring the doping-dependent evolution of the dispersion that underpins the ability to control many-body interactions in the material.

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.

(Invited) Electroluminescence from Single-Walled Carbon Nanotubes with Quantum Defects

Individual single-walled carbon nanotubes with covalent sidewall defects have emerged as a new class of photon sources whose photoluminescence spectra can be tailored by the carbon nanotube chirality and the attached functional group/molecule. Here we present electroluminescence spectroscopy data from single-tube devices based on (7,5) carbon nanotubes, functionalized with dichlorobenzene molecules, and wired to graphene electrodes. We observe electrically generated, defect-induced emissions that are controllable by electrostatic gating and strongly red-shifted compared to emissions from pristine nanotubes. The defect-induced emissions are assigned to excitonic and trionic recombination processes by correlating electroluminescence excitation maps with electrical transport and photoluminescence data. At cryogenic conditions additional, gate-dependent emission lines appear which are assigned to phonon-assisted hot-exciton electroluminescence from quasi-levels. Similar results were obtained with functionalized (6,5) nanotubes. We also compare functionalized (7,5) electroluminescence data with photoluminescence of pristine and functionalized (7,5) nanotubes redox-doped using gold(III) chloride solution. This work shows that electroluminescence excitation is selective toward neutral defect-state configurations with the lowest transition energy, which in combination with gate-control over neutral versus charged defect-state emission leads to high spectral purity.Reference: Min-Ken Li et al., ACS Nano 2022 (doi: 10.1021/acsnano.2c03083) Figure 1

(Invited) High-Performance Field-Effect Transistors Based on Two-Dimensional Materials for VLSI Circuits

Introduction Nowadays, the scaling of silicon very large-scale integration(VLSI) technologies has reached channel thicknesses of 7nm. However, further downscaling becomes increasingly difficult as the gate electrostatics require a substantial reduction of the channel thickness to about a fourth of the gate length. As a result, the actual gate length of high-performance(HP) FETs at the current state-of-the-art amounts to 16nm and is projected to stall at 12nm for the 1.5nm node and the following nodes, according to the International Roadmap for Devices and Systems(IRDS)[1]. For these nodes, two-dimensional(2D) materials could have the potential to replace silicon as the channel material. They can maintain sizable mobilities at atomic thicknesses, thus providing enhanced gate control in stacked channel nanosheet transistor structures[2]. Even though FETs based on 2D materials hold the promise to serve as FETs at the front end of the line, numerous challenges still need to be overcome. Downscaling Dimensions For ultra-scaled device designs, 2D materials can be used as a channel in stacked nanosheet FETs. In such a structure, the 2D material is gated from both sides, as depicted in Fig.1(a). By stacking multiple double-gated channels on top of each other, the required on-current density of around 1mA/μm can be achieved[3]. The first experimental demonstrations have achieved sub-5nm gate lengths[4] or, in a different design, a gate pitch of only 42nm[5], meeting the requirements for the 1.5nm node. While these prototypes show that 2D FETs can be scaled down, they have been fabricated in a laboratory. Many challenges must be overcome before such small devices can be fabricated in industry-compatible batch processes which require a high yield and low variability. Contact Engineering In order to enable sufficiently high on-current densities, small contact resistances to 2D semiconductors are required, which are inhibited by the formation of Schottky barriers at the metal to semiconductor interface. Schottky contacts to 2D materials are so prevalent because there is, on one side, a lack of stable doping schemes, and on the other side, pronounced Fermi-level pinning at the metal-to-semiconductor interface. Semi-metallic bismuth contacts can provide low-resistive contacts to n-type MoS2 FETs, as the bismuth suppresses the metal-induced gap states which pin the Fermi-level[6]. This way, a small contact resistance of 123Ωμm has been achieved, reaching the IRDS limit for the 1.5nm node. While comparable results have been realized for antimony contacts to n-type FETs, low-resistive contacts to p-type FETs are more challenging. Gate Stack Design A good gate stack for 2D FETs must provide excellent gate control while maintaining small gate leakage currents, which requires a capacitive equivalent thickness(CET) smaller than 0.9 nm. At these small CETs, a small gate leakage can only be obtained with a high-dielectric constant gate insulator and sizable band offsets, rendering some insulators, e.g. hexagonal boron nitride, unsuitable. Simultaneously, the gate insulator should form a van-der Waals interface with the 2D semiconductor, as otherwise, interface traps degrade the carrier mobility and the sub-threshold slope[7]. Charge traps within the insulator are the root cause of the limited stability and reliability of 2D FETs, as seen by a large hysteresis in the transfer characteristics or in pronounced Bias Temperature Instabilities(BTI). The electrical stability can be improved, if the defect bands in the gate insulator are energetically far away from the semiconductor’s conduction and valence band edges, see Fig.1(b)[8]. Conclusions Despite all the progress achieved within the last decade, the challenges for VLSI integration of 2D materials are enormous. First, stacked 2D FETs with scaled dimensions still need to be realized at an industrial scale. Second, despite low contact resistance demonstrations for n-type FETs, the resistances for p-type FETs are one order of magnitude too high. Finally, one of the most serious obstacles is identifying a suitable gate stack. Even though promising combinations of insulators to semiconductors have been suggested, like Bi2O5Se/Bi2O2Se, CaF2/MoS2 or SrTiO3/MoS2, it is at the moment unclear, which of them provides the best performance. Acknowledgments The authors thank for funding from the European Research Council under grant agreement no. 101055379.

Novel Mixed-Dimensional hBN-Passivated Silicon Nanowire Reconfigurable Field Effect Transistors: Fabrication and Characterization.

This work demonstrates the novel concept of a mixed-dimensional reconfigurable field effect transistor (RFET) by combining a one-dimensional (1D) channel material such as a silicon (Si) nanowire with a two-dimensional (2D) material as a gate dielectric. An RFET is an innovative device that can be dynamically programmed to perform as either an n- or p-FET by applying appropriate gate potentials. In this work, an insulating 2D material, hexagonal boron nitride (hBN), is introduced as a gate dielectric and encapsulation layer around the nanowire in place of a thermally grown or atomic-layer-deposited oxide. hBN flake was mechanically exfoliated and transferred onto a silicon nanowire-based RFET device using the dry viscoelastic stamping transfer technique. The thickness of the hBN flakes was investigated by atomic force microscopy and transmission electron microscopy. The ambipolar transfer characteristics of the Si-hBN RFETs with different gating architectures showed a significant improvement in the device's electrical parameters due to the encapsulation and passivation of the nanowire with the hBN flake. Both n- and p-type characteristics measured through the top gate exhibited a reduction of hysteresis by 10-20 V and an increase in the on-off ratio (ION/IOFF) by 1 order of magnitude (up to 108) compared to the values measured for unpassivated nanowire. Specifically, the hBN encapsulation provided improved electrostatic top gate coupling, which is reflected in the enhanced subthreshold swing values of the devices. For a single nanowire, an improvement up to 0.97 and 0.5 V/dec in the n- and p-conduction, respectively, is observed. Due to their dynamic switching and polarity control, RFETs boast great potential in reducing the device count, lowering power consumption, and playing a crucial role in advanced electronic circuitry. The concept of mixed-dimensional RFET could further strengthen its functionality, opening up new pathways for future electronics.

Thermally stable quantum Hall effect in a gated ferroelectric-graphene heterostructure

The quantum Hall effect is widely used for the investigation of fundamental phenomena, ranging from topological phases to composite fermions. In particular, the discovery of a room temperature resistance quantum in graphene is significant for compact resistance standards that can operate above cryogenic temperatures. However, this requires large magnetic fields that are accessible only in a few high magnetic field facilities. Here, we report on the quantum Hall effect in graphene encapsulated by the ferroelectric insulator CuInP2S6. Electrostatic gating of the graphene channel enables the Fermi energy to be tuned so that electrons in the localized states of the insulator are in equilibrium with the current-carrying, delocalized states of graphene. Due to the presence of strongly bound states in this hybrid system, a quantum Hall plateau is observed over a wide range of temperatures in relatively modest magnetic fields.

Ionic liquid gating induced self-intercalation of transition metal chalcogenides

Ionic liquids provide versatile pathways for controlling the structures and properties of quantum materials. Previous studies have reported electrostatic gating of nanometer-thick flakes leading to emergent superconductivity, insertion or extraction of protons and oxygen ions in perovskite oxide films enabling the control of different phases and material properties, and intercalation of large-sized organic cations into layered crystals giving access to tailored superconductivity. Here, we report an ionic-liquid gating method to form three-dimensional transition metal monochalcogenides (TMMCs) by driving the metals dissolved from layered transition metal dichalcogenides (TMDCs) into the van der Waals gap. We demonstrate the successful self-intercalation of PdTe2 and NiTe2, turning them into high-quality PdTe and NiTe single crystals, respectively. Moreover, the monochalcogenides exhibit distinctive properties from dichalcogenides. For instance, the self-intercalation of PdTe2 leads to the emergence of superconductivity in PdTe. Our work provides a synthesis pathway for TMMCs by means of ionic liquid gating driven self-intercalation.

Direct visualization of electronic transport in a quantum anomalous Hall insulator.

A quantum anomalous Hall (QAH) insulator is characterized by quantized Hall and vanishing longitudinal resistances at zero magnetic field that are protected against local perturbations and independent of sample details. This insensitivity makes the microscopic details of the local current distribution inaccessible to global transport measurements. Accordingly, the current distributions that give rise to transport quantization are unknown. Here we use magnetic imaging to directly visualize the transport current in the QAH regime. As we tune through the QAH plateau by electrostatic gating, we clearly identify a regime in which the sample transports current primarily in the bulk rather than along the edges. Furthermore, we image the local response of equilibrium magnetization to electrostatic gating. Combined, these measurements suggest that the current flows through incompressible regions whose spatial structure can change throughout the QAH regime. Identification of the appropriate microscopic picture of electronic transport in QAH insulators and other topologically non-trivial states of matter is a crucial step towards realizing their potential in next-generation quantum devices.

Enhanced electrodynamic gating in two-dimensional transistors using ferroelectric capping

Two-dimensional (2D) materials such as semiconductors and ferroelectrics are promising for future energy-efficient logic devices because of their extraordinary electronic properties at atomic thickness. In this work, we investigated a van der Waals heterostructure composited of 2D semiconducting MoS2 and 2D ferroelectric CuInP2S6 (CIPS) and NiPS3. Instead of using 2D ferroelectrics as conventional gate dielectric layers, here we applied CIPS and NiPS3 as a ferroelectric capping layer, and investigated a long-distance coupling effect with the gate upon the sandwiched 2D MoS2 channels. Our experimental results showed an outstanding enhancement of the electrodynamic gating in 2D MoS2 transistors, represented by a significant reduction of subthreshold swing at room temperature. This was due to the coupling-induced polarization of 2D ferroelectrics at 2D semiconductor surface which led to an effective and dynamic magnification of the gate capacitance. Meanwhile, the electrostatic gating was remained steady after adding the ferroelectric capping layer, providing ease and compatibility for further implementation with existing circuit and system design. Our work demonstrates the long-distance coupling effect of 2D ferroelectrics in a capping architecture, reveals its impacts from both electrodynamic and electrostatic perspectives, and expands the potential of 2D ferroelectrics to further improve the performance of energy-efficient nanoelectronics.

Epitaxial Kagome Thin Films as a Platform for Topological Flat Bands.

Systems with flat bands are ideal for studying strongly correlated electronic states and related phenomena. Among them, kagome-structured metals such as CoSn have been recognized as promising candidates due to the proximity between the flat bands and the Fermi level. A key next step will be to realize epitaxial kagome thin films with flat bands to enable tuning of the flat bands across the Fermi level via electrostatic gating or strain. Here, we report the band structures of epitaxial CoSn thin films grown directly on the insulating substrates. Flat bands are observed by using synchrotron-based angle-resolved photoemission spectroscopy (ARPES). The band structure is consistent with density functional theory (DFT) calculations, and the transport properties are quantitatively explained by the band structure and semiclassical transport theory. Our work paves the way to realize flat band-induced phenomena through fine-tuning of flat bands in kagome materials.

Iontronic and electrochemical investigations of 2D tellurene in aqueous electrolytes

AbstractThe remarkable successes of graphene have sparked increasing interest in elemental two‐dimensional (2D) materials, also referred to as Xenes. Due to their chemical simplicity and appealing physiochemical properties, Xenes have shown particular potential for numerous (opto) electronic, iontronic, and energy applications. Among them, layered α‐phase tellurene has demonstrated the most promise, thanks to the recent successes in the chemical synthesis of highly crystalline 2D tellurene. However, the general electronic and electrochemical properties of tellurene in electrolyte systems remain ambiguous, hindering their further development. In this work, we studied the electrostatic gating, electrocatalysis, and electrochemical stability of tellurene in electrolyte systems. Our results show that tellurene obtained from both hydrothermal and chemical vapor deposition methods, two mainstream synthetic approaches for Xenes, demonstrates thickness‐dependent ambipolar transport with high hole mobility and stability in both aqueous electrolytes and ionic liquids. More importantly, the electrochemical properties of tellurene are investigated via the emerging on‐chip electrochemistry. Pristine tellurene demonstrates hydrogen evolution reaction with low Tafel slopes and remarkable electrochemical stability in acidic electrolytes over a large potential window. Our study provides a comprehensive understanding of the iontronic and electrochemical properties of tellurene, paving the way for the broad adoption of Xenes in sensors, synaptic devices, and electrocatalysis.

Buried interfacial gate oxide for tri-gate negative-capacitance fin field-effect transistors: approach and investigation

Negative-capacitance fin field-effect transistors (NC-FinFETs), due to their superior gate electrostatics and dominance over short channel effects (SCEs), have been a key technology among conventional devices. The improved device performance in terms of the various engineering practices has paved the way for the advancement of NC-FinFETs. In the following work, we have proposed a novel buried oxide strategy for the NC-FinFET architecture, in which we have altered the depth of the interfacial gate oxide (IGO) layer inside the channel and analyzed the performance characteristics using TCAD Sentaurus. First, we varied the IGO thickness that was buried inside the channel and performed a comparative analysis between the DC, mixed-mode, and SCE parameters for the various buried configurations of the proposed NC-FinFET in order to realize the optimized depth. We also present the tolerable degradation in the circuit characteristics that occurs with the varying buried IGO (BIGO) depth. It can be inferred from the presented interface trap discussion that the idea of BIGO thickness holds well for low-power electronics.

Phase-Coherent Charge Transport through a Porphyrin Nanoribbon.

Since the early days of quantum mechanics, it has been known that electrons behave simultaneously as particles and waves, and now quantum electronic devices can harness this duality. When devices are shrunk to the molecular scale, it is unclear under what conditions does electron transmission remain phase-coherent, as molecules are usually treated as either scattering or redox centers, without considering the wave-particle duality of the charge carrier. Here, we demonstrate that electron transmission remains phase-coherent in molecular porphyrin nanoribbons connected to graphene electrodes. The devices act as graphene Fabry-Pérot interferometers and allow for direct probing of the transport mechanisms throughout several regimes. Through electrostatic gating, we observe electronic interference fringes in transmission that are strongly correlated to molecular conductance across multiple oxidation states. These results demonstrate a platform for the use of interferometric effects in single-molecule junctions, opening up new avenues for studying quantum coherence in molecular electronic and spintronic devices.

Three-terminal vertical ferroelectric synaptic barristor enabled by HZO/graphene heterostructure with rebound depolarization

Ferroelectric switching devices employing doped hafnium oxide (HfO2)-based thin films have expanded their range of electronic applications from densely-packed memory to brain-inspired artificial synapses. Here, we introduce a novel and distinctive three-terminal vertical device using a heterogeneous stack of hafnium-zirconium-oxide (HZO) thin film and graphene, called ferroelectric synaptic barristor (FSB), which can function as a scalable artificial synapse for energy-efficient neuromorphic computing. Electrostatic gating in the FSB can simultaneously reorient the polarization degree and the direction of HZO as well as the Schottky barrier and the trapping degree at the graphene interface. With these peculiar controlling factors, this process mimics crucial synaptic characteristics with rebound depolarization (RD), which converts an incoming inhibitory pre-spike into cell excitation. Using the RD function mediated by both ferroelectric switching and trap-mediated charge transport, the FSB exhibited a stable long-term potentiation/depression for 5000 identical pulse schemes with excellent linearity, high yield (47/48 cells), and a good state-retaining ability for 5000 s. The learning ability and energy consumption based on a single neural network were evaluated using MNIST handwritten digits and fashion patterns. The FSB with RD exhibited better accuracy (90.03% and 74.65% for handwritten digits and fashion patterns, respectively), fast and low-power learning ability than that without RD. Our FSB device can bring the advantages of conventional ferroelectric synaptic devices while mitigating their ingrained technical and operational issues.

Zero-dimensionality of a scaled-down VO2 metal-insulator transition via high-resolution electrostatic gating

An understanding of the phase transitions at the nanoscale is essential in state-of-the-art engineering1–5, instead of simply averaging the heterogeneous domains formed during phase transitions6,7. However, as materials are scaled down, the steepness of the phase transition rapidly increases8–13 and requires extremely high precision in the control method. Here, a three-terminal device, which could precisely control the phase transition electrically14–19, was applied for the first time to a scaled-down metal-insulator transition material VO2. The crossover from continuous to binary transitions with the scaled-down material was clarified, and the critical channel length was successfully elucidated via phase boundary energy. Notably, below the critical channel length, the spatial degrees of freedom degenerated, and the impact of drain voltage application disappeared in the phase transition, indicating zero-dimensionality of the VO2 channel. This zero-dimensionality could be the fundamental property in the scaled-down phase transition and have a significant impact on various fields that need nanoscale engineering.

Single-Molecule Junction Formation in Deep Eutectic Solvents with Highly Effective Gate Coupling.

The environment surrounding a molecular junction affects its charge-transport properties and, therefore, must be chosen with care. In the case of measurements in liquid media, the solvent must provide good solvation, grant junction stability, and, in the case of electrolyte gating experiments, allow efficient electrical coupling to the gate electrodes through control of the electrical double layer. We evaluated in this study the deep eutectic solvent mixture (DES) ethaline, which is a mixture of choline chloride and ethylene glycol (1:2), for single-molecule junction fabrication with break-junction techniques. In ethaline, we were able to (i) measure challenging and poorly soluble molecular wires, exploiting the improved solvation capabilities offered by DESs, and (ii) efficiently apply an electrostatic gate able to modulate the conductance of the junction by approximately an order of magnitude within a ∼1 V potential window. The electrochemical gating results on a Au-VDP-Au junction follow exceptionally well the single-level modeling with strong gate coupling (where VDP is 1,2-di(pyridine-4-yl)ethene). Ethaline is also an ideal solvent for the measurement of very short molecular junctions, as it grants a greatly reduced snapback distance of the metallic electrodes upon point-contact rupture. Our work demonstrates that DESs are viable alternatives to often relatively expensive ionic liquids, offering good versatility for single-molecule electrical measurements.

Tunable charge injection from graphene to halide perovskite induced by reversible ion segregation

Migration of point defects can result in various performance instabilities in organometal halide perovskite devices. In particular, the segregation of charged defects can influence the electron transport, but the correlation between ionic and electronic transports remains elusive. In this work, we use a graphene/methylammonium lead iodide capacitor to probe the effect of ion segregation on the charge injection behavior at the graphene/perovskite junction. In our samples, the ion segregation in the perovskite film is induced by a controllable electric field applied through an electrostatic gate. At the same time, the charge injection from graphene to the perovskite is probed by monitoring changes in the graphene conductivity. It is found that a positive (negative) defect accumulation layer near the graphene/perovskite interface can facilitate electron (hole) injection from the graphene electrode to the perovskite. Because the polarity of the defect accumulation layer is switchable by changing the direction of the applied electric field, the graphene/perovskite interface behaves like a Schottky junction with a tunable charge injection barrier height. This behavior should be generally found in other metal/halide perovskite interfaces as well.

Reversible Ionic Liquid Intercalation for Electrically Controlled Thermal Radiation from Graphene Devices.

Using graphene as a tunable optical material enables a series of optical devices such as switchable radar absorbers, variable infrared emissivity surfaces, or visible electrochromic devices. These devices rely on controlling the charge density on graphene with electrostatic gating or intercalation. In this paper, we studied the effect of ionic liquid intercalation on the long-term performance of optoelectronic devices operating within a broad infrared wavelength range. Our spectroscopic and thermal characterization results reveal the key limiting factors for the intercalation process and the performance of the infrared devices, such as the electrolyte ion-size asymmetry and charge distribution scheme and the effects of oxygen. Our results provide insight for the limiting mechanism for graphene applications in infrared thermal management and tunable heat signature control.