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At least 1,639 records · Page 91

Evaluating Safety with Automated Vehicles at Signalized Intersections: Application of Adaptive Cruise Control in Mixed Traffic

Automated Vehicles (AV) can potentially improve the performance of transportation system by reducing human errors and enhancing mobility and safety. In lower levels of automation, humans are still controlling the vehicle and receiving some advisory information regarding their surrounding environment. This paper investigates the safety impact of low and high levels of AVs, and their interaction with conventional human-driven vehicles at intersections. In order to enhance our understanding of the future interactions between conventional vehicles with AVs, we developed a framework to simulate the mixed traffic environment. Different market penetration scenarios are simulated using VENTOS (VEhicular NeTwork Open Simulator) software. A modified Wiedemann car-following model was calibrated to represent the behavior of human drivers of both conventional and low-level AVs, while an Adaptive Cruise Control model was used to represent high-level AVs. Notably, this study investigates purely the automation improvement in the system. We modified the acceleration and deceleration regimes of the Wiedemann model and tuned it by harnessing real-world connected vehicle data. Next, the simulation was calibrated utilizing two measures of driving volatility to ensure it closely represents the volatility measures of the real-world data. To evaluate the safety performance of a representative intersection under different scenarios, the number of longitudinal conflicts and driving volatility are used as surrogate safety indicators. The results reveal that increase in market penetration rate of LAVs and HAVs substantially improves intersection safety performance by reducing the number of conflicts and driving volatility.

Arvin, Ramin↗

Tuning Catalyst Activation and Utilization Via Controlled Electrode Patterning for Low-Loading and High-Efficiency Water Electrolyzers

An anode electrode concept of thin catalyst-coated liquid/gas diffusion layers (CCLGDLs), by integrating Ir catalysts with Ti thin tunable LGDLs with facile electroplating in proton exchange membrane electrolyzer cells (PEMECs), is proposed. The CCLGDL design with only 0.08 mg Ir cm -2 can achieve comparative cell performances to the conventional commercial electrode design, saving ~97% Ir catalyst and augmenting a catalyst utilization to ~24 times. CCLGDLs with regulated patterns enable insight into how pattern morphology impacts reaction kinetics and catalyst utilization in PEMECs. A specially designed two-sided transparent reaction-visible cell assists the in situ visualization of the PEM/electrode reaction interface for the first time. Oxygen gas is observed accumulating at the reaction interface, limiting the active area and increasing the cell impedances. In this work, it is demonstrated that mass transport in PEMECs can be modified by tuning CCLGDL patterns, thus improving the catalyst activation and utilization. The CCLGDL concept promises a future electrode design strategy with a simplified fabrication process and enhanced catalyst utilization. Furthermore, the CCLGDL concept also shows great potential in being a powerful tool for in situ reaction interface research in PEMECs and other energy conversion devices with solid polymer electrolytes.

08 HYDROGEN↗

Tuned to Terrible: A Study of Parallel Particle Advection State of the Practice

The algorithms foundational to visualization are central to the production visualization tools running at computing centers around the world and consume tremendous amounts of finite, limited resources. We believe that understanding the performance characteristics of these algorithms is critical in being good stewards of computational centers' resources. In this paper, we report initial studies on one such foundational algorithm: parallel particle advection. We have performed an extensive parameter study of the de facto standard algorithm that is commonly used in parallel production visualization tools as well as for in situ visualization environments. Our study has shown that the default parameters used in this algorithm lead to generally poor results, and identify settings that optimized performance on the system in our parameter sweep.

97 MATHEMATICS AND COMPUTING↗

Low-Cost Transformation of Biomass-Derived Carbon to High-Performing Nano-graphite via Low-Temperature Electrochemical Graphitization

Graphite, an essential component of energy storage devices, is traditionally synthesized via an energy-intensive thermal process (Acheson process) at ~3300 K. However, the battery performance of such graphite is abysmal under fast-charging conditions, which is deemed essential for the propulsion of electric vehicles to the next level. Herein, a low-temperature electrochemical transformation approach has been demonstrated to afford a highly crystalline nano-graphite with the capability of tuning interlayer spacing to enhance the lithium diffusion kinetics in molten salts at 850 °C. The essence of our strategy lies in the effective electrocatalytic transformation of carbon to graphite at a lower temperature that could significantly increase the energy savings, reduce the cost, shorten the synthesis time, and replace the traditional graphite synthesis. The resulting graphite exhibits high purity, crystallinity, a high degree of graphitization, and a nanoflake architecture that all ensure fast lithium diffusion kinetics (~2.0 × 10 –8 cm2 s –1 ) through its nanosheet. Such unique features enable outstanding electrochemical performance (~200 mA h g –1 at 5C for 1000 cycles, 1C = 372 mA g –1 ) as a fast-charging anode for lithium-ion batteries. Overall, this finding paves the way to make high energy-density fast-charging batteries that could boost electromobility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

MABAL: a Novel Deep-Learning Architecture for Machine-Assisted Bone Age Labeling

Bone age assessment (BAA) is a commonly performed diagnostic study in pediatric radiology to assess skeletal maturity. The most commonly utilized method for assessment of BAA is the Greulich and Pyle method (Pediatr Radiol 46.9:1269–1274, 2016; Arch Dis Child 81.2:172–173, 1999) atlas. The evaluation of BAA can be a tedious and time-consuming process for the radiologist. As such, several computer-assisted detection/diagnosis (CAD) methods have been proposed for automation of BAA. Classical CAD tools have traditionally relied on hard-coded algorithmic features for BAA which suffer from a variety of drawbacks. Recently, the advent and proliferation of convolutional neural networks (CNNs) has shown promise in a variety of medical imaging applications. There have been at least two published applications of using deep learning for evaluation of bone age (Med Image Anal 36:41–51, 2017; JDI 1–5, 2017). However, current implementations are limited by a combination of both architecture design and relatively small datasets. The purpose of this study is to demonstrate the benefits of a customized neural network algorithm carefully calibrated to the evaluation of bone age utilizing a relatively large institutional dataset. In doing so, this study will aim to show that advanced architectures can be successfully trained from scratch in the medical imaging domain and can generate results that outperform any existing proposed algorithm. The training data consisted of 10,289 images of different skeletal age examinations, 8909 from the hospital Picture Archiving and Communication System at our institution and 1383 from the public Digital Hand Atlas Database. The data was separated into four cohorts, one each for male and female children above the age of 8, and one each for male and female children below the age of 10. The testing set consisted of 20 radiographs of each 1-year-age cohort from 0 to 1 years to 14–15+ years, half male and half female. The testing set included left-hand radiographs done for bone age assessment, trauma evaluation without significant findings, and skeletal surveys. A 14 hidden layer-customized neural network was designed for this study. The network included several state of the art techniques including residual-style connections, inception layers, and spatial transformer layers. Data augmentation was applied to the network inputs to prevent overfitting. A linear regression output was utilized. Mean square error was used as the network loss function and mean absolute error (MAE) was utilized as the primary performance metric. MAE accuracies on the validation and test sets for young females were 0.654 and 0.561 respectively. For older females, validation and test accuracies were 0.662 and 0.497 respectively. For young males, validation and test accuracies were 0.649 and 0.585 respectively. Finally, for older males, validation and test set accuracies were 0.581 and 0.501 respectively. The female cohorts were trained for 900 epochs each and the male cohorts were trained for 600 epochs. An eightfold cross-validation set was employed for hyperparameter tuning. Test error was obtained after training on a full data set with the selected hyperparameters. Using our proposed customized neural network architecture on our large available data, we achieved an aggregate validation and test set mean absolute errors of 0.637 and 0.536 respectively. To date, this is the best published performance on utilizing deep learning for bone age assessment. Our results support our initial hypothesis that customized, purpose-built neural networks provide improved performance over networks derived from pre-trained imaging data sets. We build on that initial work by showing that the addition of state-of-the-art techniques such as residual connections and inception architecture further improves prediction accuracy. This is important because the current assumption for use of residual and/or inception architectures is that a large pre-trained network is required for successful implementation given the relatively small datasets in medical imaging. Instead we show that a small, customized architecture incorporating advanced CNN strategies can indeed be trained from scratch, yielding significant improvements in algorithm accuracy. It should be noted that for all four cohorts, testing error outperformed validation error. One reason for this is that our ground truth for our test set was obtained by averaging two pediatric radiologist reads compared to our training data for which only a single read was used. This suggests that despite relatively noisy training data, the algorithm could successfully model the variation between observers and generate estimates that are close to the expected ground truth.

62 RADIOLOGY AND NUCLEAR MEDICINE↗

Analysis of double stub tuner control stability in a phased array antenna with strong cross-coupling

Active stub tuning with a fast ferrite tuner (FFT) has greatly increased the ability of fusion ion cyclotron range of frequency (ICRF) systems (50–100 MHz) by allowing for the antenna system to respond dynamically to changes in the plasma load impedance such as during the L–H transition or edge localized modes (ELMs). A high power waveguide double-stub tuner is under development for use with the Alcator C-Mod lower hybrid current drive (LHCD) system at 4.6 GHz. The amplitude and relative phase shift between adjacent columns of an LHCD antenna are critical for control of the launched n || spectrum. Adding a double-stub tuning network will perturb the phase and amplitude of the forward wave particularly if the unmatched reflection coefficient is high. This effect can be compensated by adjusting the phase of the low power microwave drive for each klystron amplifier. Cross-coupling of the reflected power between columns of the launcher must also be considered. The problem is simulated by cascading a scattering matrix for the plasma provided by a linear coupling model with the measured launcher scattering matrix and that of the FFTs. The solution is advanced in an iterative manner similar to the time-dependent behavior of the real system. System performance is presented under a range of edge density conditions from under-dense to over-dense and a range of launched n || . Simulations suggest power reflection coefficients (Γ 2 ) of less than 1% with no contamination of the n || spectrum. Instability of the FFT tuning network can be difficult for certain plasma conditions and relative phasings, but reducing the control gain of the FFT network stabilizes the system.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Advanced thermal/environmental barrier coatings of high-entropy rare earth disilicates tuned by strong anharmonicity of Eu 2 Si 2 O 7

Advancing thermal/environmental barrier coating (TEBC) materials with integrated thermal-mechanical functions is paramount for safeguarding SiC-based ceramic matrix composites (CMCs) in high-efficiency gas turbines. Herein, we employ a synergistic approach, combining density functional theory (DFT) methods and combinatorial chemistry techniques, to design high-performance and low-cost RE 2 Si 2 O 7 (RE = rare earth elements) TEBC materials tailored for enhanced compatibility with SiC-based CMCs. Expanding on phase stability of alloying pure RE 2 Si 2 O 7 , the investigation extends to the mechanical and thermal properties of solid solution systems, including Er 1/2 Y 3/4 Yb 3/4 Si 2 O 7 , Gd 1/4 Er 1/4 Y 3/4 Yb 3/4 Si 2 O 7 , and Eu 1/4 Er 1/4 Y 3/4 Yb 3/4 Si 2 O 7 . The solid solution systems exhibit a major reduction in lattice thermal conductivity relative to their pure counterparts, achieving ultralow values of 0.25 to 0.39 W m −1 K −1 at 1500 K. Furthermore, the coefficients of thermal expansion (CTE) of these solid solutions are precisely tuned within the desired range for SiC (4.4 to 5.5 × 10 −6 K −1 ), while maintaining good mechanical properties. Here, in particular, the addition of Eu 2 Si 2 O 7 demonstrates to be an important variable to the tuning of CTE and lattice thermal conductivity by leveraging its strong anharmonicity, presenting a pioneering avenue for fine-tuning material properties. In summary, this research not only identifies promising TEBC materials with superior thermal properties, but also introduces a valuable computational material design methodology for the rapid discovery of complex materials for harsh environments.

36 MATERIALS SCIENCE↗

Epitaxial Design of Complex Nickelates as Electrocatalysts for the Oxygen Evolution Reaction

Abstract The oxygen evolution reaction (OER) is a crucial process in electrochemical water splitting, a promising technology to renewably yield hydrogen gas from water. Designing and developing earth‐abundant, efficient, and stable OER electrocatalysts to replace the most widely used but scarce RuO 2 and IrO 2 are thus of critical interest. Recently, ABO 3 ‐structured perovskite oxides, especially rare‐earth nickelates, are extensively studied for their potential use as OER electrocatalysts. In particular, the epitaxial synthesis of complex oxide thin films allows flexible and precise control over the materials so that their structure–stability–property relationships can be established. Using nickelate thin films as model systems, this review illustrates how epitaxial design allows researchers to test different hypotheses and proposed descriptors, as well as formulate new design principles. Following a brief introduction to the background of OER mechanisms, proposed activity descriptors, and synthesis methods, various epitaxial design strategies are surveyed including strain tuning, composition control, surface termination/orientation selection, defect engineering, and interface design. These have led to precise control over the atomic structures and electronic properties of nickelates which in turn determine their electrochemical performance. Finally, the remaining challenges and perspectives toward a deeper understanding and use of complex oxides as OER catalysts are discussed.

Choi, Min‐Ju↗

Charge Transfer from Carbon Nanotubes to Silicon in Flexible Carbon Nanotube/Silicon Solar Cells

Mechanical fragility and insufficient light absorption are two major challenges for thin flexible crystalline Si-based solar cells. Flexible hybrid single-walled carbon nanotube (SWNT)/Si solar cells are demonstrated by applying scalable room-temperature processes for the fabrication of solar-cell components (e.g., preparation of SWNT thin films and SWNT/Si p–n junctions). The flexible SWNT/Si solar cells present an intrinsic efficiency ≈7.5% without any additional light-trapping structures. By using these solar cells as model systems, the charge transport mechanisms at the SWNT/Si interface are investigated using femtosecond transient absorption. Although primary photon absorption occurs in Si, transient absorption measurements show that SWNTs also generate and inject excited charge carriers to Si. Such effects can be tuned by controlling the thickness of the SWNTs. Thus, findings from this study could open a new pathway for designing and improving the efficiency of photocarrier generation and absorption for high-performance ultrathin hybrid SWNT/Si solar cells.

14 SOLAR ENERGY↗

Balancing Flexible Side Chains on 2D Conjugated Acceptors Enables High‐Performance Organic Solar Cell

Abstract Balancing the rigid backbones and flexible side chains of light‐harvesting materials is crucially important to reach optimized intermolecular packing, micromorphology, and thus photovoltaic performance of organic solar cells (OSCs). Herein, based on a distinctive CH‐series acceptor platform with 2D conjugation extended backbones, a series of nonfullerene acceptors (CH‐6F‐Cn) are synthesized by delicately tuning the lengths of flexible side chains fromn‐octyl ton‐amyl. A systemic investigation has revealed that the variation of the side chain's length can not only modulate intermolecular packing modes and crystallinity but also dramatically improve the micromorphology of the active layer and eventual photovoltaic parameters of OSCs. Consequently, the highest PCE of 18.73% can be achieved by OSCs employingD18:PM6:CH‐6F‐C8as light‐harvesting materials.

Chemistry↗

Predicting critical heat flux with uncertainty quantification and domain generalization using conditional variational autoencoders and deep neural networks

Deep generative models (DGMs) can generate synthetic data samples that closely resemble the original dataset, addressing data scarcity. In this work, we developed a conditional variational autoencoder (CVAE) to augment critical heat flux (CHF) data used for the 2006 Groeneveld lookup table. To compare with traditional methods, a fine-tuned deep neural network (DNN) regression model was evaluated on the same dataset. Both models achieved small mean absolute relative errors, with the CVAE showing more favorable results. Uncertainty quantification (UQ) was performed using repeated CVAE sampling and DNN ensembling. The DNN ensemble improved performance over the baseline, while the CVAE maintained consistent results with less variability and higher confidence. Both models achieved small errors inside and outside the training domain, with slightly larger errors outside. Altogether, the CVAE performed better than the DNN in predicting CHF and exhibited better uncertainty behavior.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

Machine learning-based ethylene and carbon monoxide estimation, real-time optimization, and multivariable feedback control of an experimental electrochemical reactor

Electrochemical reduction of CO 2 gas is a novel CO 2 utilization technique that has the potential to mitigate the global climate crisis caused by anthropogenic CO 2 emissions, and enable the large-scale storage of energy generated from renewable sources in the form of carbon-based chemicals and fuels. However, due to the complexity of the electrochemical reactions, the explicit first-principles models for CO2 reduction are not available yet, and there has been a limited effort to develop process modeling, optimization and control of CO 2 electrochemical reactors. To this end, a rotating cylinder electrode (RCE) reactor has been constructed at UCLA to understand the mass transfer and reaction kinetics effects separately on the productivity. In the RCE reactor, the applied potential strongly influences the reaction energetics and the electrode rotation speed affects the hydrodynamic boundary layer and modifies the film mass transfer coefficient, which involves convective and diffusive transport. Further, the present work aims to develop a multi-input multi-output (MIMO) control scheme for the RCE reactor that integrates techniques from artificial and recurrent neural network modeling, nonlinear optimization, and process controller design. Specifically, production rates of two products from the experimental reactor, ethylene and carbon monoxide, are controlled by manipulating two inputs, applied potential and catalyst rotation speed. Process dynamics and controllability are analyzed, a feedback control strategy is designed and the controllers are tuned accordingly. The experimental electrochemical cell is employed to gather data for process modeling and implement the multivariable control system. Finally, the experimental results are presented which demonstrate excellent closed-loop performance by the control system and regulation of the outputs at three different set-points including an economically-optimal set-point.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Recent trends on the application of PGM-free catalysts at the cathode of anion exchange membrane fuel cells

Anion exchange membrane fuel cells (AEMFCs) are becoming more and more attractive due to their alkaline environment, being less aggressive and favorable to the use of low-cost materials. Furthermore, the alkaline medium displays enhanced alcohol oxidation reaction kinetics, which favors the use of fuels different from hydrogen, ranging from alcohols to polyols, and enhanced oxygen reduction reaction (ORR) kinetics. This allows the use of non-noble transition metals to synthesize cathodic catalysts, avoiding the costly platinum-group metals (PGM). In particular, the most active catalysts developed so far are mostly synthesized by sacrificial support method, which allows the fine tuning of the morphology, favoring oxygen transport, water removal, density of Fe-Nx active sites, and thus an enhanced electrochemical ORR activity. This mini-review analyzes the best AEMFCs cell performance achieved so far in recent years when PGM-free catalysts based on Me-N-C (Me = Fe, Co) are used for ORR at the cathode side, for AEMFCs fed with hydrogen, methanol, and ethanol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Nanotubes from the Misfit Layered Compound (SmS) 1.19 TaS 2 : Atomic Structure, Charge Transfer, and Electrical Properties

Misfit layered compounds (MLCs) MX-TX 2 , where M, T = metal atoms and X = S, Se, or Te, and their nanotubes are of significant interest due to their rich chemistry and unique quasi-1D structure. In particular, LnX-TX 2 (Ln = rare-earth atom) constitute a relatively large family of MLCs, from which nanotubes have been synthesized. The properties of MLCs can be tuned by the chemical and structural interplay between LnX and TX 2 sublayers and alloying of each of the Ln, T, and X elements. In order to engineer them to gain desirable performance, a detailed understanding of their complex structure is indispensable. MLC nanotubes are a relative newcomer and offer new opportunities. In particular, like WS 2 nanotubes before, the confinement of the free carriers in these quasi-1D nanostructures and their chiral nature offer intriguing physical behavior. High-resolution transmission electron microscopy in conjunction with a focused ion beam are engaged to study SmS-TaS 2 nanotubes and their cross-sections at the atomic scale. The atomic resolution images distinctly reveal that Ta is in trigonal prismatic coordination with S atoms in a hexagonal structure. Furthermore, the position of the sulfur atoms in both the SmS and the TaS 2 sublattices is revealed. X-ray photoelectron spectroscopy, electron energy loss spectroscopy, and X-ray absorption spectroscopy are carried out. These analyses conclude that charge transfer from the Sm to the Ta atoms leads to filling of the Ta 5d z 2 level, which is confirmed by density functional theory (DFT) calculations. Transport measurements show that the nanotubes are semimetallic with resistivities in the range of 10 –4 Ω·cm at room temperature, and magnetic susceptibility measurements show a superconducting transition at 4 K.

36 MATERIALS SCIENCE↗

Effect of Redox-Inactive Metal Ion–Nickel(III) Interactions on the Redox Properties and Proton-Coupled Electron Transfer Reactivity

We report Mononuclear nickel(II) and nickel(III) complexes of a bisamidate-bisalkoxide ligand, (NMe 4 ) 2 [Ni- II (HMPAB)] (1) and (NMe 4 )[Ni III (HMPAB)] (2), respectively, have been synthesized and characterized by various spectroscopic techniques including X-ray crystallography. The reaction of redox-inactive metal ions (M n+ = Ca 2+ , Mg 2+ , Zn 2+ , Y 3+ , and Sc 3+ ) with 2 resulted in 2-M n+ adducts, which was assessed by an array of spectroscopic techniques including X-ray absorption spectroscopy (XAS), electron paramagnetic resonance (EPR), and reactivity studies. The X-ray structure of Ca 2+ coordinated to Ni(III) complexes, 2Ca 2+ T, was determined and exhibited an average Ni-Ca distance of 3.1253 angstrom, close to the metal ions' covalent radius. XAS analysis of 2-Ca 2+ and 2-Y 3+ in solution further revealed an additional coordination to Ca and Y in the 2-M n+ adducts with shortened Ni-M distances of 2.15 and 2.11 Å, respectively, implying direct bonding interactions between Ni and Lewis acids (LAs). Such a short interatomic distance between Ni(III) and M is unprecedented and was not observed before. EPR analysis of 2 and 2-M n+ species, moreover, displayed rhombic signals with g av > 2.12 for all complexes, supporting the +III oxidation state of Ni. The Ni III /Ni II redox potential of 2 and 2-M n+ species was determined, and a plot of E 1/ 2 of 2-M n+ versus pK a of [M(H 2 O) n ] m+ exhibited a linear relationship, implying that the Ni III /Ni II potential of 2 can be tuned with different redox-inactive metal ions. Reactivity studies of 2 and 2-M n+ with different 4-X-2,6-ditert-butylphenol (4-XDTBP) and other phenol derivatives were performed, and based on kinetic studies, we propose the involvement of a proton-coupled electron transfer (PCET) pathway. Analysis of the reaction products after the reaction of 2 with 4-OMe-DTBP showed the formation of a Ni(II) complex (1a) where one of the alkoxide arms of the ligand is protonated. A pK a value of 24.2 was estimated for 1a. The reaction of 2-M n+ species was examined with 4-OMe-DTBP, and it was observed that the k 2 values of 2-M n+ species increase by increasing the Lewis acidity of redox-inactive metal ions. However, the obtained k 2 values for 2-M n+ species are much lower compared to the k 2 value for 2. Such a variation of PCET reactivity between 2 and 2-M n+ species may be attributed to the interactions between Ni(III) and LAs. Our findings show the significance of the secondary coordination sphere effect on the PCET reactivity of Ni(III) complexes and furnish important insights into the reaction mechanism involving high-valent nickel species, which are frequently invoked as key intermediates in Ni-mediated enzymatic reactions, solar-fuel catalysis, and biomimetic/synthetic transformation reactions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Gate-Tunable Semiconductor Heterojunctions from 2D/3D van der Waals Interfaces

Van der Waals (vdW) semiconductors are attractive for highly scaled devices and heterogeneous integration since they can be isolated into self-passivated, two-dimensional (2D) layers that enable superior electrostatic control. These attributes have led to numerous demonstrations of field-effect devices ranging from transistors to triodes. By exploiting the controlled, substitutional doping schemes in covalently-bonded, three-dimensional (3D) semiconductors and the passivated surfaces of 2D semiconductors, one can construct devices that can exceed performance metrics of “all-2D” vdW heterojunctions. Here, we demonstrate, 2D/3D semiconductor heterojunctions using MoS2 as the prototypical 2D semiconductor laid upon Si and GaN as the 3D semiconductor layers. By tuning the Fermi levels in MoS2, we demonstrate devices that concurrently exhibit over seven orders of magnitude modulation in rectification ratios and conductance. Our results further suggest that the interface quality does not necessarily affect Fermi-level tuning at the junction opening up possibilities for novel 2D/3D heterojunction device architectures

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Ionic Control over Ferroelectricity in 2D Layered van der Waals Capacitors

The van der Waals layered material CuInP 2 S 6 features interesting functional behavior, including the existence of four uniaxial polarization states, polarization reversal against the electric field through Cu ion migration, a negative-capacitance regime, and reversible extraction of Cu ions. At the heart of these characteristics lies the high mobility of Cu ions, which also determines the spontaneous polarization. Therefore, Cu migration across the lattice results in unusual ferroelectric behavior. Here, we demonstrate how the interplay of polar and ionic properties provides a path to ionically controlled ferroelectric behavior, achieved by applying selected DC voltage pulses and subsequently probing ferroelectric switching during fast triangular voltage sweeps. Using current measurements and theoretical calculations, we observe that increasing DC pulse duration results in higher ionic currents, the buildup of an internal electric field that shifts polarization loops, and an increase in total switchable polarization by ~50% due to the existence of a high polarization phase which is stabilized by the internal electric field. Apart from tuning ferroelectric behavior by selected square pulses, hysteretic polarization switching can even be entirely deactivated and reactivated, resulting in three-state systems where polarization switching is either inhibited or can be performed in two different directions.

36 MATERIALS SCIENCE↗