Ion Dynamics Research Articles

First-principles molecular dynamics of exciton-driven initial stage of plasma phase transition in warm dense molecular nitrogen.

Understanding the properties of molecular nitrogen N2 at extreme conditions is the fundamental problem for atomistic theory and the important benchmark for the capabilities of first-principles molecular dynamics (FPMD) methods. In this work, we focus on the connection between the dynamics of ions and electronic excitations in warm dense N2. The restricted open-shell Kohn-Sham method gives us the possibility to reach relevant time and length scales for FPMD modeling of an isolated exciton dynamics in warm dense N2. Wannier localization sheds light on the corresponding mechanisms of covalent bond network rearrangements that stand behind polymerization kinetics. FPMD results suggest a concept of energy transfer from the thermal energy of ions into the internal energy of polymeric structures that form in warm dense N2 at extreme conditions. Our findings agree with the thermobaric conditions for the onset of absorption in the optical spectroscopy study of Jiang et al. [Nat. Commun. 9, 2624 (2018)].

All‐Polymer Organic Electrochemical Synaptic Transistor With Controlled Ionic Dynamics for High‐Performance Wearable and Sustainable Reservoir Computing

All‐Polymer Organic Electrochemical Synaptic Transistor With Controlled Ionic Dynamics for High‐Performance Wearable and Sustainable Reservoir Computing

Translational Dynamics of Cations and Anions in Ionic Liquids from NMR Field Cycling Relaxometry: Highlighting the Importance of Heteronuclear Contributions.

NMR field cycling relaxometry is a powerful method for determining the rotational and translational dynamics of ions, molecules, and dissolved particles. This is in particular true for ionic liquids (ILs) in which both ions carry NMR sensitive nuclei. In the IL triethylammonium bis(trifluoromethanesulfonyl)imide ([TEA][NTf2]), there are 1H nuclei at the [TEA]+ cations and 19F nuclei at the [NTf2]- anions. Moreover, the high viscosity of this IL leads to frequency-dependent relaxation rates, leaving the so-called extreme narrowing regime. Both the rotational and the translational dynamics of the constituents of ILs can be obtained by separating the contributions of intra- and intermolecular relaxation rates. In particular, the translational dynamics can be obtained separately by applying the so-called "low-frequency approach" (LFA), utilizing the fact that the change in the total relaxation rates at low frequencies results solely from translational motions. However, for systems containing multiple NMR active nuclei, heteronuclear interactions can also affect their relaxation rates. For [TEA][NTf2], the intermolecular relaxation rate is either the sum of 1H-1H cation-cation and 1H-19F cation-anion interactions or the sum of 19F-19F anion-anion and 19F-1H anion-cation interactions. Due to the lack of available experimental information, the 1H-19F heteronuclear intermolecular contribution has often been neglected in the past, assuming it to be negligible. Employing a suitable set of ILs and by making use of isotopic H/D substitution, we show that the 1H-19F heteronuclear intermolecular contribution in fact cannot be neglected and that the LFA cannot be applied to the total 1H and total 19F relaxation rates.

Na+ conductivity of (100−x)Na3PS4−xCa3N2 glass and glass−ceramics

AbstractThe ionic conductivity of Na3PS4 can be improved via the aliovalent substitution of P and S as well as multivalence cation substitution of Na. Although the enhanced ionic conductivities of tetragonal and cubic Na3PS4 have been theoretically and experimentally studied, the dynamics of sodium ions in these systems have been rarely reported. In this study, (100−x)Na3PS4−xCa3N2 (0 ≤ x ≤ 10) glass samples were synthesizing using high‐energy planetary ball‐milling method. These samples were subjected to heat treatment at 280°C for 1 h in an argon atmosphere to obtain glass–ceramic samples. The structures of these samples were characterized via Raman spectroscopy and X‐ray diffraction analysis. The lattice parameter and cell volume of the glass–ceramic samples strongly depended on the x value in (100−x)Na3PS4−xCa3N2 (0 ≤ x ≤ 10). Their ionic conductivities were determined via alternating current electrochemical impedance spectroscopy (EIS). 92Na3PS4−8Ca3N2 glass–ceramics exhibited an ionic conductivity of 8.14 × 10−4 Scm−1 at 25°C. Charge carrier concentration and hopping rate were extracted from the EIS data to determine the ionic conductivities of the samples. The activation energies of DC conductivity and mobile ion formation and migration were also derived from the EIS data to analyze the effect of Ca3N2 doping on the ionic conductivity of the synthesized samples.

Boolean Computation in Single-Transistor Neuron.

Brain neurons exhibit far more sophisticated and powerful information-processing capabilities than the simple integrators commonly modeled in neuromorphic computing. A biological neuron can in fact efficiently perform Boolean algebra, including linear nonseparable operations. Traditional logic circuits require more than a dozen transistors combined as NOT, AND, and OR gates to implement XOR. Lacking biological competency, artificial neural networks require multilayered solutions to exercise XOR operation. Here, it is shown that a single-transistor neuron, harnessing the intrinsic ambipolarity of graphene and ionic filamentary dynamics, can enable in situ reconfigurable multiple Boolean operations from linear separable to linear nonseparable in an ultra-compact design. By leveraging the spatiotemporal integration of inputs, bio-realistic spiking-dependent Boolean computation is fully realized, rivaling the efficiency of a human brain. Furthermore, a soft-XOR-based neural network via algorithm-hardware co-design, showcasing substantial performance improvement, is demonstrated. These results demonstrate how the artificial neuron, in the ultra-compact form of a single transistor, may function as a powerful platform for Boolean operations. These findings are anticipated to be a starting point for implementing more sophisticated computations at the individual transistor neuron level, leading to super-scalable neural networks for resource-efficient brain-inspired information processing.

Reduced electrostatic turbulence in the quasi-isodynamic stellarator configuration CIEMAT-QI4

Abstract CIEMAT-QI4 is a quasi-isodynamic stellarator configuration that simultaneously features very good fast-ion confinement in a broad range of β values, low neoclassical transport and bootstrap current, and ideal magnetohydrodynamic stability up to β=5%. In this paper it is shown that CIEMAT-QI4 also exhibits reduced turbulent transport. This is demonstrated through nonlinear electrostatic simulations with the gyrokinetic code stella, including kinetic ions and electrons. The relation between reduced turbulent transport and the fact that CIEMAT-QI4 very approximately satisfies the so-called maximum-J property is discussed.

Controlling directional emission of ions attached on the surface of nanoparticles

Abstract The interaction between lasers and nanoparticles holds significant theoretical and practical importance. Here, we investigate the near-field enhancement effects on silver nanotriangles and nanodiscs under ultrafast laser pulses, as well as the dynamics of protons and ions attached to the nanoparticle surfaces. By adjusting the size parameters of the nanoparticles, we explore the near-field enhancement effects and proton emission dynamics at different laser wavelengths. The results demonstrate that nanoparticles with varying morphologies substantially impact the proton momentum spectrum. The directional proton emission of nanotriangle structures is more pronounced compared to that of nanodiscs, and this effect can be further enhanced by adjusting the laser wavelength. Additionally, manipulating the thickness of particles also controls the Mie scattering phenomenon of light. Finally, we qualitatively discuss the emission processes of alpha particles and 9C6+ heavy ions. This research has important implications for proton and heavy ion radiotherapy in cancer treatment and targeted drug delivery, while providing theoretical foundations for understanding, characterizing, and controlling experimental studies of nanosystems with significant potential for expanding research into microdynamic behavior in complex nanomaterial superstructures.

Triboelectric Programmed Droplet Manipulation for Plug‐and‐Play Assembly

AbstractProgrammed droplet transport which is typically directed by surface energy gradients or external fields, is crucial in domains ranging from chemical reaction modulation to self‐powered intelligent sensing. However, droplet motion control remains constrained by path reconfiguration, requirements on chemical surface modification, and platform complexity. Here, a more universal plug‐and‐play droplet manipulation paradigm based on liquid‐solid contact electrification and triboelectricwetting on common dielectric surfaces is reported. By regulating the electrical double layer via asymmetric ion dynamics, the triboelectric charge polarity of droplets can be adjusted, enabling in situ manipulation without path reconfiguration dictated by the conventional droplet motion output. Droplets achieved an ultrahigh velocity of 450 mm s−1 on general surfaces, significantly exceeding the speeds observed in droplets subjected to constant electrostatic fields with chemical modifications. This flexible and modular functionally decoupled manipulation strategy offers an environmentally friendly, cost‐effective, and versatile paradigm, facilitating applications in chemical analysis and smart sensing.

On the potential of the Cluster Ion Counter (CIC) to observe local new particle formation, condensation sink and growth rate of newly formed particles

Abstract. The Cluster Ion Counter (CIC) is a simple three-channel instrument designed to observe ions in the electrical mobility equivalent diameter range from 1.0 to 5 nm. With the three channels, we can observe concentrations of both ion clusters (sub-2 nm ions) and intermediate ions. Furthermore, as derived here, we can estimate condensation sink (CS), intensity of local new particle formation, growth rate of newly formed particles from 2 to 3 nm and formation rate of 2 nm ions. We compared CIC measurements with those of a multichannel ion spectrometer, the Neutral cluster and Air Ion Spectrometer (NAIS), and found that the concentrations agreed well between the two instruments, with correlation coefficients of 0.89 and 0.86 for sub-2 nm and 2.0–2.3 nm ions, respectively. According to the observations made in Hyytiälä, Finland, and Beijing, China, the ion source rate was estimated to be about two to four ion pairs cm−3 s−1. The new CIC is a simple and cheap instrument that can be used in different environments to obtain information about small ion dynamics, local intermediate ion formation and CS in a robust way when combined with the theoretical framework presented here.

Binding kinetics of quaternary ammonium ions in Kcv potassium channels.

Kcv channels from plant viruses represent the autonomous pore module of potassium channels, devoid of any regulatory domains. These small proteins show very reproducible single-channel behavior in planar lipid bilayers. Thus, they are an optimum system for the study of the biophysics of ion transport and gating. Structural models based on homology modeling have been used successfully, but experimental structural data are currently not available. Here we determine the size of the cytosolic pore entrance by studying the blocker kinetics. Blocker binding and dissociation rate constants ranging from 0.01 to 1000 ms-1 were determined for different quaternary ammonium ions. We found that the cytosolic pore entrance of KcvNTS must be at least 11 Å wide. The results further indicate that the residues controlling a cytosolic gate in one of the Kcv isoforms influence blocker binding/dissociation as well as a second gate even when the cytosolic gate is in the open state. The voltage dependence of the rate constant of blocker release is used to test, which blockers bind to the same binding site.

Comparison of Construction Strategies of Solid Electrolyte Interface (SEI) in Li Battery and Mg Battery-A Review.

The solid electrolyte interface (SEI) plays a critical role in determining the performance, stability, and longevity of batteries. This review comprehensively compares the construction strategies of the SEI in Li and Mg batteries, focusing on the differences and similarities in their formation, composition, and functionality. The SEI in Li batteries is well-studied, with established strategies that leverage organic and inorganic components to enhance ion diffusion and mitigate side reactions. In contrast, the development of the SEI in Mg batteries is still in its initial stages, facing significant challenges such as severe passivation and slower ion kinetics due to the divalent nature of magnesium ions. This review highlights various approaches to engineering SEIs in both battery systems, including electrolyte optimization, additives, and surface modifications. Furthermore, it discusses the impact of these strategies on electrochemical performance, cycle life, and safety. The comparison provides insights into the underlying mechanisms, challenges, and future directions for SEI research.

Low‐Temperature Sodium–Sulfur Batteries Enabled by Ionic Liquid in Localized High Concentration Electrolytes

AbstractLow ionic migration and compromised interfacial stability pose challenges for low‐temperature batteries. In this work, we discovered that even with the state‐of‐the‐art localized high‐concentration electrolytes (LHCEs), uncontrolled Na electrodeposition occurs with a huge overpotential of >1.2 V at −20 °C, leading to cell failure within tens of hours. To address this, we introduce a new electrolyte category that incorporates an ionic liquid as a key solvation species. Diverging from traditional LHCEs, the IL‐tailored LHCE facilitates an anion–solvent‐molecules exchange within the solvation sheath between Na+ and organic cations at low temperatures. This behavior reduces solvation cluster size and strengthens Na+–anion coordination, which proves instrumental in enabling fast ionic dynamics in both the bulk liquid and at the interface. Therefore, durable Na electrodeposition and shuttle‐free, 0.5 Ah sodium–sulfur pouch cells are achieved at −20 °C, for the first time, surpassing the limitations of typical LHCEs. This tailoring strategy opens a new design direction for advanced batteries operating in fast‐charge and wide‐temperature scenarios.

Graphene/chitosan nanoreactors for ultrafast and precise recovery and catalytic conversion of gold from electronic waste

The extraction of gold (Au) from electronic waste (e-waste) has both environmental impact and inherent value. Improper e-waste disposal poses environmental and health risks, entailing substantial remediation and healthcare costs. Large efforts are applied for the recovery of Au from e-waste using complex processes which include the dissolution of Au, its adsorption in an ionic state and succeeding reduction to metallic Au. These processes themselves being complex and utilizing harsh chemicals contribute to the environmental impact of e-waste. Here, we present an approach for the simultaneous recovery and reduction of Au3+ and Au+ ions from e-waste to produce solid Au0 forms, thus skipping several technological steps. We develop a nanoscale cross-dimensional composite material via self-assembly of two-dimensional graphene oxide and one-dimensional chitosan macromolecules, capable of acting simultaneously as a scavenger of gold ions and as a reducing agent. Such multidimensional architecture doesn't require to apply any voltage for Au adsorption and reduction and solely relies on the chemisorption kinetics of Au ions in the heterogeneous GO/CS nanoconfinements and their chemical reduction on multiple binding sites. The cooperative phenomena in ionic absorption are responsible for the extremely high efficiency of gold extraction. The extraction capacity reaches 16.8 g/g for Au3+ and 6.2 g/g for Au+, which is ten times larger than any existing gold adsorbents can propose. The efficiency is above 99.5 wt.% (current limit is 75 wt.%) and extraction ability is down to very low concentrations of 3 ppm.

Ammonium-ion thermal charging supercapacitors for low-grade heat conversion and storage

Thermal charging supercapacitors capable of heat conversion and storage have emerged as a cutting-edge technology for efficiently utilizing low-grade heat. However, the sluggish kinetics of the insertion ions have hindered their thermoelectric performance and practical applications. Herein, we design a novel thermal charging supercapacitor utilizing the reversible insertion/thermo-extraction of NH4+ into/from the V2O5 microflowers, achieving efficient heat-to-electric conversion and storage. Benefiting from the fast diffusion of NH4+ and the micro-nanostructure of the V2O5 cathode, a high thermopower of 12.34 mV K−1 is obtained. Furthermore, an impressive heat-to-electric conversion and storage performance is also demonstrated in the quasi-solid-state ammonium-ion thermal charging supercapacitors (ATSCs). Integrating thermodiffusion with thermoextraction effects, the ATSCs exhibit a high thermopower of 9.78 mV K−1 and an output power density of 12.5 μW cm−2, confirming the potential of NH4+ as an insertion ion in the thermal charging supercapacitor applications.

Role of Ion Dynamics in Electron‐Only Magnetic Reconnection

AbstractStandard magnetic reconnection couples with both ions and electrons on different scales. Recently, a new type of magnetic reconnection, electron‐only reconnection without the coupling of ions, has been observed in various plasma environments. Standard reconnection typically has a reconnection outflow velocity of about one Alfvén speed. According to the scaling analysis, the electron outflow velocity is expected to be about one electron Alfvén speed in electron‐only reconnection. However, observations and simulations both find that the electron outflows are much slower than the electron Alfvén speed. In this letter, by performing two‐dimensional particle‐in‐cell simulations, we show that this is because ions play a role in electron‐only reconnection. The ions move slower than the electrons in the outflow direction, and such charge separation forms an in‐plane Hall electric field, which prevents the electrons from being accelerated to the electron Alfvén speed in electron‐only reconnection.

Effect of stress and irradiation fluence on latent track formation in swift heavy ion irradiation: A case study on TiO2

Swift Heavy Ions (SHI) irradiation, characterized by high kinetic energy ions, induces significant material/structural modification, e.g., latent track. However, the intricate interaction among various physics, i.e., mechanical stress, phase transition, and heat transfer, has been ignored in the continuum-based approaches in favor of simplicity. Here, we developed a two-dimensional coupled phase-field inelastic-thermal spike (PF-iTS) model to investigate the effect of thermal cross-talk, elastic energy, and irradiation fluence on latent track formation and size. The results reveal a shift in the critical electronic stopping energy and a reduced track radius under mechanical stress. Additionally, the study demonstrates the impact of thermal cross-talk between incidents, i.e., simultaneous and delayed double ion impacts, showing potential track merging and variations in track morphology.

Ionic conduction and cathodic properties of CaMO3 (M=Fe and Mn) electrode materials via molecular dynamics and first-principles simulations

Calcium-ion(Ca-ion) batteries are gaining ever-increasing attention for next-generation energy storage systems due to affordability, highly abundant, high energy density, high theoretical capacity, and low redox potential close to Li-ion. In this work, we deployed the first-principles and classical molecular dynamics simulations to investigate the electronic and diffusive properties of isostructural ternary perovskite CaMO3 (M= Fe and Mn). The transport properties at various temperatures from ion dynamics and electronic properties of CaMO3 perovskites are examined using classical molecular dynamics and quantum mechanical simulations, respectively. We present the microscopic origin of the diffusion of multivalent ions like Ca2+ within the crystal structure of perovskite material and the effects of two transition metals, manganese and iron. Dynamic studies of Ca-ions were performed using molecular dynamic simulation, which depicts the diffusivity and conductivity of Ca-ion in CaMO3 material. We find that the diffusivity in both the crystals increases with temperature; as a result, conductivity increases. Among both the crystals, CaFeO3 requires less activation energy for diffusion and ionic conduction than CaMnO3. Using density functional theory, we calculated specific capacity, electronic density of states, phase stability and equilibrium cell voltage, and charge transfer process during intercalation-deintercalation from first-principles calculations. The electronic behavior of these materials shows that CaFeO3 has better electronic and transport properties than CaMnO3.

Local electronic structure modulation via S substitution enables fast-discharging capability for Li-rich Mn-based oxides cathodes

Anionic and cationic redox reaction contribute to the ultrahigh specific capacities of Li-rich Mn-based oxides cathodes (LMNC). However, the irreversible oxygen evolution and sluggish kinetics result in the continuous capacity decay and poor rate performance, which limited its application as cathode material in lithium-ion batteries. Herein, the local electronic structure of LMNC is appropriately modulated via S2− doping to alleviate oxygen release, stabilize the crystal structure stability, and facilitate Li+ diffusion via facile surface defect engineering. The effect of S2− doping site on the systematically energy is investigated by DFT. Under the guidance of this result, LNMC-S is prepared by co-precipitation and high-temperature solid-phase reaction method. The effect of doping concentration on electrochemical property of LMNC was systematically investigated. The results exhibit that S2− doping can effectively suppress the electronic insulation of Li2MnO3, enhance the transport dynamics of lithium ion and inhibit the phase transition of LMNC sample during charge-discharge process. Thereby, the modified sample exhibits superior electrochemical property, such as the 200th discharge capacity is 184.3 mAh·g−1 under 1C, with a capacity retention rate of 87.6 %. This paper is beneficial for enriching the existing theoretical findings and discoveries, providing theoretical guidance for the preparation of high-performance material.

Ultrafast X-ray laser-induced explosion: How the depth influences the direction of the ion trajectory

Single particle imaging using X-ray lasers is a technique aiming to capture atomic resolution structures of biomolecules in their native state. Knowing the particle's orientation during exposure is crucial for method enhancement. It has been shown that the trajectories of sulfur atoms in a Coulomb exploding lysozyme are reproducible, providing orientation information. This study explores if sulfur atom depth influences explosion trajectory. Employing a hybrid collisional-radiative/molecular dynamics model, we analyze the X-ray laser-induced dynamics of a single sulfur ion at varying depths in water. Our findings indicate that the ion spread-depth relationship depends on pulse parameters. At a photon energy of 2 keV, high-charge states are obtained, resulting in an increase of the spread with depth. However, at 8 keV photon energy, where lower charge states are obtained, the spread is essentially independent with depth. Finally, lower ion mass results in less reproducible trajectories, opening a promising route for determining protein orientation through the introduction of heavy atoms.

Construction of iodine-rich solid electrolyte interphase to achieve highly stable aqueous zinc-ion batteries

Aqueous zinc ion batteries (AZIBs) are considered highly potential secondary energy storage equipment for their higher energy density, lower risk, and affordability. However, parasitic reactions within the anode affect the Zn2+ deposition behavior with uncontrollable dendrite formation significantly shortening the battery lifetime. For improvement of the Zn anode cycling stability, tetraethylammonium iodide (TEAI), a multifunctional additive was introduced into ZnSO4, which constructs an iodine-rich solid electrolyte interphase (SEI) on the zinc anode surface and significantly inhibits the parasitic reactions and nucleation of zinc dendrites. Furthermore, the TEAI also reshapes the solvation sheath of Zn2+, contributing to better transportation kinetics of zinc ions. Attributing to these functions, highly stable AZIBs are realized with the addition of TEAI, in which a stable cycling life of over 3500 h was achieved for symmetric Zn//Zn batteries under 1 mA cm-2. With higher current densities, the battery also exhibited excellent cycling stability over 3500 h. Full cells with the V2O5 cathode were fabricated to examine the commercial availability of TEAI additives, achieving a high reversible discharge capacity of 381 mAh g-1, and the capacity of 102 mAh g-1 was still maintained after 800 cycles at 1 A g-1.