Electric Field Gradient Research Articles

Lithium Anode Stability Enhanced by Micro-Potentials from Spontaneous Polarization in BaTiO3 Films

Lithium metal is widely recognized as an ideal anode material due to its high specific capacity and low redox potential. However, challenges such as severe lithium dendrite growth have significantly impeded its practical applications. Herein, we introduce a BaTiO3 (BTO) ferroelectric thin film into the lithium anode. During the charge/discharge cycles, the BTO film generates a micro-potential in the direction opposite to the applied electric field, owing to its spontaneous polarization. The micro-potential effectively reduces the electric field gradient, thereby suppressing inhomogeneous nucleation and the growth of lithium dendrites. Consequently, the incorporation of the BTO ferroelectric thin film significantly enhances the cycling performance of the batteries. The half cells demonstrate stable operation after more than 100 cycles at high capacity of 4 mAh·cm−2. Furthermore, the LiFePO4 (LFP) full cell delivers a specific capacity of 146.6 mAh·g−1 after 300 cycles. This work demonstrates a promising strategy for the development of lithium batteries with improved longevity and enhanced capacity.

Advances in Design and Fabrication of Micro-Structured Solid Targets for High-Power Laser-Matter Interaction

Accelerated particles have multiple applications in materials research, medicine, and the space industry. In contrast to classical particle accelerators, laser-driven acceleration at intensities greater than 1018 W/cm2, currently achieved at TW and PW laser facilities, allow for much larger electric field gradients at the laser focus point, several orders of magnitude higher than those found in conventional kilometer-sized accelerators. It has been demonstrated that target design becomes an important factor to consider in ultra-intense laser experiments. The energetic and spatial distribution of the accelerated particles strongly depends on the target configuration. Therefore, target engineering is one of the key approaches to optimizing energy transfer from the laser to the accelerated particles. This paper provides an overview of recent progress in 2D and 3D micro-structured solid targets, with an emphasis on fabrication procedures based on laser material processing. Recently, 3D laser lithography, which involves Two-Photon Absorption (TPA) effects in photopolymers, has been proposed as a technique for the high-resolution fabrication of 3D micro-structured targets. Additionally, laser surface nano-patterning followed by the replication of the patterns through molding, has been proposed and could become a cost-effective and reliable solution for intense laser experiments at high repetition rates. Recent works on numerical simulations have also been presented. Using particle-in-cell (PIC) simulation software, the importance of structured micro-target design in the energy absorption process of intense laser pulses—producing localized extreme temperatures and pressures—was demonstrated. Besides PIC simulations, the Finite-Difference Time-Domain (FDTD) numerical method offers the possibility to generate the specific data necessary for defining solid target material properties and designing their optical geometries with high accuracy. The prospects for the design and technological fabrication of 3D targets for ultra-intense laser facilities are also highlighted.

Water compression induced ionic negative differential resistance in nanopores.

The mass transport behavior through nanoscale channels, greatly influenced by the structures and dynamics of nanoconfined water, plays an essential role in many biophysical processes. However, the dynamics of nanoconfined water under an external field and its effects are still not fully understood. Here, on the basis of molecular dynamics simulations, we theoretically show that the ionic current of [Bmim][PF6] through narrow pores in graphene membrane exhibits an ionic negative differential resistance effect-the ionic current decreases as the voltage increases over a certain threshold. This effect arises from the violation of traditional fluid dynamics as the assumption of continuity and homogeneity of fluids is no longer effective in ultrathin nanopores. The gradient of electric field around the atomic-thin layer produces a strong gradient force on the polarized water inside the nanopore. This dielectrophoretically compressed water leads to a hydrostatic force that repels ions from entering the nanopore. Our findings may advance the understanding of hydrostatic mechanism, which governs ion transport through nanopores.

Long range self-transport of liquid droplets driven by electric field and roughness gradient

It is well known that roughness and charge gradients could be used for droplet self-transport. The key issue is how to synergize the two effects. The uniform density charge can form linearly increasing charge gradient on a roughness gradient surface. Under this condition, the influence on the droplet self-transport under the synergy of these two effects was obtained by statics analysis, and the driving function was presented. An energy equation was constructed to study the conditions for crossing periodic boundaries, and the problem of distance limitation on periodic surfaces due to energy dissipation was solved by converting electric potential into droplet kinetic energy. A periodic roughness gradient surface with K = 0.07 was designed and prepared via 3D printing. Water droplets can be transported over long distances and the maximum velocity increases with charge density up to 46 mm/s. Finally, the effect of different structures on the maximum charge density in the Cassie state was investigated by simulation. The biomimetic structures exhibit great compressive stability, which can increase the surface charge density of droplets in the Cassie state by 3.6 times compared to pillar structures. It can be widely used in the fields of materials science and interface chemistry, etc.

Protoporphyrin IX iron(II) revisited. An overview of the Mössbauer spectroscopic parameters of low-spin porphyrin iron(II) complexes.

Mössbauer parameters of low-spin six-coordinate [Fe(II)(Por)L2] complexes (where Por is a synthetic porphyrin; L is a nitrogenous aliphatic, an aromatic base or a heterocyclic ligand, a P-bonding ligand, CO or CN) and low-spin [Fe(Por)LX] complexes (where L and X are different ligands) are reported. A known point charge calculation approach was extended to investigate how the axial ligands and the four porphyrinato-N atoms generate the observed quadrupole splittings (ΔEQ) for the complexes. Partial quadrupole splitting (p.q.s.) and partial chemical shifts (p.c.s.) values were derived for all the axial ligands, and porphyrins reported in the literature. The values for each porphyrin are different emphasising the importance/uniqueness of the [Fe(PPIX)] moiety, (which is ubiquitous in nature). This new analysis enabled the construction of figures relating p.c.s and p.q.s values. The relationships presented in the figures indicates that strong field ligands such as CO can, and do change the sign of the electric field gradient in the [Fe(II)(Por)L2] complexes. The limiting p.q.s. value a ligand can have and still form a six-coordinate low-spin [Fe(II)(Por)L2] complex is established. It is shown that the control the porphyrin ligands exert on the low-spin Fe(II) atom limits its bonding to a defined range of axial ligands; outside this range the spin state of the iron is unstable and five-coordinate high-spin complexes are favoured. Amongst many conclusions, it was found that oxygen cannot form a stable low-spin [Fe(II)(Por)L(O2)] complex and that oxy-haemoglobin is best described as an [Fe(III)(Por)L(O2-)] complex, the iron is ferric bound to the superoxide molecule.

Ionic selectivity of nanopores: Comparison among cases under the hydrostatic pressure, electric field, and concentration gradient

The ionic selectivity of nanopores is crucial for the energy conversion based on nanoporous membranes. It can be significantly affected by various parameters of nanopores and the applied fields driving ions through porous membranes. Here, with finite element simulations, the selective transport of ions through nanopores is systematically investigated under three common fields, i.e. the electric field (V), hydrostatic pressure (p), and concentration gradient (c). For negatively charged nanopores, through the quantitative comparison of the cation selectivity (t+) under the three fields, the cation selectivity of nanopores follows the order of t+V > t+c > t+p. This is due to the transport characteristics of cations and anions through the nanopores. Because of the strong transport of counterions in electric double layers under electric fields and concentration gradients, the nanopore exhibits a relatively higher selectivity to counterions. We also explored the modulation of t+ on the properties of nanopores and solutions. Under all three fields, t+ is directly proportional to the pore length and surface charge density, and inversely correlated to the pore diameter and salt concentration. Under both the electric field and hydrostatic pressure, t+ has almost no dependence on the applied field strength or ion species, which can affect t+ in the case of the concentration gradient. Our results provide detailed insights into the comparison and regulation of ionic selectivity of nanopores under three fields which can be useful for the design of high-performance devices for energy conversion based on nanoporous membranes.

Synergistic Gradient Anodes for Long-Term Stability in Aqueous Zinc-Ion Batteries.

The stability of aqueous zinc metal anodes is still constrained by their severe dendrite growth. Optimizing electric field distribution and crystallography to modulate the diffusion and deposition behavior of zinc ions can effectively suppress dendrite growth. However, the fabrication strategy to directly endow specific textured zinc anodes with gradient electric field distribution is still lacking. Herein, a strategy combining crystal reconstruction of commercial zinc foil with graphene oxide (GO) protective layer is proposed to construct an in situ gradient electric field-enhanced strong (002) textured GO@ZnO/Zn(002) anode. Based on the experimental and theoretical results, the GO protective layer can regulate a wide-range homogeneous Zn2+ ions flow, while the dense and uniform ZnO/Zn(002) nanoneedles /nanoparticles can enhance localized polarized electric field to accelerate rapid localized transfer of Zn2+ ions and guide them toward directional deposition along (002) plane. Therefore, the hierarchical GO@ZnO/Zn(002) anode enables the symmetric cell to operate continuously and stably for 5700 and 4200h at 2 and 4mA cm-2, respectively, which is comparable to or better than most high-end Zn anodes. This work presents new insights into the zinc foil reconstruction and gradient electric field fabrication strategy, offering a scalable approach for the development of long-term stable metal anodes.

Analytical model for flexoelectric sensing of structural response considering bonding compliance

Flexoelectricity has generated huge interest as an alternative to piezoelectricity for developing electromechanical systems such as actuators, sensors, and energy harvesters. This article presents a generic theoretical framework for the sensing mechanism of a flexoelectric sensor bonded to a host beam through an adhesive layer. The model incorporates piezoelectric and flexoelectric effects and considers both shear-lag and peel stresses at the sensor-beam interface. The formulation also includes the electric field gradient terms that are often overlooked. Consistent one-dimensional constitutive relations and governing equations of equilibrium are derived from the electric Gibb’s energy density function and extended Hamilton’s principle. The sensor is assumed to follow the Euler–Bernoulli beam-type membrane and bending deformation behaviour. Closed-form solutions are obtained for the interfacial stresses by analytically solving a seventh-order non-homogeneous ordinary differential equation, satisfying the stress-free boundary conditions at the sensor edges. The induced electric potential at the sensor top is derived by solving a fourth-order differential equation obtained from the charge balance equation, satisfying the electric boundary conditions. For validation, the sensor output is compared with the results of the existing non-rigid bonding piezoelectric sensor model. Numerical results show a significant impact of non-rigid bonding and the electric field gradient terms on the induced electric potential. Further, the importance of bonding compliance on the interfacial stress distributions is illustrated. Finally, the effects of adhesive and transducer thicknesses on the peak amplitudes of interfacial stresses and sensory potential are presented.

Geometry of the argon…imidazole complex revealed by the microwave spectra of four isotopologues

The rotational spectra of four isotopologues of an isolated complex formed between an argon atom and imidazole, Ar…imidazole, have been recorded in the 6–19 GHz region by Fourier transform microwave spectroscopy. Rotational transition frequencies have been fitted to Watson’s S-reduced Hamiltonian to yield rotational, centrifugal distortion and nuclear quadrupole coupling constants for the complex. Rotational constants determined for the parent and three 15N-containing isotopologues allow the three-dimensional structure of the complex to be described. The two angles, θ and ϕ, which define the orientation of the Ar atom relative to the imidazole ring have been determined for the first time in addition to the distance between Ar and the center of mass of the imidazole sub-unit, R. Fitting of structural parameters to the experimentally-determined moments of inertia yields a structure where Ar is positioned above the ring plane at a distance of 3.519 Å from the center of mass of the imidazole sub-unit. In the experimentally determined, average geometry, the intermolecular axis (drawn through Ar and the center of mass of the imidazole sub-unit) is oriented at 6° from the normal to the ring plane. The experimental results allow for four alternative possibilities for ϕ with 62.0(39)° being that which is most consistent with expectations for this parameter based on previous work. The experimentally-determined nuclear quadrupole coupling constants imply that the electric field gradient at each of the nitrogen nuclei of imidazole does not significantly change on formation of the complex with Ar.

Modulating the fracture behavior of interface cracks via electric field gradient in flexoelectric solids

Interface cracks seriously affect the performance and service life of layered electronic devices. At nanoscale, the electric field concentration can be generated at the tip of insulating cracks by solely applying a uniform electric field loading, resulting in a large electric field gradient and thus inducing a significant converse flexoelectric effect. The deformation generated by the converse flexoelectric effect is expected to achieve crack shielding, however, its mechanism is still not clear. In this paper, the role of electric field gradients on interface crack behavior is studied by the collocation mixed finite element method (MFEM) and the J-integral. The result shows that the electric field gradient generated by a uniform electric displacement loading can reduce the J-integral of crack tips, achieving crack shielding. The result provides new ideas for the study of failure assessment, nanoscale fracture experiment and others.

The Difference between Traditional Magnetic Stimulation and Microcoil Stimulation: Threshold and the Electric Field Gradient

This paper considers the threshold value of the activating function needed for stimulation in traditional magnetic stimulation and microcoil stimulation. Two analyses of excitation have been studied: spatial frequency analysis and active membrane analysis using the Hodgkin−Huxley model. The activating function depends on the spatial distribution of the electric field gradient in the active membrane analysis and the spatial frequency in the spatial frequency analysis. Both analyses show that a microcoil (tens of microns in size) has a higher threshold than a traditional coil (tens of millimeters in size) when the spatial frequency is large or the spatial extent of the activating function is small. Consequently, the stimulation threshold for a microcoil is much higher than that for a conventional coil.

Heteronanotrimers by Selective Photodeposition of Gold Nanodots on Janus-Type Cu2‒ xS/CuInS2 Heteronanocrystals.

This study focuses on the development of environmentally friendly Au-Cu2-xS/CuInS2 heteronanotrimers. The chosen strategy relies on the laser photodeposition of a single gold nanodot (ND) onto Janus Cu2- xS/CuInS2 heteronanocrystals (HNCs). This method offers precise control over the number, location, and size (5 to 8nm) of the Au NDs by adjusting laser power for the career production, concentration of hole scavenger for charge equilibration in redox reactions, and gold precursor concentration, and exposure time for the final ND size. The photoreduction of gold ions onto HNCs starts systematically at the Cu2- xS tip. The Au deposition then depends on the CuInS2 segment length. For short HNCs, stable Au-Cu2- xS/CuInS2 heteronanotrimers form, while long HNCs undergo a secondary photo-induced step: the initial Au ND is progressively oxidized, with concomitant deposition of a second gold ND on the CuInS2 side, to yield Au2S-Cu2- xS/CuInS2-Au heteronanotrimers. Results are rationalized by quantitative comparison with a model that describes the growth kinetics of NDs and Au-Cu2- xS transformation and emphasizes the importance of charge separation in predicting selective deposition in heteronanotrimer production. The key parameter controlling Au-Cu2‒ xS/CuInS2 HNCs is the photoinduced electric field gradient generated by charge separation, which is tailored by controlling the CuInS2 segment size.

Emergence and transformation of polar skyrmion lattices via flexoelectricity

As analogies to magnetic skyrmions, polar skyrmions in ferroelectric superlattices and multilayers have garnered widespread attention for their non-trivial topology and novel properties like negative capacitance and nonlinear optical effect. So far, they have only been theoretically predicted to be able to assemble ordered hexagonal skyrmion lattices (SkLs) in ferroelectric thin films. Here, based on phase-field simulations, we report the critical roles of flexoelectricity playing in the stabilization and transformation of polar SkLs. Different polar SkL patterns can emerge in the ferroelectric thin films, including tetragonal-SkL, and hexagonal-SkLs with diverse orientations, as summarized by phase diagrams. These emergent SkL states are attributed to the material anisotropy modified by the flexoelectric effect. Interestingly, we further found that the hexagonal-SkLs can be rotated by applying strain gradient or in-plane electric field to the films. Moreover, a nonreciprocal bending response of tetragonal-SkL is also induced by the flexoelectric effect. Our results provide useful guidelines for the implementation of polar skyrmion lattices in experiments.

Electrokinetic particle trapping in microfluidic wells using conductive nanofiber mats.

The frequency dependence of electrokinetic particle trapping using large-area (>mm2) conductive carbon nanofiber (CNF) mat electrodes is investigated. The fibers provide nanoscale geometric features for the generation of high electric field gradients, which is necessary for particle trapping via dielectrophoresis (DEP). A device was fabricated with an array of microfluidic wells for repeated experiments; each well included a CNF mat electrode opposing an aluminum electrode. Fluorescent microspheres (1µm) were trapped at various electric field frequencies between 30kHz and 1MHz. Digital images of each well were analyzed to quantify particle trapping. DEP trapping by the CNF mats was greater at all tested frequencies than that of the control of no applied field, and the greatest trapping was observed at a frequency of 600kHz, where electrothermal flow is more significantly weakened than DEP. Theoretical analysis and measured impedance spectra indicate that this result was due to a combination of the frequency dependence of DEP and capacitive behavior of the well-based device.

Machine learning assisted mechanism modeling for gas phase electrohydrodynamic system

In this paper, a hybrid physics-data driven model for electrohydrodynamic gas system (EHDGS) was developed by combining artificial neural network (ANN) with mechanism modeling method. ANN was used to correlate the relationship between the variables (electrode distance, diameter of grounding cylinder, applied voltage, electric field gradient, etc.) in a needle-cylinder EHDGS and the initial space charge density. The results showed that the ANN model of nine neurons can well predict the initial space charge density. The coefficient of determination (R2) reaches 0.9874, and the mean absolute error is as low as 0.0067. Subsequently, a hybrid mechanism model where the initial space charge density was predicted from the ANN model was constructed to simulate the needle-cylinder EHDGS. The experiment with the needle-cylinder EHDGS was carried out. The simulation results were in good agreement with the experimental data, demonstrating the reliability of the proposed hybrid model. The electric field distribution, space charge distribution, and flow field distribution behavior of the EHDGS were then analyzed in detail. The effects of key parameters on the flow characteristics of EHDGS were systematically studied, showing that higher voltage and shorter distance give higher flow rate up to 2.5 m/s. The diameter of the cylinder also significantly influences the breakdown voltage. Three dimensionless groups were defined and their effects on spatial charge density distribution were investigated. This study provides both insights and an efficient tool for the design and optimization of EHDGS.

Single Molecule Thermodynamic Penalties Applied to Enzymes by Whispering Gallery Mode Biosensors.

Optical microcavities, particularly whispering gallery mode (WGM) microcavities enhanced by plasmonic nanorods, are emerging as powerful platforms for single-molecule sensing. However, the impact of optical forces from the plasmonic near field on analyte molecules is inadequately understood. Using a standard optoplasmonic WGM single-molecule sensor to monitor two enzymes, both of which undergo an open-to-closed-to-open conformational transition, the work done on an enzyme by the WGM sensor as atoms of the enzyme movethrough the electric field gradient of the plasmonic hotspot during conformational change has been quantified. As the work done by the sensor on analyte enzymes can be modulated by varying WGM intensity, the WGM microcavity system can be used to apply free energy penalties to regulate enzyme activity at the single-molecule level. The findings advance the understanding of optical forces in WGM single-molecule sensing, potentially leading to the capability to precisely manipulate enzyme activity at the single-molecule level through tailored optical modulation.

Influence of Sr doping on the structural and magnetic properties of (Y,Gd)Ba[formula omitted]Sr[formula omitted]CuFeO[formula omitted] ([formula omitted]) studied by FTIR and 57Fe Mössbauer spectroscopy

The effect of replacing Y by Gd and Ba by Sr in YBaCuFeO5 is studied by Fourier Transform Infrared spectroscopy, 57Fe Mössbauer spectroscopy and DC susceptibility measurements. Site disorder is inferred from FTIR and Mössbauer spectra using a Maximum-Entropy-Method. A doping dependence of the IR peaks and the hyperfine parameters is explained in terms of bonding energies and electric field gradient variations in the crystal lattice caused by Fe/Cu site disorder. We find an influence of doping on the structural and magnetic properties through a correlation of hyperfine parameters such as the electric quadrupole splitting and the magnetic hyperfine field. We also find that a paramagnetic volume fraction appears for GdBaCuFeO5 that increases upon Sr doping at the Ba site. The different behavior of the susceptibility upon replacing Y by Gd is attributed to the lack of a favorable environment to enable a Gd-Fe or Gd-Cu exchange interaction.

TENG-driven single-droplet green electrochemical etching and deposition for chemical sensing applications

Selected area electrochemical etching (EE) and electrochemical deposition (ED) are widely used for fabricating microstructures and devices, but they require complex processes and expensive equipment and generate significant electrolyte waste. This study demonstrates a novel single-droplet electrochemical system using a triboelectric nanogenerator (TENG) for self-powered selected area EE and ED reactions. Utilizing TENG's pulsed power, Al nanostructures were created by EE, while nano-Ag and Cu2O nanocubes were synthesized by ED. The generated nanomaterials were applied to detect trace chemicals through the Surface-Enhanced Raman Scattering effect. The electrochemical reaction area can be controlled by droplet size, and patterns can be created using a needle movement platform. The size and density of nanostructures can be adjusted by the TENG's current, collision frequency, and electrolyte concentration. The deposition gradient from the center to the edge of the droplet is controlled by the distance between the needle and the substrate. COMSOL Multiphysics calculations show that a smaller D creates a larger electric field gradient. However, the varied deposition gradients were attributed to competition of electric field, diffusion effects, and capillary flow. This proposed green technology offers low cost, simplicity, no waste electrolyte, and self-powering capabilities, pioneering new research directions in EE and ED.

Recent Advances in Dielectrophoretic Manipulation and Separation of Microparticles and Biological Cells.

Dielectrophoresis (DEP) is an advanced microfluidic manipulation technique that is based on the interaction of polarized particles with the spatial gradient of a non-uniform electric field to achieve non-contact and highly selective manipulation of particles. In recent years, DEP has made remarkable progress in the field of microfluidics, and it has gradually transitioned from laboratory-scale research to high-throughput manipulation in practical applications. This paper reviews the recent advances in dielectric manipulation and separation of microparticles and biological cells and discusses in detail the design of chip structures for the two main methods, direct current dielectrophoresis (DC-DEP) and alternating current dielectrophoresis (AC-DEP). The working principles, technical implementation details, and other improved designs of electrode-based and insulator-based chips are summarized. Functional customization of DEP systems with specific capabilities, including separation, capture, purification, aggregation, and assembly of particles and cells, is then performed. The aim of this paper is to provide new ideas for the design of novel DEP micro/nano platforms with the desired high throughput for further development in practical applications.

First-principle study of the ground-state crystal structure and optoelectronic response of CsPbX3 (X= Cl, Br, I) for photovoltaic applications

The optoelectronic response and ground state crystal structure of tetragonal (P4/mbm), orthorhombic (Pmnb) and monoclinic (P21/m) phases of CsPbX3 (X = Cl, Br, I) are studied for optoelectronic applications using first principle simulations. Electric field gradient (EFG) and magnetic hyperfine interactions are investigated to explore the charge distributions surrounding the nucleus and local magnetic environment of the atomic nucleus. The orthorhombic phase of these compounds is more stable having lowest ground-state energy compared to tetragonal and monoclinic phases. The understudied halide perovskites have direct band gap nature and spin orbit coupling (SOC) effect splits Pb-p and X-p orbitals at the edges of conduction and valence band (CB and VB) respectively. At the edge of VB, the strongly hybridized X-p and Pb-p orbital and direct band gap nature of CsPbX3 is excellent for the light absorption and photovoltaic (PV) applications. The n-i-p configuration (FTO/ETL/CsPbX3/HTL/Au) of the simulated structure shows that CsPbI3 has improved power conversion efficiency (PCE) of 22.48 % and 22.32 % and quantum efficiency (QE) about ∼80 % in tetragonal and monoclinic phases respectively. The Pb and Cs values of EFG tensor in z-direction (Vzz) are close to each other, which show that the distribution of electronic charge density is similar near these nuclei. Moreover, Cs-s orbital has negligible contribution and Pb-p and I-p orbitals have higher contribution in the hyperfine field (HFF). The negative HFF indicates the opposite HFF contribution.