Free Charge Research Articles

A novel ballistic model for the subthreshold behavior of nanosheet transistors

A novel ballistic model for the subthreshold current of nanosheet transistors is successfully developed based on the Landauer approach with the three-dimensional number of channels. The ballistic threshold voltage can also be achieved through the calculated free charge density induced by the three-dimensional density-of-states equal to the substrate doping concentration. It indicates that under the low drain voltage corresponding to the Fermi distribution function, the subthreshold current is mainly governed by the low contact potential. However, under the high drain voltage corresponding to the Fermi distribution function, the thermal voltage, instead of the contact potential between the source and drain, initiates the subthreshold current. Besides subthreshold current and threshold voltage, the ballistic conductance and subthreshold swing are also revealed in the subthreshold conduction. It indicates that the thin silicon, thin gate oxide, heavy substrate doping density, and high work function will alleviate the ballistic effects, decrease the subthreshold current/swing, and increase the threshold voltage/ballistic resistance.

Delocalizing Excitation for Highly-Active Organic Photovoltaic Catalysts.

Localized excitation in traditional organic photocatalysts typically prevents the generation and extraction of photo-induced free charge carriers, limiting their activity enhancement under illumination. Here, we enhance delocalized photoexcitation of small molecular photovoltaic catalysts by weakening their electron-phonon coupling via rational fluoro-substitution. The optimized 2FBP-4F catalyst we develop here exhibits a minimized Huang-Rhys factor of 0.35 in solution, high dielectric constant and strong crystallization in the solid state. As a result, the energy barrier for exciton dissociation is decreased, and more importantly, polarons are unusually observed in 2FBP-4F nanoparticles (NPs). With the increased hole transfer efficiency and prolonged charge carrier lifetime highly related to enhanced exciton delocalization, the PM6 : 2FBP-4F heterojunction NPs at varied concentration exhibit much higher optimized photocatalytic activity (207.6-561.8 mmol h-1 g-1) for hydrogen evolution than the control PM6 : BP-4F and PM6 : 2FBP-6F NPs, as well as other reported photocatalysts under simulated solar light (AM 1.5G, 100 mW cm-2).

Delocalizing Excitation for Highly‐Active Organic Photovoltaic Catalysts

AbstractLocalized excitation in traditional organic photocatalysts typically prevents the generation and extraction of photo‐induced free charge carriers, limiting their activity enhancement under illumination. Here, we enhance delocalized photoexcitation of small molecular photovoltaic catalysts by weakening their electron‐phonon coupling via rational fluoro‐substitution. The optimized 2FBP‐4F catalyst we develop here exhibits a minimized Huang–Rhys factor of 0.35 in solution, high dielectric constant and strong crystallization in the solid state. As a result, the energy barrier for exciton dissociation is decreased, and more importantly, polarons are unusually observed in 2FBP‐4F nanoparticles (NPs). With the increased hole transfer efficiency and prolonged charge carrier lifetime highly related to enhanced exciton delocalization, the PM6 : 2FBP‐4F heterojunction NPs at varied concentration exhibit much higher optimized photocatalytic activity (207.6–561.8 mmol h−1 g−1) for hydrogen evolution than the control PM6 : BP‐4F and PM6 : 2FBP‐6F NPs, as well as other reported photocatalysts under simulated solar light (AM 1.5G, 100 mW cm−2).

Insights into nitrogen-doped BiOBr with oxygen vacancy and carbon quantum dots photocatalysts for the degradation of sulfonamide antibiotics: Actions to promote exciton dissociation and carrier migration

The strong excitonic effect significantly influences the efficiency of electron-hole pair generation. Therefore, promoting the dissociation of excitons into free charge carriers has drawn much attention. In this study, nitrogen (N)-doped BiOBr photocatalyst (BOBNC) modified with carbon quantum dots (CQDs) was synthesized via a solvothermal method. We demonstrated through photoluminescence and photoelectrochemical techniques the synergistic effect of oxygen vacancies and CQDs, facilitating exciton dissociation and charge carrier migration, consequently significantly enhancing the electron density in the material. Compared to pure BiOBr, degradation experiments revealed that the optimized doping ratio of 0.5BOBNC with CQDs increased the rate constant for sulfamethoxazole (SIZ) by 19.89 times. Furthermore, based on quenching experiments, electron spin resonance (ESR) tests, and DFT calculations, h+, O2•− and 1O2 were identified as the primary reactive species for SIZ degradation, and a photocatalytic mechanism was proposed. Additionally, the influence of various environmental factors on the photocatalytic system was investigated. In conclusion, this work not only contributes to a profound understanding of BiOBr exciton dissociation but also presents a promising photocatalytic technique for the remediation of diverse water environments.

Dipole momenta and compositeness of the τ lepton at Belle II

The large number of τ leptons available at the Belle II experiment makes it possible to study their properties and the extent of their compositeness. We propose a strategy that relies on three observables defined in terms of elements of the polarization density matrix of the produced τ pairs, which we obtain via quantum tomography. We find that these observables can explore values of the magnetic dipole moment down to 6.3×10−4, which is 2 orders of magnitude better than the current experimental limit, constrain the electromagnetic radius below 4.3×10−3 fm, and exclude an electric dipole moment larger than 1.7×10−17 e cm. The quoted limits are at the 95% confidence level (CL) and are obtained for a benchmark integrated luminosity of 1 ab−1 and a Monte Carlo estimate of the statistical sensitivity. Published by the American Physical Society 2024

Analysis of the Polarization Distribution and Spin Angular Momentum of the Interference Field Obtained by Co-Planar Beams with Linear and Circular Polarization

Interference of two and four light beams with linear or circular polarization is studied analytically and numerically based on the Richards–Wolf formalism. We consider such characteristics of the interference fields as the distribution of intensity, polarization, and spin angular momentum density. The generation of light fields with 1D and 2D periodic structure of both intensity and polarization is demonstrated. We can control the periodic structure both by changing the polarization state of the interfering beams and by changing the numerical aperture of focusing. We consider examples with a basic configuration, as well as those with a certain symmetry in the polarization state of the interfering beams. In some cases, increasing the numerical aperture of the focusing system significantly affects the generated distributions of both intensity and polarization. Experimental results, obtained using a polarization video camera, are in good agreement with the simulation results. The considered light fields can be used in laser processing of thin films of photosensitive (as well as polarization-sensitive) materials in order to create arrays of various ordered nano- and microstructures.

Kinetic Evaluation on Lithium Polysulfide in Weakly Solvating Electrolyte toward Practical Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries are highly considered as next-generation energy storage techniques. Weakly solvating electrolyte with low lithium polysulfide (LiPS) solvating power promises Li anode protection and improved cycling stability. However, the cathodic LiPS kinetics is inevitably deteriorated, resulting in severe cathodic polarization and limited energy density. Herein, the LiPS kinetic degradation mechanism in weakly solvating electrolytes is disclosed to construct high-energy-density Li-S batteries. Activation polarization instead of concentration or ohmic polarization is identified as the dominant kinetic limitation, which originates from higher charge-transfer activation energy and a changed rate-determining step. To solve the kinetic issue, a titanium nitride (TiN) electrocatalyst is introduced and corresponding Li-S batteries exhibit reduced polarization, prolonged cycling lifespan, and high actual energy density of 381 Wh kg-1 in 2.5 Ah-level pouch cells. This work clarifies the LiPS reaction mechanism in protective weakly solvating electrolytes and highlights the electrocatalytic regulation strategy toward high-energy-density and long-cycling Li-S batteries.

Excited-State Dynamics of MAPbBr3: Coexistence of Excitons and Free Charge Carriers at Ultrafast Times.

Methylammonium lead tribromide perovskite (MAPbBr3) is an important material, for example, for light-emitting applications and tandem solar cells. The relevant photophysical properties are governed by a plethora of phenomena resulting from the complex and relatively poorly understood interplay of excitons and free charge carriers in the excited state. In this study, we combine transient spectroscopies in the visible and terahertz range to investigate the presence and evolution of excitons and free charge carriers at ultrafast times upon excitation at various photon energies and densities. For above- and resonant band-gap excitation, we find that free charges and excitons coexist and that both are mainly promptly generated within our 50-100 fs experimental time resolution. However, the exciton-to-free charge ratio increases upon decreasing the phonon energy toward resonant band gap excitation. The free charge signatures dominate the transient absorption response for above-band-gap excitation and low excitation densities, masking the excitonic features. With resonant band gap excitation and low excitation densities, we find that although the exciton density increases, free charges remain. We show evidence that the excitons localize into shallow trap and/or Urbach tail states to form localized excitons (within tens of picoseconds) that subsequently get detrapped. Using high excitation densities, we demonstrate that many-body interactions become pronounced and effects such as the Moss-Burstein shift, band gap renormalization, excitonic repulsion, and the formation of Mahan excitons are evident. The coexistence of excitons and free charges that we demonstrate here for photoexcited MAPbBr3 at ultrafast time scales confirms the high potential of the material for both light-emitting diode and tandem solar cell applications.

The effect of different transition metal dopants on the magnetic properties of armchair antimonene, phosphorene, and their binary nanoribbons

Binary antimonene-phosphorene, a novel two-dimensional material with a medium band gap, high carrier mobility, and environmental stability, has attracted growing attention due to its wide applications in spintronics. Using density functional theory, we comprehensively investigate and compare the structural and magnetic properties of armchair Sb, P, and binary SbP nanoribbons doped with 3d transition metal atoms (Ti, Cr, Mn, Fe, Co, and Ni) with various concentrations of dopant atoms. We investigated magnetic properties, including magnetic moment, spin polarization, and spin density. It was found that the magnetic properties for single P and Sb nanoribbons do not depend on the substitution position of TM atoms. In contrast, for binary SbP nanoribbons, the substitution of TM atoms in P or Sb positions leads to different behaviors. For example, the magnetization for substitution of Fe and Co atoms in the P position of the binary SbP nanoribbon will be greater than those of the Sb position, but for other impurity atoms, the magnetization of the binary SbP nanoribbon does not strongly depend on the substitution position. The results show that with increasing the number of impurity atoms in the nanoribbon, the magnetic moment increases, except for the nickel atom in the Sb position of the SbP nanoribbon, in which the nanoribbon prefers the ferrimagnetic state. Also, the spin density results show that the magnetism of the doped systems is mainly attributed to the dopant atoms, and the neighboring atoms have a negligible contribution. The findings of antimonene-phosphorene nanoribbons doped with TM atoms may have potential applications in spintronic nanodevices.

Strain-modulated electronics enabled by surface piezoelectricity

The strain-induced polarization in a piezoelectric semiconductor is an effective strategy to modulate its current transport. However, the piezoelectricity is degraded by the free charges, and the inevitable compromise of piezoelectricity and semiconductivity severely limits the material choice and device performance. We tackle this dilemma by investigating the polarization caused by broken translational symmetry of a material surface. The ubiquitous surface piezoelectricity of solid materials enables the strain-induced polarization change to control the electrical transport effectively in crystals without bulk piezoelectricity. The Schottky barrier is shown to prohibit the bulk charges from screening the surface polarization. The strain engineering of the barrier height leads to an exponential modulation of the current, and an unprecedented gauge factor of 3.10×108 and an on/off ratio of 2.53×105 are demonstrated. The outstanding tunability of current with the synergistic effect of the surface piezoelectricity and metal-semiconductor contact unlocks the device development from various materials.

Effect of preparation conditions on the surface morphology and edge absorption of ZnGa2O4:Cr thin films

Thin ZnGa2O4:Cr films were obtained by RF ion-plasma sputtering in argon and argon-oxygen atmospheres mixtures on single-crystal NaCl and amorphous υ-SiO2 substrates. The surface morphology of the films was studied by atomic force microscopy. It was found that during the annealing of ZnGa2O4:Cr films on υ-SiO2 substrates in oxygen, the grains forming the film grow along the film surface, and during annealing in an argon atmosphere, the growth of grains is observed normal to the film surface. The region of the fundamental absorption edge was studied by optical spectroscopy. The variation of the optical band gap of Eg depending on the deposition and annealing atmosphere was determined. The total effective mass of free charge carriers and the concentration of free charge carriers are estimated. It is shown that the shift of the fundamental absorption edge in ZnGa2O4:Cr thin films after annealing in an argon atmosphere and when oxygen is added to the sputtering atmosphere is due to the Burstein-Moss effect.

Highly efficient microbial inactivation enabled by tunneling charges injected through two-dimensional electronics.

Airborne pathogens retain prolonged infectious activity once attached to the indoor environment, posing a pervasive threat to public health. Conventional air filters suffer from ineffective inactivation of the physics-separated microorganisms, and the chemical-based antimicrobial materials face challenges of poor stability/efficiency and inefficient viral inactivation. We, therefore, developed a rapid, reliable antimicrobial method against the attached indoor bacteria/viruses using a large-scale tunneling charge-motivated disinfection device fabricated by directly dispersing monolayer graphene on insulators. Free charges can be stably immobilized under the monolayer graphene through the tunneling effect. The stored charges can motivate continuous electron loss of attached microorganisms for accelerated disinfection, overcoming the diffusion limitation of chemical disinfectants. Complete (>99.99%) and broad-spectrum disinfection was achieved <1 min of attachment to the scaled-up device (25 square centimeters), reliably for 72 hours at high temperature (60°C) and humidity (90%). This method can be readily applied to high-touch surfaces in indoor environments for pathogen control.

Polarization Saturation in Multilayered Interfacial Ferroelectrics.

Van der Waals polytypes of broken inversion and mirror symmetries have been recently shown to exhibit switchable electric polarization even at the ultimate two-layer thin limit. Their out-of-plane polarization has been found to accumulate in a ladder-like fashion with each successive layer, offering 2D building blocks for the bottom-up construction of 3D ferroelectrics. Here, it is demonstrated experimentally that beyond a critical stack thickness, the accumulated polarization in rhombohedral polytypes of molybdenum disulfide saturates. The underlying saturation mechanism, deciphered via density functional theory and self-consistent Poisson-Schrödinger calculations, point to a purely electronic redistribution involving: 1.Polarization-induced bandgap closure that allows for cross-stack charge transfer and the emergence of free surface charge; 2. Reduction of the polarization saturation value, as well as the critical thickness at which it is obtained, by the presence of free carriers. The resilience of polar layered structures to atomic surface reconstruction, which is essentially unavoidable in polar 3D crystals, potentially allows for the design of new devices with mobile surface charges. The findings, which are of general nature, should be accounted for when designing switching and/or conductive devices based on ferroelectric layered materials.

Computational fluid dynamics simulations of single-bubble evolution under synergy of ultrasound and an electrostatic field

In the study reported here, a two-phase flow model was developed for the evolution of a single bubble under ultrasonic irradiation coupled with an electrostatic force. We started with the following assumptions: (I) the liquid is incompressible, (II) the effect of gravity is negligible in the liquid, (III) the bubble is insulating, and no free charges are distributed on the liquid–gas interface, and (IV) the liquid contains only one bubble. Using computational fluid dynamics, we analyzed how the bubble shape evolves under various conditions, and the main findings are as follows: (1) With increasing electric field strength, the bubble reaches a larger maximum area and a smaller minimum area. Furthermore, during the positive phase of ultrasound, a higher electric field strength leads to faster compression and a more slender bubble. (2) As the initial bubble radius is increased from 3 to 5 μm, the cavitation becomes significantly stronger, but when the initial bubble radius reaches 10 μm, the cavitation intensity decreases instead because of greater compression resistance caused by there being more gas in the bubble. (3) Cavitation cannot be triggered under an excessively low acoustic pressure amplitude, and an excessively high acoustic pressure amplitude results in weaker cavitation; the appropriate acoustic pressure amplitude is considered to be 1.35 atm.

Entangling imidazolium-based ionic liquids and melanins: A crossover study on chemical vs electronic properties and carrier transport mechanisms

Melanins (mel) are a class of pigments that are nearly ubiquitous and among the oldest compounds found in nature. However, their practical application has been limited due to their low solubility in water and in most organic solvents. Recent research on polydopamine has revealed that ionic liquids (ILs) not only enhance melanin’s dissolution but also fine-tune its redox properties through specific dipolar interactions. In this study, we expand upon previous investigations by customizing new suspensions on a broader range of melanins. Concerning ILs, we focus on imidazolium based ILs, tailoring their chemical properties (pKa) and structural characteristics (cation radius, anion radius).The melanins under consideration include synthetic polymers derived from the oxidative polymerization of 5,6-dihydroxyindole (DHI) and its 2-carboxylic acid counterpart (DHICA), as well as the natural pigment Sepiomelanin (Sepiomel), which is isolated from the ink sack of cuttlefish. Our comparative analysis between neat ILs and ILs-mel responses reveals several key findings: the increase in solubility, the tuning of the redox ability, the decrease of the ionic charge resistance (from MΩ τo kΩ); the partial removal of the electrical polarization effects and the delocalized ionic charge hopping mechanisms in conductivity; the increase of the free ionic diffusion mobility and Debye lengths. Notably, electrical transport is influenced by both the chemical features and the steric hindrance in the ILs as well as the specific type of melanin employed. These factors contribute to the high order correlation between free ionic charge densities and their corresponding Debye lengths. Consequently, our findings suggest that for these complex systems, an improved model extending beyond a simplified electrostatic interaction mechanism is required.

Self-Induced Ge-Doped HfO2 Applied to Ge Stacked Nanowires Ferroelectric Gate-All-Around Field-Effect Transistor with Steep Subthreshold Slope Under O3 Treatment with GeO2 as Interfacial Layer

This study reports a self-induced ferroelectric Ge-doped HfO2 (Ge:HfO2) thin film through interface reactions. In the first experiment, three treatments for forming interfacial layer (IL) were discussed through TiN/2-nm-thick Al2O3/2-nm-thick Ge:HfO2/GeO2/Ge metal-ferroelectric-insulator-semiconductor capacitors. The remnant polarization (Pr), leakage current, and interface trap density (Dit) were compared to select the most appropriate IL treatment. The results show that the in-situ ozone treatment under the standard atomic layer deposition process had the second highest 2Pr value as well as lower Dit values. Next, the thicknesses of Al2O3/Ge:HfO2 would be changed to 4 nm/2 nm and 3 nm/3 nm to investigate the ferroelectricity and leakage current. Although the 3-nm-thick Al2O3/3-nm-thick Ge:HfO2 shows a lower 2Pr value, the leakage current is much lower than 2-nm-thick Al2O3/2-nm-thick Ge:HfO2. The self-induced ferroelectric 3-nm-thick Ge:HfO2 thin film was then applied to fabricate Ge stacked nanowires gate-all-around field-effect transistor. The results show a steep subthreshold slope of 58 mV/dec for pFET and on-off current ratio > 105 and have high potential in low-power IC applications.

Investigation of AC and DC Electrical Conductivity in Ethyl Cellulose (EC) and Poly Methyl Methacrylate (PMMA) Polyblends

The study of AC and DC electrical conductivity is crucial for understanding the behavior of charge carriers within materials and their mobility. Ethyl cellulose (EC) stands out among cellulose ethers due to its favorable electrical, mechanical, and weathering properties. Poly Methyl Methacrylate (PMMA) is a thermoplastic known for its rigidity, transparency, and outdoor durability, making it a valuable material. Despite being insulating materials, both EC and PMMA exhibit limited free charge carriers and low mobility. In this research, AC and DC electrical properties of Ethyl Cellulose (EC), Poly Methyl Methacrylate (PMMA), and their blends doped with tetrahydrofuran (THF) film were investigated using isothermal evaporation techniques. The investigation focused on the effects of temperature, electric field, and frequency on electrical conduction mechanisms. Measurements were conducted across frequencies ranging from 1 KHz to 1 MHz at temperatures between 323 K and 373 K. Results indicate that AC electrical conductivity of Ethyl Cellulose (EC), Poly Methyl Methacrylate (PMMA), and their blend (EC/PMMA) increases with higher frequencies of the applied electric field. Meanwhile, DC electrical conductivity of Ethyl Cellulose (EC), Poly Methyl Methacrylate (PMMA), and their blend (EC/PMMA) rises with increasing temperature. X-ray diffraction (XRD) analysis further supports these conductivity changes in the blend.

Study on time–frequency features of induced charge signals during the damage and failure process of coal medium

Monitoring and preventing coal-rock dynamic disasters are vital for safe mining. To investigate the time–frequency features of induced charge signals with coal damage and failure of roadways, the generation mechanism of free charge in loaded coal is analyzed and the induced charge monitoring test is conducted. According to the stress-induced charge-time curves, the time-domain features of charge signals at each loading stage are obtained. The wavelet threshold denoising approach and generalized Morse wavelet transform method are applied to denoise the raw signals and study the frequency-domain features. Further, the quantitative relationship between the de-noised induced charge signals and the degree of coal damage is established. The results show that the event number, amplitude and fluctuation degree of available induced charge signals are all at a low level in the compaction and elastic stages of the coal, which are mainly generated by the piezoelectric effect and predominantly represent discreteness. When entering the plastic and failure stages, the available signals are primarily produced by the crack propagation and triboelectric effects, with a significant increase in the event number, amplitude, and fluctuation degree. Then the induced charge signals gradually transit from discrete to continuous. Generally, the dominant frequency of the available induced charge signals during the coal damage process is concentrated at 0 ~ 11 Hz. The available induced charge is positively correlated with the degree of coal damage, which can perform the damage degree of coal mass, providing a new approach to evaluate the stability of roadway surrounding rocks.

Eco-Sustainable Aluminum-Air Batteries

Aluminum-air batteries are energy conversion devices considered to be promising alternative to lithium-ion batteries due to their high theoretical energy density as well as the easy availability and recyclability of the anode material. The use of neutral water-based electrolytes and raw materials of natural or synthetic but biodegradable origin in the battery components, mainly electrolytes and cathodes, adds further advantages of safety, affordable costs and eco-friendliness. In this work, the electrochemical performance of aluminum-air batteries assembled with gel polymer electrolytes, made of natural polysaccharides and saline aqueous solutions, was investigated and discussed, through comparing the results obtained using cathodes based on platinum catalyst with respect to those based on a cheaper wood-derived activated carbon. Three-electrodes discharge measurements, rate performance tests, polarization and power density curves, and linear sweep voltammetry measurements were used to critically compare different cathodic materials used in combination with neutral electrolytes. The results show that the best electrochemical performances were obtained for aluminum-air cells assembled with wooden biomass-derived air cathodes.

Enhanced Performance of Fe/WO3 Terahertz Dielectric Lenses

AbstractHerein transparent iron nanosheets deposited by the ionic coating technique onto glass and WO3 dielectric lenses are studied and characterized. The thickness of Fe nanosheets is varied in the range of 70–350 nm. It is observed that the transmittance and reflectance of the Fe nanosheets are highly affected by the layer roughness. Coating of iron nanosheets onto WO3 dielectric lenses increases the light absorption of WO3 by more than 240 times and red‐shifts the energy bandgap. Remarkable enhancements in the dielectric constant and in the optical conductivity are achieved via Fe coatings. In addition, iron coated dielectric lenses show higher terahertz cutoff limits varying in the range of 1.0–30 THz. Iron nanosheets remarkably increase the free charge carrier density and plasmon frequency in the infrared range of light. Moreover, the temperature dependent electrical conductivity shows high temperature stability and an increased electrical conductivity by more than 7 orders of magnitude by coating WO3 with 70 nm thick Fe nanosheets. The stability of the electrical conductivity at low temperatures and the wide range of terahertz cutoff limits in addition to the well‐enhanced light absorbability makes the iron coated tungsten oxide dielectric lenses promising for multifunction optoelectronic applications.