Electron Motion Research Articles

Few-femtosecond time-resolved study of the UV-induced dissociative dynamics of iodomethane

Ultraviolet (UV) light that penetrates our atmosphere initiates various photochemical and photobiological processes. However, the absence of extremely short UV pulses has so far hindered our ability to fully capture the mechanisms at the very early stages of such processes. This is important because the concerted motion of electrons and nuclei in the first few femtoseconds often determines molecular reactivity. Here we investigate the dissociative dynamics of iodomethane following UV photoexcitation, utilizing mass spectrometry with a 5 fs time resolution. The short duration of the UV pump pulse (4.2 fs) allows the ultrafast dynamics to be investigated in the absence of any external field, from well before any significant vibrational displacement occurs until dissociation has taken place. The experimental results combined with semi-classical trajectory calculations provide the identification of the main dissociation channels and indirectly reveal the signature of a conical intersection in the time-dependent yield of the iodine ion. Furthermore, we demonstrate that the UV-induced breakage of the C-I bond can be prevented when the molecule is ionized by the probe pulse within 5 fs after the UV excitation, showcasing an ultrafast stabilization scheme against dissociation.

Creating an intermediate energy band to boost the photoelectrochemical efficiency of TiO2 for solar-driven hydrogen production

The utilization of photoelectrochemical processes for hydrogen generation from water and solar energy offers a promising avenue to replace non-renewable energy sources. Nevertheless, achieving high-performance photoanode electrodes poses a significant challenge. In this study, we present the synthesis cerium and chromium-doped TiO2 (CeCrTiO2) is produced through a simple, scalable, and cost-effective hydrothermal method on a fluorine-doped tin oxide (FTO) substrate. the introduction of Ce and Cr impurities is highlighted for its role in creating an impurity band within CeCrTiO2. This impurity band is instrumental in enhancing the separation and movement of electrons and holes, contributing to the improved performance of CeCrTiO2 as a photoanode in photoelectrochemical applications. Hence, the photocurrent density value of CeCrTiO2 is 4.5 times higher than that of bare TiO2. This suggests that CeCrTiO2 exhibits improved efficiency in generating a photocurrent when exposed to light, indicating enhanced photoelectrochemical performance. The amount of hydrogen produced by CeCrTiO2 is noted to be 4.88 times greater than that of bare TiO2. This highlights the material's effectiveness in harnessing solar energy to drive the water-splitting reaction, leading to a higher yield of hydrogen gas. The synthesis of CeCrTiO2 through a hydrothermal method results in a photoanode with significantly enhanced performance, positioning it as a promising candidate for advancing photoelectrochemical processes aimed at replacing non-renewable energy sources.

On a drift‐diffusion model for perovskite solar cells

AbstractWe introduce a vacancy‐assisted charge transport model for perovskite solar cells. This instationary drift‐diffusion system describes the motion of electrons, holes, and ionic vacancies and takes into account Fermi–Dirac statistics for electrons and holes and the Fermi–Dirac integral of order for the mobile ionic vacancies in the perovskite. The free energy functional we work with corresponds to that choice of the statistical relations. To verify the existence of weak solutions, we consider a problem with regularized state equations and reaction terms on any arbitrarily chosen finite time interval. We motivate its solvability by time discretization and passage to the time‐continuous limit. A priori estimates for the chemical potentials that are independent of the regularization level ensure the existence of solutions to the original problem. These types of estimates rely on Moser iteration techniques and can also be obtained for solutions to the original problem.

Orbital Edelstein effect of electronic itinerant orbital motion at edges

Orbital Edelstein effect of electronic itinerant orbital motion at edges

Construction of α-Fe2O3 Nanorods/UiO-66-NH2 by in-situ Growth with Photocatalytic Reduction of Cr (VI)

Abstract Cr (VI) is widely used in industry but its high toxicity causes environmental pollution that needs addressing. The growth of photosensitive materials on semiconductor surfaces can successfully stop photogenerated electron-hole pair recombination, increasing photocatalytic efficiency. Herein, α-Fe2O3 nanorods/UiO-66-NH2 compounds were successfully obtained through the in-situ solvothermal approach. By using 2-aminoterephthalic acid in the solvothermal treatment of Zr4+ adsorbed α-Fe2O3 nanorods, the UiO-66-NH2 nanocrystals were evenly distributed on the nanorods. In addition, the reduction efficiency of wastewater reached 93% after 150 min of light exposure, much higher than uncompounded materials. Moreover, the α-Fe2O3/UiO-66-NH2 crystals had good regeneration ability, retaining 73% of Cr (VI) removal capacity after four cycles. In this process, α-Fe2O3 and UiO-66-NH2 effectively complexed to form a heterojunction, which effectively suppressed the complexation of electrons (e-) and holes (h+). This efficient complex facilitates the photocatalytic degradation of highly noxious Cr (VI) to Cr (III) under visible light. The efficient Cr (VI) elimination ability comes from the photocatalytic reduction mechanism where they form a special interface to promote the movement of electrons and holes for efficient removal. This work provides both a new approach for in-situ synthesis and a reference for efficient Cr (VI) elimination.

Phonon Drag Contribution to Thermopower for a Heated Metal Nanoisland on a Semiconductor Substrate.

The possible contribution of phonon drag effect to the thermoelectrically sustained potential of a heated nanoisland on a semiconductor surface was estimated in a first principal consideration. We regarded electrons and phonons as interacting particles, and the interaction cross-section was derived from the basic theory of semiconductors. The solution of the equation of motion for average electrons under the simultaneous action of phonon drag and electric field gave the distributions of phonon flux, density of charge carriers and electric potential. Dimensional suppression of thermal conductance and electron-phonon interaction were accounted for but found to be less effective than expected. The developed model predicts the formation of a layer with a high density of charge carriers that is practically independent of the concentration of dopant ions. This layer can effectively intercept the phonon flow propagating from the heated nanoisland. The resulting thermoEMF can have sufficient magnitudes to explain the low-voltage electron emission capability of nanoisland films of metals and sp2-bonded carbon, previously studied by our group. The phenomenon predicted by the model can be used in thermoelectric converters with untypical parameters or in systems for local cooling.

An Observer-Based View of Euclidean Geometry

An influence network of events is a view of the universe based on events that may be related to one another via influence. The network of events forms a partially ordered set which, when quantified consistently via a technique called chain projection, results in the emergence of spacetime and the Minkowski metric as well as the Lorentz transformation through changing an observer from one frame to another. Interestingly, using this approach, the motion of a free electron as well as the Dirac equation can be described. Indeed, the same approach can be employed to show how a discrete version of some of the features of Euclidean geometry including directions, dimensions, subspaces, Pythagorean theorem, and geometric shapes can emerge. In this paper, after reviewing the essentials of the influence network formalism, we build on some of our previous works to further develop aspects of Euclidean geometry. Specifically, we present the emergence of geometric shapes, a discrete version of the parallel postulate, the dot product, and the outer (wedge product) in 2+1 dimensions. Finally, we show that the scalar quantification of two concatenated orthogonal intervals exhibits features that are similar to those of the well-known concept of a geometric product in geometric Clifford algebras.

Topological phase transitions via attosecond x-ray absorption spectroscopy.

We present a numerical experiment that demonstrates the possibility to capture topological phase transitions via an x-ray absorption spectroscopy scheme. We consider a Chern insulator whose topological phase is tuned via a second-order hopping. We perform time-dynamics simulations of the out-of-equilibrium laser-driven electron motion that enables us to model a realistic attosecond spectroscopy scheme. In particular, we use an ultrafast scheme with a circularly polarized IR pump pulse and an attosecond x-ray probe pulse. A laser-induced dichroism-type spectrum shows a clear signature of the topological phase transition. We are able to connect these signatures with the Berry structure of the system. This work extend the applications of attosecond absorption spectroscopy to systems presenting a non-trivial topological phase.&#xD.

Suppression of Nonlinear Chorus Wave Growth by Active Control of Gyroresonant Interactions With Electron Hole Deformation

AbstractNonlinear gyroresonant acceleration is an essential mechanism for the formation of relativistic electrons in Earth's radiation belts, yet we still have only limited knowledge of how electron motion interacts nonlinearly with plasma waves. Here we demonstrate the compelling suppression of whistler‐mode chorus emissions as a resonant wave with energetic electrons by tuning an external transmitter signal in space plasmas. Through forcible modification of electron motions via phase trapping by the external waves, the nonlinear gyroresonant current is suppressed along with the electron hole deformation. Moreover, this can decrease the population of relativistic electrons due to the lack of coherent resonant waves seen by the phase‐organized electrons. Understanding such nonlinear wave suppression effects is crucial for a potential active control of Earth's plasma environment.

Laser modulation to plateau region and intensity of high-order harmonic generation in monolayer MoTe2

Abstract Through solving semiconductor Bloch equations, we theoretically investigated the high-order harmonic generation in monolayer MoTe2 under laser modulation. Adjusting the laser parameters, the plateau region and intensity of harmonics can be effectively regulated. Changing laser wavelength can regulate the width of platform region and the cutoff order of harmonic spectrum. Platform region widens with the increase of laser wavelength. Under different laser wavelengths, the number of photons that need to be absorbed for electron transition varies, which affects the inter-band transition of electrons. Laser vector potential also varies with the wavelength, affecting the intra-band motion of electrons. Laser field strength can significantly change the harmonic intensity. As the laser field strength increases, the harmonic intensity increases and may generate new plateau in the high-energy region. The emergence of new platform is due to the transition of electrons between conduction bands. Our work provides a theoretical exploration for generating high quality harmonics and understanding the micro mechanism of high-order harmonic generation.

Signal Amplification of Z-Scheme Photocathode Triggered by Directional Movement of Electrons: A Preferable Approach for Cathodic Photoelectrochemical Analysis

Signal Amplification of Z-Scheme Photocathode Triggered by Directional Movement of Electrons: A Preferable Approach for Cathodic Photoelectrochemical Analysis

Electric-Field Catalysis on Carbon Nanotubes in Electromicrofluidic Reactors: Monoterpene Cyclizations.

The control over the movement of electrons during chemical reactions with oriented external electric fields (OEEFs) has been predicted to offer a general approach to catalysis. Recently, we suggested that many problems to realize electric-field catalysis in practice under scalable bulk conditions could possibly be solved on multiwalled carbon nanotubes in electromicrofluidic reactors. Here, we selected monoterpene cyclizations to assess the scope of our system in organic synthesis. We report that electric-field catalysis can function by stabilizing both anionic and cationic transition states, depending on the orientation of the applied field. Moreover, electric-field catalysis can promote reactions which are barely accessible by general Brønsted and Lewis acids and field-free anion-π and cation-π interactions, and drive chemoselectivity toward intrinsically disfavored products without the need for pyrene interfacers attached to the substrate to prolong binding to the carbon nanotubes. Finally, interfacing with chiral organocatalysts is explored and evidence against contributions from redox chemistry is provided.

Chemical synthesis of NiO nanoparticles from Solanum trilobatum leaf extract for antibacterial and cytotoxic properties

The chemical precipitation approach was employed to synthesize Nickel oxide nanoparticles (NiONPs) using Solanum trilobatum leaf extract as the stimulant and Nickel nitrate as the precursor. The Nickel oxide is examined using a range of characterization methods including X-ray diffraction, Fourier Transform Infrared spectroscopy, High-Resolution Transmission Electron Microscopy, High-Resolution Scanning Electron Microscopy, X-ray photoelectron spectroscopy, Thermo gravimetric Analysis/Derivative Thermo gravimetric Analysis, Diffuse Reflectance Spectroscopy, cytotoxicity and antimicrobial investigations The X-ray diffraction examination determined that the average size of the crystals increases as the quantities of leaf extract in the NiO2 composites rise. The decrease in line broadening (β) value and the increase in leaf extract concentrations may be the cause of this phenomenon. The FTIR spectrum confirms that the as-synthesized NiO-NPs are of great purity and match well with the XRD pattern. The thermal stability of the synthesized samples was determined using TGA/DTG analysis. The analysis was conducted in an air atmosphere, with the temperature increasing at a rate of 10°C per minute. The temperature range for the analysis was from room temperature to 750°C. The optical properties are determined by the use of Diffuse Reflectance Spectroscopy, which examines the coordinated movement of electrons in the conduction band when exposed to electromagnetic waves. Rat skeletal muscle cell line and SKMEL cancer cells were cultured on 96-well plates and incubated at 37°C and 5 % CO2 for 24 hours to allow them to adapt to the culture conditions. An investigation was conducted to assess the antibacterial properties of synthesized nanocomposites against two types of bacteria: gram-positive Staphylococcus aureus (MTCC No: 87) and gram-negative Escherichia coli (MTCC No: 443), in order to explore their potential for biological applications.

Design of non-heat-treatable Al-Fe-Ni alloys with high electrical conductivity and high strength via CALPHAD approach

Electrical conductivity and strength are two critical properties concerned for rotors materials in electric vehicles. However, the two properties are often mutually exclusive in cast Al alloys. The present work proposes a novel non-heat-treatable Al-Fe-Ni alloy by considering the intermetallic compound’s content and morphology. With the modification of Ni and Fe content, the solidification path of designed alloy were calculated to predict the phase composition, which would greatly impact their performance. The as-cast Al-2Fe-1Ni (wt%) alloy exhibits comprehensive properties with an ultimate tensile strength of 131.2±2.5 MPa, an elongation of 20.2±3.6 % and an electrical conductivity up to 52.0±0.1 %IACS. The eutectic microstructure of Al13(Fe,Ni)4+α-Al in Al-2Fe-1Ni alloy accounts for over 90 %, much larger than the eutectic content in Al-0.4Fe-3.4Ni and Al-1Fe-1Ni alloys. The fine eutectics in Al-2Fe-1Ni alloy improve the second-phase strengthening effects and plastic deformation capability. In addition, the fibrous rod-like intermetallic reduces the electron scattering during the propagation process and leaves more space for free electron movement. The dominant second phase transforms from Al3Ni phase to Al9FeNi phase, further enhancing the thermal stability of the alloy. After aging treatment at 180 °C for 100 h, it shows no noticeable change in electrical conductivity and mechanical properties. It is hoped that this work can provide a new design approach for high-strength and high-conductivity Al alloys.

Hall effects and diamagnetic cavity collapse during a laser plasma cloud expands into a vacuum magnetic field

This paper describes the results of a laboratory experiment on the sub-Alfven expansion of a quasi-spherical laser plasma cloud into a vacuum magnetic field in the regime of nonmagnetized ions. The role of Hall fields and currents in the anomalously fast dynamics of the magnetic field during the collapse phase of a diamagnetic cavity is considered. Detailed spatial measurements of the azimuthal Hall fields configuration are demonstrated and their relationship to diamagnetic cavity collapse is determined. As a result of the experiment, data were obtained confirming the hypothesis about the transfer of the main magnetic field by the movement of electrons associated with Hall currents.

Torsional oscillations of magnetized neutron stars: Impacts of Landau-Rabi quantization of electron motion

Torsional oscillations of magnetized neutron stars: Impacts of Landau-Rabi quantization of electron motion

Roadmap on basic research needs for laser technology

Abstract Motivated by the profound impact of laser technology on science, arising from an increase in focused light intensity by seven orders of magnitude and flashes so short electron motion is visible, this roadmap outlines the paths forward in laser technology to enable the next generation of science and applications. Despite remarkable progress, the field confronts challenges in developing compact, high-power sources, enhancing scalability and efficiency, and ensuring safety standards. Future research endeavors aim to revolutionize laser power, energy, repetition rate and precision control; to transform mid-infrared sources; to revolutionize approaches to field control and frequency conversion. These require reinvention of materials and optics to enable intense laser science and interdisciplinary collaboration. The roadmap underscores the dynamic nature of laser technology and its potential to address global challenges, propelling progress and fostering sustainable development. Ultimately, advancements in laser technology hold promise to revolutionize myriad applications, heralding a future defined by innovation, efficiency, and sustainability.

Electronic Structure Modulating of W 18 O 49 Nanospheres by Niobium Doping for Efficient Hydrogen Evolution Reaction.

Developing efficient electrocatalysts to reduce HER overpotential is vital to enhance hydrogen production efficiency and minimize energy consumption. Adjusting the electronic structure of transition metal oxides via elemental doping is a potent strategy to improve the effectiveness of electrocatalysts for hydrogen evolution. In this work, we synthesized a set of niobium-doped tungsten oxides (Nbx-W18O49) under anoxic conditions using a straightforward "one-pot" solvothermal approach. After doping Nb, the oxygen vacancy content inside W18O49was increased, which induced a synergistic effect with the active sites of tungsten. In acidic environments, the hydrogen evolution activity of the Nb0.6-W18O49electrocatalyst is secondonly by 20 wt% Pt/C. It attains a current density of -10 mA cm-2at an overpotential of 102 mV. By comparison with W18O49, Nb0.4-W18O49and Nb0.5-W18O49, Nb0.6-W18O49demonstrates a reduced charge transfer resistance, which significantly enhances its conductivity and the speed of electron movement across interfaces. Coupled with this feature are notably faster HER kinetics. Additionally, it exhibits excellent stability, meaning it maintains its performance and structural integrity over prolonged periods and under various operational conditions. This article provides a new perspective for discovering inexpensive and efficient hydrogen evolution electrocatalyst materials.

Enhanced photocatalytic CO2 reduction to CH4 on oxygen vacancy-rich NiCo2O4 with surface pits: Synthesis, DFT calculations, and mechanistic insights

Unraveling the influence of surface microstructure in materials on their interaction with CO2 remains a critical challenge in achieving efficient and selective CO2 reduction. In this study, we report the engineering of pit structures on the NiCo2O4 surface for efficient photocatalytic reduction of CO2. Characterization results show that calcination temperature affects the distribution of surface pits and oxygen vacancy concentration. Oxygen vacancy sites accompanying surface pits facilitate the generation and movement of photogenerated electrons and holes, preventing their recombination and promoting the conversion of CO2. The CH4 yield from photocatalytic CO2 reduction reaches 52.4 μmol g−1 with the optimal pitted NiCo2O4 catalyst (PNCO2), significantly surpassing the 18.4 μmol g−1 yield of non-pitted NiCo2O4 (NPNCO). Additionally, PNCO2 improves selectivity from 81.8 % for NPNCO to 94.1 %. Density functional theory calculations show that CO2 adsorption on the PNCO2 surface is significantly enhanced as the d-band center shifts toward the Fermi level. The adsorbed CO2 combines with electrons enriched at the Ni sites at the edges of the surface pits, leading to further activation. The reduction of CO2 to intermediate products such as CHO* is analyzed based on in situ diffuse reflectance infrared Fourier transform spectroscopy, and a possible reaction pathway is proposed. This work offers fresh insights into engineering surface pit structures for the design and synthesis of catalysts for photocatalytic CO2 reduction.

Novel dopamine-derived carbon modified fe-based metal–organic framework enhanced aptasensor rendering ultrasensitive electrochemical detection of oxytetracycline

In the present work, an aptasensor with dual binding sites based on Au NPs modified with self-polymerized polydopamine (PDA) and Fe-MOF is successfully constructed. In terms of standard electron transfer, the cyclic voltammetry (CV) analysis showcases a rate constant (ks) of 96.0 s−1, signifying an exceptional electron transfer rate of oxytetracycline at the sensor interface of Apt/Au@PDA@NH2-MIL-101(Fe)/GCE. Further deepening the investigation into electrochemical kinetics using chronoamperometry (CA), we investigated the electrocatalytic parameters (Kcat) of Au@PDA@NH2-MIL-101(Fe) in relation to oxytetracycline. The results divulged an impressive average Kcat value of 3.06 × 105 M−1 S-1. This evidence robustly suggests the superior electrocatalytic activity of Au@PDA@NH2-MIL-101(Fe) when it comes to oxytetracycline oxidation. A custom-designed portable rapid detection platform was developed, achieving detection limits of 6.88 nM under static water flow conditions and 5.56 nM under dynamic conditions. Remarkably, the self-polymerization of PDA on Au NPs not only refines their size but also boosts their interaction with biomolecules, thereby promising excellent biocompatibility. Moreover, the abundance of –COOH groups and unsaturated Fe3+ sites on the NH2-MIL-101(Fe) surface furnishes a considerable number of grafting sites for the aptamer. More importantly, the redox interplay between Au@PDA and NH2-MIL-101(Fe) accelerates electron movement, thus amplifying the electrochemical signal and the detection sensitivity for oxytetracycline.