Angular Distribution Research Articles

The N+ Formation Mechanism of Vibrationally Selected N2O+ Ions in the C2Σ+ State: A TPEPICO Imaging Study.

The N-NO bond fission of N2O+(C2Σ+) ions can produce two major fragment ions, NO+ or N+. In contrast to the dominant NO+ fragment ion, the N+ formation mechanism remains unclear to date. Here, dissociative photoionization of N2O via the C2Σ+ ionic state has been reinvestigated using a combined approach of threshold photoelectron-photoion coincidence (TPEPICO) velocity imaging and quantum chemical calculations. Accompanying the N+(3P) formation, the NO(X2Π) neutral fragment with low and high vi-rotational distributions was identified, based on the N+ speed and angular distributions derived from the TPEPICO images. In particular, the excitation of the symmetric stretching ν1+ mode promotes the formation of high rotational components, while the asymmetric stretching ν3+ mode shows the exact opposite effect. According to our calculated multistate potential energy surfaces, intersystem crossing from C2Σ+ to 14Π exclusively provides feasible decomposition pathways to produce the N+ fragment. In a slightly bent geometry, spin-orbit couplings between C2Σ+ and two substates of 14Π, 14A' or 14A″, play a crucial role in the N+ formation from vibrationally selected N2O+(C2Σ+) ions. The mechanism also provides new insights into the charge transfer reaction of N+ + NO → N + NO+.

High-Resolution Crossed-Beam Dynamics Studies of the D + Para-H2 → HD + H Reaction at 1.21 eV.

Understanding kinetic isotope effects is important in the study of the reaction dynamics of elementary chemical reactions, particularly those involving hydrogen atoms and molecules. As one of the isotopic variants of the hydrogen exchange reaction, the D + para-H2 reaction has attracted much attention. However, experimental studies of this reaction have been limited primarily due to its strong experimental background noise. In this study, by using the velocity map ion imaging method and the near-threshold ionization technique, together with improvements on the vacuum condition in the vicinity of the collision zone, background noise was reduced significantly, and quantum state-resolved differential cross sections (DCSs) for the D + para-H2 reaction at a collision energy of 1.21 eV were acquired in a crossed molecular beams experiment. Interestingly, clear rotational state-dependent angular distributions were noticed in the quantum state-resolved DCSs. The most intense peak's positions for HD (v', j') products shift to different scattering directions as the product's ro-vibrational quantum number increases. Two different microscopic reaction mechanisms are found to be involved in this reaction for HD products in different vibrational states. The results show a direct correlation between the scattering angle and the product's rotational quantum number, revealing that the contributions of impact parameters are strongly influenced by the corresponding centrifugal barrier.

Composite Electromagnetic Scattering Characteristics of Actual Terrain and Moving Rockets

This research involved studying the characteristics of composite electromagnetic scattering from a rocket moving above actual terrain using the finite-difference time-domain method. The angular distribution curve of the composite scattering coefficient was obtained, and the influences of factors such as the angle of incidence, the frequency of the incident electromagnetic wave, the content of moisture in soil, the dielectric constant of the rocket-shell material, the height of the rocket, and the undulation of the terrain on the composite scattering coefficient were investigated. Results show that the composite scattering coefficient oscillates with the scattering angle and increases in the direction of mirror reflection. It also decreases with increasing angle of incidence, frequency of the incident wave, and altitude of the rocket, while it increases with increasing soil moisture and dielectric constant of the rocket-shell materials. Although the influence of different terrain undulations on the composite scattering coefficient is noticeable, it follows no fixed pattern.

Insights into the Mechanism of Chiral-Induced Spin Selectivity: The Effect of Magnetic Field Direction and Temperature.

Chiral oligopeptide monolayers are adsorbed on a ferromagnetic surface and their magnetoresistance is measured as a function of the angle between the magnetization of the ferromagnet and the surface normal. These measurements are conducted as a function of temperature for both enantiomers. The angle dependence is found to follow a changing trend with a period of 360°. Quantum simulations reveal that the angular distribution can be obtained only if the monolayer has significant effective spin orbit coupling (SOC), that includes contribution from the vibrations. The model shows that SOC only in the leads cannot reproduce the observed angular dependence. The simulation can reproduce the experiments if it included electron-phonon interactions and dissipation.

Scattering properties of dual Bessel beams on chiral layered particle

The paper investigates the scattering analytical solution of arbitrary direction double zero-order Bessel beams (ZOBBs) incident on a non-uniform layered chiral sphere. Using the generalized Lorenz-Mie theory (GLMT), the electromagnetic field expansion expression of the double ZOBBs is obtained through the vector superposition of the spherical vector wave functions (SVWFs). Analytical solutions of the scattering on chiral layered particles by dual Bessel beams are derived based on the boundary condition. The iterative coefficient equations are constructed to obtain the expansion coefficients of the SVWFs in each region of the multi-layer chiral sphere. The variation of radar cross section (RCS) with angular distribution is numerically simulated, and the scattering results of layered chiral spheres degenerated into isotropic layered spheres are compared with the literature, which verifies the correctness of the theory and program. The effects of incident angle, polarization angle, cone angle and chiral parameters on the scattering characteristics of far region and internal field of the layered chiral particle are analyzed in detail. The theory and results can offer significant assistance in studying the optical properties of non-uniform chiral particles and complex biological cells irradiated by multiple beams and may also provide important practical value in the micromanipulation of multi-layered biological structures.

Three-dimensional tomographic reconstruction using Voronoi weighting

Three-dimensional tomographic reconstruction requires careful selection of the illumination angles, often under certain measurement constraints. When the angular distribution must be nonuniform, appropriate selection of the reconstruction weights is necessary. We show that Voronoi weighting can significantly improve the fidelity of optical diffraction tomography.

Optimizing Horticulture Luminescent Solar Concentrators via Enhanced Diffuse Emission Enabled by Micro-Cone Arrays.

Optimizing the photon spectrum for photosynthesis concurrently with improving crop yields presents an efficient and sustainable pathway to alleviate global food shortages. Luminescent solar concentrators (LSCs), consisting of transparent host matrices doped with fluorophores, show excellent promise to achieve the desired spectral tailoring. However, conventional LSCs are predominantly engineered for photon concentration, which results in a limited outcoupling efficiency of converted photons. Here, we introduce a scheme to implement LSCs into horticulture (HLSC) by enhancing light extraction. The symmetry of the device is disrupted by incorporating microcone arrays on the bottom surface to mitigate total internal reflection. Both Monte Carlo ray tracing simulations and experimental results have verified that the greatest enhancements in converted light extraction, relative to planar LSCs, are achieved using microcone arrays (base width 50 μm, aspect ratio 1.2) with extruded and protruded profiles (85.15 and 66.55% improvement, respectively). Angularly resolved transmission measurements show that the HLSC device exhibits a broad angular radiation distribution. This characteristic indicates that the HLSC device emits diffuse light, which is conducive to optimal plant growth.

Multistate Dynamics and Kinetics of CO2 Activation by Ta+ in the Gas Phase: Insights into Single-Atom Catalysis.

The activation of carbon dioxide (CO2) by a transition-metal cation in the gas phase is a unique model system for understanding single-atom catalysis. The mechanism of such reactions is often attributed to a "two-state reactivity" model in which the high-energy barrier of a spin state correlating with ground-state reactants is avoided by intersystem crossing (ISC) to a different spin state with a lower barrier. However, such a "spin-forbidden" mechanism, along with the corresponding dynamics, has seldom been rigorously examined theoretically, due to the lack of global potential energy surfaces (PESs). In this work, we report full-dimensional PESs of the lowest-lying quintet, triplet, and singlet states of the TaCO2+ system, machine-learned from first-principles data. These PESs and the corresponding spin-orbit couplings enable us to provide an extensive theoretical characterization of the dynamics and kinetics of the reaction between the tantalum cation (Ta+) and CO2, which have recently been investigated experimentally at high collision energies using crossed beams and velocity map imaging, as well as at thermal energies using a selected-ion flow tube apparatus. The multistate quasi-classical trajectory simulations with surface hopping reproduce most of the measured product translational and angular distributions, shedding valuable light on the nonadiabatic reaction dynamics. The calculated rate coefficients from 200 to 600 K are also in good agreement with the latest experimental measurements. More importantly, these calculations revealed that the reaction is controlled by intersystem crossing, rather than potential barriers.

Anisotropic Photodetachment of Positronium Negative Ions with Linearly Polarized Light.

We report on the anisotropic photodetachment of positronium negative ions, followed by the dissociation into p-wave electrons and positronium atoms, with a linearly polarized laser beam. We have observed a strong recoil effect of the photoelectrons on the translation momentum of the dissociated positronium atoms. With polarization angle-resolved measurements, the asymmetry parameter of the photoemission angular distribution of the ions at a photon energy of 1.165eV was determined to be 1.97±0.04(stat)±0.07(syst), in agreement with a theoretical prediction. The present method can be applied to explore the unrevealed dissociation dynamics of exotic particle systems and their manipulation with polarized light.

Study of 113In(α, α) elastic scattering to determine α-optical potential relevant for astrophysical γ-process

Abstract The α-optical potential is one of the key input parameters used to measure the reaction rate of the (γ, α)-process using the Hauser-Feshbach statistical model and the principle of detailed balance. α-elastic scattering experiment on 113In p-nucleus was carried out in the energy range E lab = 26−32 MeV. The vacuum evaporation technique was used to prepare the 113In target (∼86 μg cm−2). An energy-dependent local optical potential parameters set was obtained by analysing the experimental elastic scattering angular distribution data. The local potential parameters are extrapolated for lower energies and are used to calculate the 113In(α, γ) reaction cross-section.

Investigating the angular distortion impact on vehicular optical camera communication (OCC) systems

Optical camera communication (OCC) shows promise for optical wireless communication (OWC) in vehicular networks. However, vehicle mobility-induced angular distortions hinder system throughput by degrading non-isotropic vehicular OCC channel gain. Few of the prior works have ever made a comprehensive analysis of their impact, especially based on the pixel value which reflects the camera imaging features. To address this knowledge gap, a pixel value-described vehicular OCC system model accounting for transmitter imaging location and intensity from the geometry and radiometry aspects is presented in this paper with common types of the offset and rotation angles included. We integrate a MATLAB-based simulated vehicular OCC system with an experimentally designed testbed for validation and performance analysis. For a single-time snapshot, we investigate the impacts of common angular distortion types in vehicular OCC systems on maximum pixel value, imaging location, and communication-related metrics. Furthermore, we statistically analyze their influences by considering two driving scenarios with respective angular distributions. The angular distortion characterization from this work is expected to lay a stepping stone to addressing mobility in vehicular OCC systems.

Development of a ReaxFF reactive force field for ternary phosphate-based bioactive glasses.

Phosphate-based glasses (PBGs) in the CaO-Na2O-P2O5 system have diverse applications as biomaterials due to their unique dissolution properties. A reactive force field (ReaxFF) has been developed to simulate these materials at the atomic level. The ReaxFF parameters of PBGs, including the interaction between phosphorus and calcium atoms, have been developed using a published code based on genetic algorithms. The training data, including the atomic charges, atomic forces, bond and angle parameters, and different differential energies, are chosen and measured from static quantum-mechanical calculations and abinitio molecular dynamics of PBGs. We did different short- and medium-range structural analyses on the bulk simulated PBGs with different compositions to validate the developed potential. Radial and angular distribution functions and coordination numbers of network formers and modifiers, as well as the network connectivity of the glass, are in agreement with experimental and previous simulations using both shell-model classical force fields and abinitio simulated data; for example, the coordination number of phosphorus is 4.0. This successful development of ReaxFF parameters being able to describe the bulk PBGs enables us to work on the dissolution behavior of the glasses, including the interaction of water molecules with PBGs, in future works.

A Novel UAV Air-to-Air Channel Model Incorporating the Effect of UAV Vibrations and Diffuse Scattering

In this paper, we propose a geometric channel model for air-to-air (A2A) unmanned aerial vehicle (UAV) communication scenarios. The model is established by incorporating line-of-sight, specular reflection, and diffuse scattering components, and it can capture the impacts of UAV vibrations induced by the propeller’s rotation. Based on UAV heights and ground scatterer density, a closed-form expression is derived to jointly capture the zenith and azimuth angular distributions of diffuse rays. The power of diffuse rays is modeled according to the grazing angle of the rays and the electrical properties and roughness of the ground materials. Key statistics, including the temporal autocorrelation function, spatial cross-correlation function, Doppler power spectrum density, and coherence time are derived, providing an in-depth understanding of the time-variant characteristics of the channel. The results indicate that the presented model is capable of capturing certain A2A channel characteristics, which align with the corresponding theoretical analysis. The findings suggest that the scattering effect of the A2A channel is significantly influenced by the altitude of the UAV. Additionally, it is shown that UAV vibrations can introduce extra Doppler frequencies, notably decreasing the temporal correlation and coherence time of the channel. This effect is more prominent when the system operates at high-frequency bands. The effectiveness of the presented model is confirmed through a comparison of its statistics with those of an existing model and with available measurement data.

The role of Ti in mitigating thermal expansion of silica from molecular dynamics simulations

AbstractMolecular dynamics simulations are performed to investigate the structural response of titania silicate glass to temperature. The coefficient of thermal expansion is computed for two titania silicate glasses with 0 and 10 mol% titania content, the structures of which are presented in terms of radial and angular distributions. Revealed by the different changing rates of intertetrahedra bond angles and bond lengths with respect to the Ti and Si atoms, the glass structures tend to exhibit a nonvectorized expansion process at elevated temperatures, leading to inconsistent expansion rates of the structures in different scales. While the average length of TiO and Si‐O bonds both increases with temperature, the decrease in the coefficient of thermal expansion by the addition of Ti atoms is associated with the different expansion rate of tetrahedra. Arising from the gradual decrease in atomic overlapping, decrease in free volume inside the glass with temperature is also identified.

Strong Angular Oscillation of Rotationally Resolved Differential Cross Section in the H + HD → H2 + D Reaction at the Collision Energy of 2.07 eV: Evidence of Geometric Phase Effects.

Geometric phase (GP) effects in chemical reactions are subtle quantum phenomena that are challenging to identify. In this work, we report a joint experimental and theoretical study of the H + HD → H2 + D reaction at a collision energy of 2.07 eV, which is far below the energy of the conical intersection of 2.53 eV. The rotationally state-resolved differential cross sections were measured by a crossed-beam experiment with the scheme of D-atom Rydberg tagging time-of-flight detection. Experimental angular distributions of three rotational states of H2 products exhibit notable variation near the backward scattering direction. Time-dependent quantum mechanics calculations (TDQMs) were carried out at the same collision energy, with and without the inclusion of GP. The experimental angular distributions are in good agreement with TDQM results with the inclusion of GP but do not agree with TDQM results without the inclusion of GP. This work demonstrates the existence of GP effects at energy far below the conical intersection.

Deuteron breakup effects on the d + 12C, 15N, 16O, 24Mg, 32S, 58Ni, and 70Ge elastic scattering angular distributions

Motivated by the well-known n + p cluster structure of deuterons, which appears at breakup threshold energy of 2.225 MeV, the angular distributions (ADs) for elastically scattered deuterons from various targets, namely, 12C, 15N, 16O, 24Mg, 32S, 58Ni, and 70Ge at different energies, are investigated microscopically within the continuum discretized coupled channel (CDCC) method as well as an effective potential (Ueff), considered as the sum of cluster folding and dynamical polarization potentials. The Ueff potentials were employed successfully to reproduce the elastic ADs data for the considered systems in a wide range of energies. The investigation gives evidence for the applicability of the Ueff in describing the ADs data for many nuclear systems.

Diamond-like carbon conversion surfaces for space applications

We present diamond-like carbon (DLC) conversion surfaces to detect particles with energy below 2 keV. Conversion surfaces have been widely applied in measurements of low-energy particles by instruments onboard planetary and heliophysics missions. Their effectiveness is characterized by the efficiency in changing the charge state of the incident particles while maintaining a narrow angular distribution for the reflected particles. DLC as a conversion surface coating material has high conversion efficiency. We developed a conversion surface production process that provides ultra-smooth and ultra-thin DLC conversion surfaces. The process includes substrate preparation through precision cleaning, plasma immersion ion deposition of the DLC film, and diagnostics of the film parameters. The latter includes the measurement of the coating thickness, surface roughness, and the conversion efficiency for ion beams with energy below 2 keV. The process we developed provides the DLC conversion surface coating of repeatable parameters with a mean surface roughness of 3.4 ± 0.2 Å and a mean film thickness of 46.7 ± 0.8 nm uniform across the sample area. Ion beam measurements showed a negative ion yield of 1%–2% for hydrogen atoms and 8%–15% for oxygen atoms with an angular scatter distribution of 10°–20° at full width of half maximum. These results agree with those of other conversion surface coatings in the literature. The DLC conversion surfaces presented here are implemented in the conversion surface subsystem of the Interstellar Mapping and Acceleration Probe (IMAP)-Lo instrument of the IMAP mission scheduled for launch in 2025.

Investigation of breakup process in 9Be(α,n)12C reaction

Neutron energies and angular distributions were measured in 9Be(α,n)12C reaction for α energies of 5.5 and 6.5 MeV. Three major neutron groups were observed in the spectrum, which correspond to the ground and first two excited states of 12C. Measured data could only be explained by the TALYS calculation if reaction at more than one location within the target is considered for a given beam energy. The preferred locations are driven by the resonance energy levels existing in 13C. Neutron yield due to the 9Be breakup process was determined which is found to be 12.6 ± 0.2% and 18.4 ± 0.5% of the total reaction cross-section for 5.5 and 6.5 MeV respectively.

Machine learning model to efficiently predict the structure and properties of MgCl2–NaCl–KCl melts

MgCl2–NaCl–KCl ternary melts hold great promise as thermal energy storage and heat transfer fluid for the next generation of concentrating solar power (CSP), offering major advantages such as high-temperature storage capacity, adjustable temperature ranges, and renewable usability. However, a critical challenge is the lack of an accurate model to analyze the structural and property aspects of this complex melt. In response, a machine learning-based model with high accuracy and applicability has been developed for this purpose. Based on DPMD techniques, the trained model is used to investigate the structure information, transport and thermal properties of the melt. Temperature and composition effects are introduced. Radial distribution functions, coordination numbers, and angular distribution functions are applied to investigate the microscopic ionic environment within the melt. Transport properties studied include density, self-diffusion coefficient, ionic conductivity, and viscosity, while thermal properties include heat capacity at constant pressure and volume and thermal conductivity. Our model accurately reproduces the results obtained from FPMD simulations and accurately predicts the macroscopic properties of the melt through validation. The high stability of the Mg2+-Cl- interactions is introduced, which remains relatively unaffected by temperature and concentration changes. The presence of MgCl53− species in the melt was observed. We are devoted to the development of AI for the CSP science field. Due to the application of machine learning strategies, our models have proven to have exceptional accuracy and ease of study for MgCl2–NaCl–KCl ternary melts, and they can provide valuable insights into their properties and ionic behaviors.

Imaging Rovibrational Excitation of Scattered YO Molecules in Inelastic Collisions with Kr and Ne.

Energy transfer between atoms and molecules is fundamental to many physical and chemical processes, and understanding the mechanisms and outcomes of energy transfer is crucial for various applications in physics and chemistry. Here, the rovibrational excitation of YO(X 2Σ+) molecules with the collision of Kr and Ne has been studied in the laser-ablation crossed beam and time-sliced ion velocity map imaging setup in combination with the resonance enhanced multiphoton ionization scheme. Significant changes in the angular distribution for different rovibrational excitations of YO molecules are observed with the collision of Kr. The sharp forward distribution for low rovibrational excitation of YO(v' = 0, 1) molecules suggest that the weak attractive potential between Kr and YO is dominant at large impact parameters. Comparatively, the strong sideway distribution for highly rovibrationally excited YO(v' = 1, 2, 3, and 5) is due to rainbow scattering from the stronger attractive potential of Kr···YO at relatively small impact parameters. The more isotropic angular distribution in the highly rovibrationally excited YO(v' = 11) indicates the formation of a short-lived complex. A change in the angular distribution of scattered YO with different rovibrational excitations was also observed in the collisions of Ne. For YO as a heteronuclear diatomic molecule, collisions of the Y- and the O-end of YO with rare gases would affect the contribution of inelastic processes at different impact parameters.