Dissociative Attachment Research Articles

Theoretical kinetics with one-dimensional fluid model and experimental investigation on coaxial XeCl excilamps

Abstract This paper presents a one-dimensional homogenous model of high power-density XeCl excilamp pumped by dielectric barrier discharge (DBD) with larger discharge gap and lower Cl2 density in Xe/Cl2 mixture, to research the electrical and chemical discharge characteristics leading to the production of XeCl* molecules for the optimal discharge parameters. The peaked wavelength 308 nm from the emission band of XeCl* exciplex molecules, show great promise as photochemotherapy for biomedicine applications. The temporal evolutions of the plasma voltage, current density and the species densities have been analyzed. The model validity has been checked by comparing with the experimental results. It is shown that the XeCl excilamp is a capacitive discharge during the entire voltage cycle and the accumulation of charge deposited in the dielectric surfaces play an extreme role in promoting the extinction of this discharge and the generation of next discharge. The UV radiant efficiency of the DBD XeCl excilamp depends on effect of the discharge behavior on the amplitude of the applied voltage, the total gas pressure, and the Cl2 density. XeCl excilamp has an optimized pressure around 150 mbar with the maximum radiant efficiency of 8.5% for 308 nm from XeCl* molecules and 1.3% for 172 nm from Xe2* molecules. According to the corrected simulation, the radiant efficiency of the optimum pressure is 6.0% for XeCl*molecules. Cl2 density in DBD-based XeCl excilamp strongly influence the balance of electron production and loss due to the dominant dissociative attachment process of electrons to Cl2 molecules, which have significant dependence on the UV light output efficiency. It is demonstrated that the highest XeCl* density occurs near the dielectric during the current pulse. Therefore, electrical and radiant characteristics of XeCl excilamps can be considered as the basis to design the high power-density exciplex lamps in practical applications.

Simulation on the hollow cathode discharge in hydrogen

A rectangular hollow cathode discharge (HCD) in hydrogen with a pressure of 2 Torr is simulated using a 2-D fluid model. The potential, electric field, particle density, and average electron temperature are calculated. The discharge space consists of the cathode sheath region near the cathode electrode and the negative glow (NG) region in the central region of the discharge cell. A high electric field of thousands of V/cm and a low electric field of tens of V/cm appear in the cathode sheath region and NG region, respectively. The average electron temperature in the cathode sheath region is tens of eV, which is significantly higher than that in the NG region. Electrons and H3 + are the main negative particles and positive ions, whose peaks appear in the NG region, and the peak magnitude is on the order of 1010 cm−3. H atom is the highest-density neutral particle other than H2 with a peak density of 1013 cm−3. The reaction kinetics of the generation and consumption of different particles are explored. The results show that each reaction generates certain particles while consuming other particles, ultimately achieving a dynamic equilibrium in the density of various particles. The electrons mainly originate from the ground state ionization between electron and H2 (e+H2 → e+H2 ++e) and are consumed by the dissociative attachment (e+H2 → H−+H). The charge transfer collision reaction (H2 ++H2 → H3 ++H) is the only reaction that produces H3 + ions. Different reactions to the consumption of H3 + ions do not differ significantly. The generation and consumption of H mainly originate from the electron collision dissociation reaction (e+H2 → e+H+H) and the ionization reaction (e+H→H++2e).

Numerical Simulation of the Dynamics of RF Capacitive Discharge in Carbon Dioxide

In this research, the one-dimensional fluid code SIGLO-rf was used to study the internal parameters of RF capacitive discharge in carbon dioxide, focusing mainly on time-averaged and spatio-temporal distributions of discharge parameters. With the help of this code, in the range of distances between electrodes d = 0.04 – 8 cm, RF frequencies f = 3.89 – 67.8 MHz, and values of carbon dioxide pressure p = 0.1 – 9.9 Torr, averaged over the RF period axial profiles of the density of electrons, positive and negative ions were calculated as well as potential and electric field strength. It is shown that the discharge plasma in CO2 contains electrons, positive ions, as well as negative ions. The negative ions of atomic oxygen are formed by the dissociative attachment of electrons to CO2 molecules. Studies of the spatio-temporal dynamics of plasma parameters (electron density, potential and electric field strength, as well as ionization and attachment rates) in RF capacitive discharge in CO2 showed that during half of the RF period, 1 to 3 ionization bursts are usually observed. They correspond to stochastic heating in the near-electrode sheath and the formation of passive and active double layers near the sheath boundaries. The passive double layer appears in the cathode phase and maintains the discharge plasma. The active layer is formed in the anodic phase and ensures a balance of positive and negative charges escaping to the electrode during the RF period. It was found that when the conditions pd = 2 Torr cm and fd = 27.12 MHz cm are met simultaneously, during half of the RF period, 4 intense ionization peaks are observed: resulting from stochastic heating, passive, active, and additional (auxiliary) double layers. The auxiliary double layer helps bring electrons to the surface of the temporary anode and occurs near its surface inside the near-electrode sheath. Using the similarity law, the conditions for the existence of these 4 ionization peaks in a wide range of RF frequencies, carbon dioxide pressures, and distances between electrodes were verified.

Transformer coupled toroidal wave-heated remote plasma sources operating in Ar/NF3 mixtures

Remote plasmas are used in semiconductor device manufacturing as sources of radicals for chamber cleaning and isotropic etching. In these applications, large fluxes of neutral radicals (e.g. F, O, Cl, H) are desired with there being negligible fluxes of potentially damaging ions and photons. One remote plasma source (RPS) design employs toroidal, transformer coupling using ferrite cores to dissociate high flows of moderately high pressure (up to several Torr) electronegative gases. In this paper, results are discussed from a computational investigation of moderate pressure, toroidal transformer coupled RPS sustained in Ar and Ar/NF3 mixtures. Operation of the RPS in 1 Torr (133 Pa) of argon with a power of 1.0 kW at 0.5 MHz and a single core produces a continuous toroidal plasma loop with current continuity being maintained dominantly by conduction current. Operation with dual cores introduces azimuthal asymmetries with local maxima in plasma density. Current continuity is maintained by a mix of conduction and displacement current. Operation in NF3 for the same conditions produces essentially complete NF3 dissociation. Electron depletion as a result of dissociative attachment of NF3 and NF x fragments significantly alters the discharge topology, confining the electron density to the downstream portion of the source where the NF x density has been lowered by this dissociation.

H− production in hydrogen DC glow discharge

The H− ion dynamics in the positive column of H2 DC glow discharge was studied by the laser photodetachment technique in a wide range of pressure, 0.1–3 Torr, and current, 1–30 mA, which cover a range of E/N from ∼40 Td up to ∼170 Td. Using a partial modulation of the discharge current, it is shown that the H−concentration follows H atom dynamics due to a fast detachment reaction with the atoms; the higher the H density, the lower the H–/n e ratio. The dynamics of H atom density during discharge modulation was measured by time-resolved actinometry on Ar atoms, while H2 vibrational temperature was estimated by comparing measured and simulated H2 VUV absorption spectra. The analysis of the experimental dependencies of H− and H/H2 on the discharge parameters allowed estimating the effective rate constant of H− production in the discharge as a function of the reduced electric field. For this discharge model, self-consistent state-to-state vibrational kinetics as well as H2 highly excited electronic states were developed. The main processes that contribute to H− production and loss are discussed in detail. Dissociative attachment to vibrationally excited H2(v) molecules is the main channel of H – production but occurs via the excitation of the well-known low-energy ( ϵ th ≈ 3 eV) shape resonance of H2 −(X2Σu +) only at low E/N. At high E/N, the H– production mostly occurs via the excitation of high-energy H2 − states, such as H2 –(B2Σg +, A2Σg +, C2Πu) and Feshbach resonances similar to H2 −(2Σg +) Rydberg state.

Variability of Ionospheric Total Electron Content Over Morocco During the Godzilla Sand and Dust Storm of June 2020

During sand and dust storm (SDS) events, atmospheric suspension and transport of sand and dust brings a reasonable amount of electrification in the atmosphere which plays a very important role in the atmosphere-ionosphere coupling. The Godzilla SDS began on 5<sup>th</sup> June 2020 in Algeria following a decrease in pressure and spread to other areas across the Sahara between 6<sup>th</sup> and 28<sup>th</sup> June 2020. Using SDS data from Copernicus Sentinel-5P satellite mission and Vertical Total Electron Content (VTEC) data from four GNSS receiver stations: IFR1 (Ifrane Seismic), MELI (Melilla), TETN (Tetouan) and OUCA (Ouca) over Morocco, we investigate the possible ionospheric TEC variability over the four GNSS receiver stations during the Godzilla SDS event which was tracked using the Sentinel-5P Satellite mission. Solar wind parameters: Horizontal component of Interplanetary Magnetic Field (IMF-Bz), interplanetary Electric Field (IEF-Ey) and solar wind speed (V) and geomagnetic indices: Disturbance Storm Time (Dst) and Planetary K (Kp) indices were examined and showed very minimal geomagnetic influence during the period. We observed major ionospheric disturbances over the four Global Navigation Satellite System (GNSS) receiver stations on 16<sup>th</sup>, 17<sup>th</sup>, 18<sup>th</sup>, 21<sup>st</sup>, 22<sup>nd</sup>, 23<sup>rd</sup> 25<sup>th</sup> and 26<sup>th</sup> June 2020: the period with the Sentinel-5P Aerosol Index (SAI) of more than 4 as recorded by the Sentinel-5P Satellite engine. The daily VTEC values over the four GNSS receiver stations recorded continuous electron density perturbations during these days. Apart from the ionospheric TEC perturbations, significant enhancements and decreases in daily maximum VTEC values over the four GNSS receiver stations were also noted. These were attributed to the changes in the atmospheric electric fields generated by the SDS event. The VTEC plots for each day exhibited similar trends, hence exhibited the same ionospheric dynamics. VTEC depletions of depths 3 to 6 TECU over all the four GNSS receiver stations were noted on 12<sup>th</sup>, 14<sup>th</sup>, 17<sup>th</sup>, 20<sup>th</sup> and 25<sup>th</sup> June 2020. Nighttime VTEC enhancements were also noted and majorly occurred between 20:00 and 21:00 UT on 9<sup>th</sup>, 13<sup>th</sup>, 15<sup>th</sup>, 17<sup>th</sup>, 19<sup>th</sup>, 20<sup>th</sup> and 21<sup>st</sup> June 2020. This was attributed to the development of the electron avalanche processes including dust and electron absorption or losses and the active conversion to electron dissociative attachment leading to electron excitation. In conclusion, the Godzilla SDS of June 2020 led to the electron density perturbations over Morocco.

Kinetic insights into ammonia-hydrogen doped ignition and emission assisted by nanosecond pulsed discharge

Non-equilibrium plasma is applied for the first time to ignite the ammonium-hydrogen mixture and reduce the NOx/N2O emission with effect in this work. Gas chromatography (GC) experiments as well as a detailed kinetic model, including neutral molecules, free radicals, charged particles, vibratory excited states, and electron excited states, are integrated to investigate the kinetic process of ammonia-hydrogen doped ignition and NOx/N2O emission facilitated by nanosecond pulsed discharge. The numerical model closely matches the GC-measured values of NH3 consumption, H2 increase, and N2O production. Pathway fluxes of important species and sensitivity analysis of ignition delay time reveal that the addition of non-equilibrium plasma has an obvious promotion effect on ammonia and hydrogen-doped oxidation and ignition. The initial ignition temperature significantly impacts the ignition delay time, with a more pronounced plasma-promotion effect observed at lower temperatures. Conversely, as the hydrogen mixing ratio increases, the ignition delay time decreases, yet the generation of NO and N2O increases. This is attributed to the heightened production of H and NH through elementary reactions such as NH3+HNH2+ H2, H + O2O + OH, and OH + H2H + H2O. Nevertheless, NO and N2O emissions are reduced by 1-2 orders of magnitude with plasma assistance compared to auto-ignition. The reduction in NO emissions can be attributed to increased consumption in the pathway of NO + NH2N2 + H2O and decreased formation in the pathways of HNO + O2HO2 + NO and NH + NON2O + H. Additionally, it was discovered that the electron attachment dissociation reaction e + N2O → O− + N2 predominantly contributes to the reduction of N2O. These research findings significantly contribute to advancing our understanding of the kinetics involved in ammonia-hydrogen doped ignition and emissions, particularly with plasma assistance, for potential engine applications.

Hydrogen isotope effects on recombination dominant plasmas in NAGDIS-II

The detachment processes of the hydrogen (H) and deuterium (D) plasmas are comparatively investigated in the linear plasma device NAGDIS-II. The laser Thomson scattering measurements demonstrate that the recombination rate of the H plasma is greater than that of the D plasma as the neutral pressure increases in the molecular activated recombination (MAR) dominant detachment phase. As the recombination process by MAR is strongly dependent on the vibrational and rotationally excited states of the molecule, the rovibrational quantum state populations of the H and D molecules are measured using the Fulcher-α band spectroscopy. The results indicate that the vibrational temperature in the electronic ground state is considerably higher than the rotational temperature during detachment. The reaction rate coefficients for MARs due to charge exchange chains (CX-MAR) and dissociative attachment chains (DA-MAR) are calculated by the collision-radiation model under the measured temperature conditions. It can be observed that the CX-MAR is larger than the DA-MAR for both H and D, and that the CX-MAR of H is larger than the CX-MAR of D at electron temperatures T e above 1 eV. In consideration of the experimentally observed vibrational and rotational excitation temperatures, the reaction rate coefficients of CX-MAR and DA-MAR are increasing in the low T e region. These calculations are in accordance with the experimental results, which indicate that recombination processes due to MAR are more predominant in the H plasma compared to the D plasma. Furthermore, a transition from MAR to electron–ion recombination processes is observed in the D plasma at T e below 0.5 eV.

On the influence of electrode surfaces on the plasma chemistry of a capacitive chlorine discharge

One-dimensional particle-in-cell/Monte Carlo collisional simulations are performed on capacitive chlorine discharges with 2.54 cm gap rf driven by a sinusoidal with voltage amplitude of 222 V at driving frequency of 13.56 MHz. The properties of the discharge, the reaction rates for creation and loss of a few key species, the electron energy probability function, and the primary electron power absorption processes are explored as the gas pressure and the inclusion of secondary electron emission processes in the discharge model is varied. Five cases are investigated, including and neglecting electron, ion, and fast neutrals induced secondary electron emission. The negative ion Cl− is almost entirely created by dissociative attachment and lost through ion-ion recombination, and therefore the capacitive chlorine discharge is recombination dominated.

Reaction mechanism investigation on Plasma-Assisted steam reforming of toluene based on emission spectrum analysis and kinetic simulation

Plasma-enhanced reforming has been widely studied as an efficient technology for online tar removal. By combining reforming experiments with kinetic modeling and in-situ optical emission spectrometry (OES) analysis, interaction mechanism and coupling rules of plasma/thermal reactions during plasma-assisted steam reforming of toluene were well explored in this study. A chemistry model was innovatively developed for plasma-assisted steam reforming of toluene, and predicted experimental results under different operations conditions with superb agreements. The rate of production and sensitivity analysis implied that OH, H and N2* mainly contributed to primary toluene conversion, while the electronic attachment dissociation of H2O, H addition onto benzene ring and benzyl oxidation by OH were the most enhancing-sensitive reactions. Resultantly, toluene conversion was greatly increased with steam addition before VfH2O = 10 %, but after which VfH2O increase deteriorated the reforming performance due to the inhibition of E-N2 collision by high VfH2O. As temperature increased, plasma and thermal synergistically promoted reforming performance before 300 °C, at which > 60 % toluene was converted into small molecules such as CO, H2 and C2H2, with yields of 23.6 %, 9.4 % and 16.3 % correspondingly at 12 kJ/L, but further temperature increase would not benefit due to the reduced discharge field strength at higher temperatures, being confirmed by the decreased relative intensity of OH, CN feature bands on OES. It was initially proposed that non-thermal plasma governed the reforming process at T < 300 °C, and thermal reactions predominated at T > 500 °C after a transition region (300 ∼ 500 °C). Increase of input energy caused higher discharge field strength, promoted the electronic collision ionization or dissociation of N2 and H2O, thus enhanced toluene conversion and gas yields. A detailed reaction pathway has also been clarified.

Discrimination of Aspartic and Isoaspartic Acid Residues in Peptides by Tandem Mass Spectrometry with Hydrogen Attachment Dissociation.

Long-lived proteins undergo chemical modifications that can cause age-related diseases. Among these chemical modifications, isomerization is the most difficult to identify. Isomerization often occurs at the aspartic acid (Asp) residues. In this study, we used tandem mass spectrometry equipped with a newly developed ion activation method, hydrogen attachment dissociation (HAD), to analyze peptides containing Asp isomers. Although HAD preferentially produces [cn + 2H]+ and [zm + 2H]+ via N-Cα bond cleavage, [cn + 58 + 2H]+ and [zm - 58 + 2H]+ originate from the fragmentation of the isoAsp residue. Notably, [cn + 58 + 2H]+ and [zm - 58 + 2H]+ could be used as diagnostic fragment ions for the isoAsp residue because these fragment ions did not originate from the Asp residue. The detailed fragmentation mechanism was investigated by computational analysis using density functional theory. According to the results, hydrogen attachment to the carbonyl oxygen in the isoAsp residue results in the Cα-Cβ bond cleavage. The experimental and theoretical joint study indicates that the present method allows us to discriminate Asp and isoAsp residues, including site identification of the isoAsp residue. Moreover, we demonstrated that the molar ratio of peptide isomers in the mixture could be estimated from their fragment ion abundance. Therefore, tandem mass spectrometry with HAD is a useful method for the rapid discrimination and semiquantitative analysis of peptides containing isoAsp residues.

Problematic sexual behaviours, dissociation, and adult attachment: A path analysis model

BackgroundProblematic sexual behaviours are controversial phenomena, lacking diagnostic consensus, yet they are significant and warrant in-depth scientific research due to their clinically significant consequences. Therefore, this study aimed to explore the association between potential risk factors of sex addiction and problematic online pornography use, with a specific focus on the role of attachment and dissociation. MethodA sample of 375 participants (Mage = 30 years; SD = 12.441) was involved in the research. The collected data were analysed by implementing a path analysis model. ResultsSignificant and positive total effects in the relationships between fearful/preoccupied attachment patterns and both sex addiction and problematic online pornography use were shown. Furthermore, these associations were significantly mediated by dissociation. Finally, sex addiction and problematic online pornography use were significantly associated with daily thoughts about sex and weekly online pornography use, respectively. LimitationsThe cross-sectional design and the use of only self-report measures in an online survey should be kept in mind while interpreting the results. ConclusionsSuch data provide useful insight into the complex interplay of attachment, dissociation, and problematic sexual behaviours, providing information that may inform and guide targeted clinical interventions.

A 3D kinetic Monte Carlo study of streamer discharges in CO2

We theoretically study the inception and propagation of positive and negative streamers in CO2 . Our study is done in 3D, using a newly formulated kinetic Monte Carlo discharge model where the electrons are described as drifting and diffusing particles that adhere to the local field approximation. Our emphasis lies on electron attachment and photoionization. For negative streamers we find that dissociative attachment in the streamer channels leads to appearance of localized segments of increased electric fields, while an analogous feature is not observed for positive-polarity discharges. Positive streamers, unlike negative streamers, require free electrons ahead of them in order to propagate. In CO2 , just as in air, these electrons are supplied through photoionization. However, ionizing radiation in CO2 is absorbed quite rapidly and is also weaker than in air, which has important ramifications for the emerging positive streamer morphology (radius, velocity, and fields). We perform a computational analysis which shows that positive streamers can propagate due to photoionization in CO2 . Conversely, photoionization has no effect on negative streamer fronts, but plays a major role in the coupling between negative streamers and the cathode. Photoionization in CO2 is therefore important for the propagation of both positive and negative streamers. Our results are relevant in several applications, e.g. CO2 conversion and high-voltage technology (where CO2 is used in pure form or admixed with other gases).

&lt;i&gt;Ab initio&lt;/i&gt; molecular dynamics study on dissociation process of 2-thiouracil and its tautomers under low-energy electron interactions

When biomolecules interact with high-energy particles and rays, they are directly ionized or dissociated, then a large number of low-energy electrons are formed as secondary particles. These low-energy electrons will attach to biomolecules, and trigger off the secondary dissociation, forming free radicals and ions with high reactivity, which can damage the structure and function of the biomolecule and cause irreversible radiation damage to the biomolecule. It is important to study the low-energy dissociative electron attachment (DEA) process of biomolecules for understanding radiation damage to biological organisms. Currently, the theoretical studies of DEA have mainly focused on the bound states of negative ions and the types of resonances in the dissociation process. The dissociation process is well described by quantum computational method, but the diversity and complexity of dissociation channels present in the dissociation process of 2-thiouracil molecule also pose a great computational challenge to these methods. In addition, the quantum computational methods are not ideal for dealing with the discrete states of chemical bonds and the problem of continuity coupling of electrons. The dissociation dynamics of biomolecules mainly results from ionization and electron attachment. &lt;i&gt;Ab initio&lt;/i&gt; molecular dynamics simulation can reasonably describe these processes. In light of these considerations, &lt;i&gt;ab initio&lt;/i&gt; molecular dynamics simulation is used in this work to study dynamic variation process in DEA. The low-energy electron dissociative attachment to 2-thiouracil in the gas phase is studied by using the Born-Oppenheimer molecular dynamics model combined with density functional theory. It is found that an important dehydrogenation phenomenon of 2-thiouracil and its tautomers occurs in the DEA process, and that the N—H and C—H bond are broken at specific locations. Due to the loss of hydrogen atoms at the N and C sites, the closed-shell dehydrogenated negative ion (TU-H)&lt;sup&gt;–&lt;/sup&gt; forms, which is the most important negative ion fragments in the dissociation process. The potential energy curves, the bond dissociation energy and the electron affinity energy of the broken bond show that the N—H bond is the most likely to break, indicating the formation of the negative ion (TU-H)&lt;sup&gt;–&lt;/sup&gt; mainly comes from the breaking of N—H bond. The theoretical calculations in this work are in good agreement with the available experimental results, indicating that the chosen calculation method is fully reliable. ​The BOMD simulations can not only dynamically recover the process of dissociative attachment of low-energy electrons to 2-thiouracil, but also more importantly provide an insight into the mechanisms of dehydrogenation and dissociation channels of 2-thiouracil molecules in DEA process.

Fundamental data for modeling electron-induced processes in plasma remediation of perfluoroalkyl substances.

Plasma treatment of per- and polyfluoroalkyl substances (PFAS) contaminated water is a potentially energy efficient remediation method. In this treatment, an atmospheric pressure plasma interacts with surface-resident PFAS molecules. Developing a reaction mechanism and modeling of plasma-PFAS interactions requires fundamental data for electron-molecule reactions. In this paper, we present results of electron scattering calculations, potential energy landscapes and their implications for plasma modelling of a dielectric barrier discharge in PFAS contaminated gases, a first step towards modelling of plasma-water-PFAS intereactions. It is found that the plasma degradation of PFAS is dominated by dissociative electron attachment with the importance of other contributing processes varying depending on the molecule. All molecules posses a large number of shape resonances - transient negative ion states - from near-threshold up to ionization threshold. These states lie in the region of the most probable electron energies in the plasma (4-5 eV) and consequently are expected to further enhance the fragmentation dynamics in both dissociative attachment and dissociative excitation.

Numerical simulation of inductively coupled Ar/O&lt;sub&gt;2&lt;/sub&gt; plasma

In the inductively coupled plasma (ICP) discharge, surface processes, such as reflection, de-excitation, and recombination, can occur when active species arrive at material surfaces, which accordingly influences the plasma properties. In this work, a fluid model is used to study the Ar/O&lt;sub&gt;2&lt;/sub&gt; plasma generated by ICP reactors made of different materials. In simulation, sticking coefficient is employed to estimate the surface reactions on different materials. As the reactor material changes from stainless steel to anodized aluminum to Cu, the sticking coefficient of surface reaction O→1/2O&lt;sub&gt;2&lt;/sub&gt; decreases accordingly. It is found that the reactor material has a great effect on species density. In the stainless steel reactor, the density of O atoms at grounded state and excited state are much lower because more O&lt;sub&gt;2&lt;/sub&gt; molecules are generated from the surface reaction, yielding a much higher density of &lt;inline-formula&gt;&lt;tex-math id="M5"&gt;\begin{document}$ {\text{O}}_2^ + $\end{document}&lt;/tex-math&gt;&lt;alternatives&gt;&lt;graphic specific-use="online" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M5.jpg"/&gt;&lt;graphic specific-use="print" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M5.png"/&gt;&lt;/alternatives&gt;&lt;/inline-formula&gt; molecular ions which are mainly created from the ionization process of O&lt;sub&gt;2&lt;/sub&gt; molecules. Similarly, the high density of O&lt;sub&gt;2&lt;/sub&gt; molecules also enhances the production of &lt;inline-formula&gt;&lt;tex-math id="M6"&gt;\begin{document}${{{\mathrm{O}}} _2}\left( {{{\mathrm{a}}^1}{\Delta _{\mathrm{g}}}} \right)$\end{document}&lt;/tex-math&gt;&lt;alternatives&gt;&lt;graphic specific-use="online" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M6.jpg"/&gt;&lt;graphic specific-use="print" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M6.png"/&gt;&lt;/alternatives&gt;&lt;/inline-formula&gt; molecules through the excitation process and O&lt;sup&gt;–&lt;/sup&gt; ions through the dissociation attachment reaction. On the contrary, more electrons are consumed via the collisions between electrons and O&lt;sub&gt;2&lt;/sub&gt; molecules or &lt;inline-formula&gt;&lt;tex-math id="M7"&gt;\begin{document}$ {\text{O}}_2^ + $\end{document}&lt;/tex-math&gt;&lt;alternatives&gt;&lt;graphic specific-use="online" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M7.jpg"/&gt;&lt;graphic specific-use="print" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M7.png"/&gt;&lt;/alternatives&gt;&lt;/inline-formula&gt; molecular ions. Therefore, the electron density obtained in the Cu reactor is highest. The density of Ar&lt;sup&gt;+&lt;/sup&gt; ions and Ar&lt;sub&gt;m&lt;/sub&gt; atoms also increase with sticking coefficient decreasing. The density of O&lt;sup&gt;+&lt;/sup&gt; ions and &lt;inline-formula&gt;&lt;tex-math id="M8"&gt;\begin{document}$ {\text{O}}_2^ + $\end{document}&lt;/tex-math&gt;&lt;alternatives&gt;&lt;graphic specific-use="online" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M8.jpg"/&gt;&lt;graphic specific-use="print" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M8.png"/&gt;&lt;/alternatives&gt;&lt;/inline-formula&gt; molecular ions peak below the coil in the stainless steel reactor, whereas the radial uniformities are improved in the Cu reactor. In the three reactors, the electrons distribute evenly at the reactor center region. The O density and &lt;inline-formula&gt;&lt;tex-math id="M9"&gt;\begin{document}${{{\mathrm{O}}} _2}\left( {{{\mathrm{a}}^1}{\Delta _{\mathrm{g}}}} \right)$\end{document}&lt;/tex-math&gt;&lt;alternatives&gt;&lt;graphic specific-use="online" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M9.jpg"/&gt;&lt;graphic specific-use="print" xmlns:xlink="http://www.w3.org/1999/xlink" xlink:href="13-20240436_M9.png"/&gt;&lt;/alternatives&gt;&lt;/inline-formula&gt; density significantly peak at the reactor center, while the maximum value of Ar&lt;sup&gt;+&lt;/sup&gt; density and Ar&lt;sub&gt;m&lt;/sub&gt; density are below the coil. As for O(&lt;sup&gt;1&lt;/sup&gt;D), the maximum density below the coil region moves toward the reactor center as the reactor material changes from stainless steel to Cu. Finally, the effect of sticking coefficient of O→1/2O&lt;sub&gt;2&lt;/sub&gt; is studied. The results show that the O atom density decreases with the sticking coefficient increasing, but the opposite trend is observed in O&lt;sub&gt;2&lt;/sub&gt; molecular density. It is noticed that the sticking coefficient has little effect on species density when it is higher than 0.5.

Two- and three-body attachment, electron transport and ionisation in water-air mixtures

Three-body electron attachment in the mixtures of H2O and dry air have been measured over a wide range of the density-reduced electric field, E/N, from 3–130 Td and gas pressures, for mixture combinations ranging from 1% to 50% of H2O. We have measured the regions of three-body attachment (3–30 Td) and two-body dissociative attachment (40–130 Td). Besides, the increasing amount of H2O in the mixture causes an increase in the three-body reaction rates of up to two orders of magnitude in comparison with that measured for dry air. On the other hand, the three-body attachment coefficients exceed the two-body ones (dissociative attachment) at high pressures. Good agreement has been found with previous measurements of H2O-dry air mixtures with H2O concentrations of up to 2%. We know of no previous work for higher H2O concentrations. Values of the effective ionisation coefficients and longitudinal diffusion coefficients derived from the same measurements are also presented.

Nitrogen Reduction to Ammonia on a Fe16 Nanocluster: A Computational Study of Catalysis.

The sequence of elementary steps leading to reductive ammonia formation from N2 and H2 catalyzed by a Fe16 cluster is studied using generalized gradient approximation density functional theory and an all-electron basis set of triple-ζ quality. The computational methods are validated by comparison to experimental data such as binding energies where possible. First, the associative and dissociative attachment of N2 to Fe16 is considered, followed by exploration of the pathways leading to distal (Fe16-N-NH2) and enzymatic (NFe16-NH2) formation of an amino group. Next, the pathways leading to NH3 formation in both distal and enzymatic cases are examined. Two mechanisms for NH3 detachment have been discovered. An interesting peculiarity of the pathways is that they often proceed with total spin fluctuations, which are related to the rupture and formation of bonds on the surface of the catalyst over the course of the reactions. The reaction Fe16 + N2 + 2H2 → Fe16NH + NH3 is found to be exothermic by 1.02 eV (93.8 kJ/mol).

Study of the efficiency of ozone synthesis in a point‐to‐plain discharge in N2–O2 mixtures

AbstractThe experimental results of the ozone synthesis and electrodynamic characteristics of the point‐to‐plane DC voltage corona discharge in N2–O2 mixtures at atmospheric pressure are presented. Four different modes of DC corona discharge were investigated: stationary mode of positive point‐to‐plane discharge, two non‐stationary (streamers) modes of positive point‐to‐plane discharge, and mode of negative point‐to‐plane discharge. It was shown that ozone synthesis highly depends on discharge modes and correlates with discharge conditions appropriated to dissociative attachment processes. In the case of positive point‐to‐plane discharge, ozone synthesis behavior is similar to that of the pulse component of the discharge current. It was shown that the mode with secondary streamers propagation is the most effective for ozone production among the four different modes of the point‐to‐plane DC corona discharge.

Correlation of H- beam properties to Cs-coverage

A caesiated RF driven source delivers H- ions that, after stripping at the end of the 160 MeV H- linear injector, provides protons to CERN's accelerator complex including LHC, where the protons reached a record energy of 6.8 TeV. In Caesiated RF sources, H- ions are produced via dissociative attachment of electrons onto roto-vibrationally excited H2-molecules (volume) and re-emission as negative ions of protons or hydrogen atoms colliding on a low work function caesiated molybdenum plasma electrode (surface). During initial caesiation, the production mechanism evolves from the initial Cs-free volume production to a predominant surface production mode; the observed stunning reduction of co-extracted electrons is concomitant to an increase of the H- ion current to RF-power yield. This paper describes the evolution of the beam-profile at today's operational beam intensities of 35 mA for various ratios of volume and surface ion-origin. The presence of surface produced ions occurring on a conical plane is characterized by the electron to ion ratio and by measurement of the Cs-coverage of the molybdenum plasma electrode down to a fraction of a monolayer. Angular distributions are extracted from beam profile and Beam Emission Spectroscopy (BES) measurements. These experimental results provide an initial comparison to beam formation simulation that, at a later stage, could be coupled to beam transport software packages.The paper focuses on the caaesiation transient to present experimental evidence for 3D beam formation studies, it provides insight into the mixing of volume and surface production modes, reduction of co-extracted electrons and Cs-coverage. The paper also establishes magnetic field induced asymmetries in the beam's current density.