Ground State Of Ion Research Articles

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).

The linear Paul Trap's Confined Stability Area for 40Ca+ Ions

تقدم تكنولوجيا الكم طرقًا حسابية واتصالات ومحاكاة وقياسًا جديدة. تحتاج أجهزة الكمبيوتر التقليدية إلى المساعدة في حل المشكلات المهمة مثل التحليل بسبب الزيادات الهائلة في وقت الحساب. ومع ذلك، تستخدم أجهزة الكمبيوتر الكمومية ميكانيكا الكم لحجم المشكلة الأسي الفرعي ويمكنها محاكاة الطبيعة على المستوى الكمي. يهتم العلماء بشكل متزايد بتطوير أجهزة الكمبيوتر الكمومية باستخدام ذرات متأينة مفردة في مصائد باولي. تمثل الحالة الأساسية لكل أيون أقل قيمة ممكنة للبت الكمي. تم استخدام الأيونات المحتجزة 40Ca+ في إحدى الدراسات كمثال على الكيوبت الكمومي. تم استخدام برنامج MATLAB على العوامل النموذجية التي تؤثر على الحالة المقيدة وتأثيراتها. يجب أن تكون الحلول مستقرة في كلا الاتجاهين، مما يتطلب حصرًا ثلاثي الأبعاد لمعادلة ماثيو. تؤثر المتغيرات على المسافة من مركز المصيدة لنهاية القطب، وجهد UDC، وكتلة الأيون، والترددات الراديوية. تم استخدام جهد متغير للتحكم وإظهار تأثيره على سلسلة محددة من الأيونات المحاصرة. يهدف هذا البحث إلى فهم أفضل للظروف المثلى للحجز وحركة الأيونات من الحالة (4S1/2) إلى الحالة (4P1/2) بالرنين. تخضع الحالة الكمومية للتعديل والتغيير، مما يجعلها أداة واعدة لحل المشكلات المعقدة.

Investigating quantum coherence of N-methylpyrrole through vibrational spectroscopy and potential energy: A theoretical study

Quantum chemical calculations are utilized to analyze the potential causes of N-methylpyrrole oscillations, focusing on vibration spectra and potential energy curves. Optimization of the ground state, ionic state and 3s state structure reveal mostly sp2 hybridization. An analysis of the 3s state vibration spectrum and adiabatic binding energy indicate that changes in dihedral angles D2,3,4,1 and plane angle A3,2,1 are potential factors contributing to molecular oscillations. The role of vertical binding energy and adiabatic binding energy in the oscillation process are also discussed, shedding light on the possible dynamic processes of N-methylpyrrole.

Fluid simulation of atmospheric argon RF dielectric barrier discharges: Role of neutral gas temperature

For atmospheric argon RF dielectric barrier discharges, a self-consistent one-dimensional fluid model based on the drift-diffusive approximations of the particles is established to investigate the role of the neutral gas temperature on the discharge process and the plasma characteristics. A finite difference method is used to solve numerically the model, and the numerical results are obtained for the cases that the neutral gas temperature varies from 300 to 600 K. It shows that an increase in the neutral gas temperature causes a decrease in the ionization rate peak and a decrease in the plasma density, but the electric field and the electron temperature do not change very much. Moreover, the discharge mode transition from α mode to α-γ mode occurs because the growing ion flux induces more secondary electron flux, even if the ions entering the sheaths decrease. In addition, the ground state ionization and the ground state excitation are the main collisions in the argon discharges. When metastable atoms are focused on, the three-body quenching is also an important collision progress.

Ternary recombination of excited Ar+(P1/22) ions, established experimental results reinterpreted with a new extended model.

For many years, the recombination of excited ions of argon, Ar+(P1/22), has been assumed negligible under ambient conditions as compared to the recombination of ground-state ions, Ar+(P3/22). This opinion was confronted with detailed experimental results that seem to clearly support it. Here, we propose a new interpretation in light of our recent calculations, which shows that the recombination efficiency is comparable for both fine-structure states. Noteworthily, in our model leading to a picture consistent with the experiment, residual dimer ions emerge from Ar+(P1/22) due to non-adiabatic dynamics effects and interplay in measured data.

Formation of Ar2+ ions in cold argon plasmas through the ternary recombination mechanism

A general scheme for calculating ternary recombination rate constants of atomic species based on a hybrid quantum–classical nonadiabatic dynamics approach is presented and applied to the specific case of the ternary recombination of atomic ions of argon in cold argon plasmas. Rate constants are reported for both fine-structure states of the Ar+ ion, 2P3/2 and 2P1/2 , T = 300 K, and for selected values of the reduced electric field. A thorough comparison with the literature data available for T = 300 K and a couple of close temperatures is performed with a favorable agreement achieved. It is shown that the excited Ar+(2P1/2) ions may contribute to the formation of dimer ions, Ar2+ , as efficiently as the ground-state ions, Ar+(2P3/2) , due to fast internal conversion of the electronic energy, which takes place in ternary collision complexes, Ar+/Ar/Ar .

Ground state property calculations of LiHn complexes using IBM Qiskit’s quantum simulator

In this study, the variational quantum eigensolver (VQE) on a quantum simulator is used in calculating ground state electronic structure properties of the LiHn, n = 1–3, complexes including their singly charged ions. Results calculated using classical electronic structure algorithms are also included. We investigate the use of the unitary coupled cluster with singles and doubles (UCCSD) Ansatz using VQE within Qiskit and compare results to full configuration interaction (FCI) calculations. Computed ground state energies, electron affinities, ionization potentials, and dipole moments are considered. We report the first-of-its-kind simulated quantum computing results of selected LiHn species and use the parity orbital to qubit mapping scheme. We find that VQE/UCCSD results are comparable to classical coupled clusters with singles and doubles for all considered systems with respect to FCI. A VQE calculation cost evaluation is included in which we evaluate performance using both Jordan–Wigner and parity orbital to qubit mapping schemes. We also discuss some of the current limitations of utilizing VQE for the study of chemical systems.

Oxygen Hole Formation Controls Stability in LiNiO2 Cathodes: DFT Studies of Oxygen Loss and Singlet Oxygen Formation in Li-Ion Batteries

Ni-rich cathode materials achieve both high voltages and capacities in Li-ion batteries but are prone to structural instabilities and oxygen loss via the formation of singlet oxygen. Using ab initio molecular dynamics simulations, we observe spontaneous O2 loss from the (012) surface of delithiated LiNiO2, singlet oxygen forming in the process. We find that the origin of the instability lies in the pronounced oxidation of O during delithiation, i.e., O plays a central role in Ni-O redox in LiNiO2. For LiNiO2, NiO2, and the prototype rock salt NiO, density-functional theory and dynamical mean-field theory calculations based on maximally localised Wannier functions yield a Ni charge state of ca. +2, with O varying between –2 (NiO), –1.5 (LiNiO2) and –1 (NiO2). Predicted XAS Ni K and O K-edge spectra are in excellent agreement with experimental XAS spectra, confirming the predicted charge states. The calculations also show that a high-voltage O K-edge feature at 531 eV previously assigned to lattice O-redox processes could alternatively arise from O-redox induced water intercalation and O–O dimer formation with lattice O at high states of charge. The O2 surface loss route observed here consists of 2 surface O•– radicals combining to form a peroxide ion, which is oxidised to O2, leaving behind 2 O vacancies and 2 O2– ions: effectively 4 O•– radicals disproportionate to O2 and 2 O2– ions. The reaction liberates ca. 3 eV per O2 molecule. Singlet oxygen formation is caused by the singlet ground state of the peroxide ion, with spin conservation dictating the preferential release of 1O2, the strongly exergonic reaction providing the free energy required for the formation of 1O2 in its excited state.

Theoretical investigation of electron-impact ionization of W8+ ion

The electron-impact single ionization cross section for W8+ ion has been calculated using flexible atomic code, employing the level-to-level distorted-wave approximation. This calculations takes into account contributions form both direct ionization (DI) and excitation autoionization (EA). However, the theoretical predictions, based solely on the ground state, tends to underestimate the experimental values. This discrepancy can be mitigated by incorporation contributions from excited states. We extended the theoretical analysis, including the contributions from the long-lived metastable states with lifetimes exceeding 1.5 × 10−5 s. We employed two statistical models to predict the fraction of ground state ions in the parent ion beam. Assuming a 79% fraction of parent ions in ground configuration, the experiment measurements align with the predictions. Furthermore we derived the theoretical cross-section for the ground state as correlated plasma rate coefficients, and compared it with existing data. Despite the uncertainty in our calculations, our results are still acceptable.

Vibrational transitions of [formula omitted]: Potential energy surface and anharmonic computations

A new three-dimensional potential energy surface of the electronic ground state of the chloronium ion, H2Cl+, based on the explicitly correlated coupled cluster method with a triple zeta basis set adapted to this method has been expanded in an analytical representation. This potential energy surface is later incorporated into our home-made Fortran code to compute variationally the vibrational levels, zero-point ground average structural parameters and the rotational constants of the chloronium ion and several isotopologues. Our results show a good agreement with experimental data and that our results will help to detect H2Cl+ isotopologues in the interstellar medium.

A switch from ferro- to antiferromagnetic ordering in the solid solutions CeAuGe1−x Sn x

Abstract CeAuGe and CeAuSn (both NdPtSb type, space group P63 mc) form a complete solid solution CeAuGe1−x Sn x with Vegard-type behavior of the cell volume. Samples with steps of x = 0.1 were synthesized from the pure elements by arc-melting. The structure of CeAuGe0.13(2)Sn0.87(2) was refined from single-crystal X-ray diffractometer data: a = 469.10(6), c = 773.90(10) pm, wR 2 = 0.0359, 251 F 2 values and 12 variables. The induced structural disorder caused by the Ge/Sn mixing affects the magnetic ground state of the cerium ions. From the germanium-rich side, the Curie temperature of CeAuGe (10.0 K) decreases towards CeAuGe0.6Sn0.4, while the Néel temperature of CeAuSn (4.4 K) decreases at the tin-rich side toward CeAuGe0.4Sn0.6. The switch of the magnetic ground state occurs approximately around the Ge/Sn ratio of 1:1. 119Sn Mössbauer spectra of CeAuGe0.1Sn0.9 and CeAuGe0.7Sn0.3 confirm the presence of single crystallographic tin sites in both cases, and the isomer shifts are comparable to that of pure CeAuSn, indicating similar electron density distribution at the tin nuclei.

The Role of Stepwise Photoionization in Measurements of the Ionization Potentials in Dense Plasma

The interaction of high-contrast high-intensity laser radiation with solids allows us to create hot or warm plasma of solid or even over-solid density, such as in the case of inertial fusion particularly. The multicharged ions contained in it can no longer be considered isolated. As a result, this leads to a decrease in the ionization potentials and to the disappearance of a number of bound ionic states. To describe the ionization potential depression, two major approaches are now used predominantly, where the key parameter is either average interelectronic or interionic distance. Since neither of the approaches can be substantiated purely theoretically, their applicability can only be established by comparison with experimental results. In recent experiments with X-ray free-electron lasers, it was concluded that the ionization potential depression rather depends on the interelectronic distance. However, when measuring ionization potentials, it was assumed that the main role in ionization processes is played by the direct photoionization of the ion ground state. In the present paper, we show that stepwise photoionization processes should play a significant role in dense plasma, disrupting a straight correspondence between the threshold in direct photoionization by X-ray laser photons and the actual ionization potential of multicharged ions. It means that the measurement results mentioned above are not correct, and the main conclusion about the importance of the interelectronic distance for depression of the ionization potential is not correct.

H2 formation via non-Born-Oppenheimer hydrogen migration in photoionized ethane

Neutral H2 formation via intramolecular hydrogen migration in hydrocarbon molecules plays a vital role in many chemical and biological processes. Here, employing cold target recoil ion momentum spectroscopy (COLTRIMS) and pump-probe technique, we find that the non-adiabatic coupling between the ground and excited ionic states of ethane through conical intersection leads to a significantly high yield of neutral H2 fragment. Based on the analysis of fingerprints that are sensitive to orbital symmetry and electronic state energies in the photoelectron momentum distributions, we tag the initial electronic population of both the ground and excited ionic states and determine the branching ratios of H2 formation channel from those two states. Incorporating theoretical simulation, we established the timescale of the H2 formation to be ~1300 fs. We provide a comprehensive characterization of H2 formation in ionic states of ethane mediated by conical intersection and reveals the significance of non-adiabatic coupling dynamics in the intramolecular hydrogen migration.

Applying machine learning methods for the analysis of two-dimensional mass spectra

In a measurement of isomeric yield-ratios in fission, the Phase-Imaging Ion-Cyclotron-Resonance technique, which projects the radial motions of ions in the Penning trap (JYFLTRAP) onto a position-sensitive micro-channel plate detector, has been applied. To obtain the yield ratio, that is the relative population of two states of an isomer pair, a novel analysis procedure has been developed to determine the number of detected ions in each state, as well as corrections for the detector efficiency and decay losses. In order to determine the population of the states in cases where their mass difference is too small to reach full separation, a Bayesian Gaussian Mixture model was implemented. The position-dependent efficiency of the micro-channel plate detector was calibrated by mapping it with ^{133}Cs^+ ions, and a Gaussian Process was trained with the position data to construct an efficiency function that could be used to correct the recorded distributions. The obtained numbers of counts of excited and ground-state ions were used to derive the isomeric yield ratio, taking into account decay losses as well as feeding from precursors.

High-precision Ramsey-comb spectroscopy on molecular deuterium for tests of molecular quantum theory

Precision spectroscopy of simple, calculable molecules has become an important tool to compare experiments with theory in an effort to test our understanding of the fundamental laws of physics. For this purpose, we have measured the transition frequency of molecular deuterium () with unprecedented accuracy. We use Ramsey-Comb spectroscopy at deep-ultraviolet wavelengths (201 nm) with a two-photon, Doppler-free interrogation scheme. The resulting transition frequency is kHz. The 1-σ uncertainty of 19 kHz represents an improvement of more than two orders of magnitude compared to the best previous measurement. In this paper, we give an extensive description of our methods and the experimental apparatus that we employed. Particular attention is given to aspects that we recently improved, such as the frequency comb laser system, the method of signal recording, and the cryogenic molecular beam apparatus. In combination with future measurements of the ionisation energy of the EF state, our measurement paves the way for an improved determination of the ground state ionisation and dissociation energy of molecular deuterium.

Interference between dielectronic and radiative recombination of Be-like highly charged ions

We perform a systematical study for the polarization of x rays emitted when a free electron is captured by Be-like highly charged ions theoretically. We focus on the dielectronic recombination of the $J=1/2\ensuremath{\rightarrow}J=1/2$ transition and its polarization is zero due to axial symmetry. Including the interference between the dielectronic and radiative recombinations, the polarization changes dramatically when the electron energy crosses the resonant energy. By comparing the simulations with or without certain interactions, we found that the Breit interaction is not important even for very high-$Z$ ions. For low-$Z$ ions, the configuration interaction of the dielectronic recombination states affects the polarization greatly, while for high-$Z$ ions the configuration interaction of the ground state of Be-like ions plays an important role.

The vacuum UV photoabsorption spectrum of 1,1-dibromo-2,2-difluoroethylene (1,1-Br2C2F2) in the 5-15 eV photon energy range. Combining experimental and theoretical investigations

Using synchrotron radiation, we have measured the vacuum UV photoabsorption spectrum (PAS) of 1,1-Br2C2F2 for the first time between 5 eV and 15 eV photon energy. Quantum chemical calculations have been performed for the determination of excitation and ionization energies. At low energy a weak broad band spreads between 5.2 eV and 6.0 eV and is assigned to nBr→Rpz (31B2) valence transition. A broad continuum starting at 6.18 eV corresponds to the π(3b1)→5s (41B1) Rydberg transition. Starting at Eexcad=6.595 eV a group of four narrower peaks likely corresponds to the vibrational excitation of the characteristic π(3b1)→π*(71A1) valence transition. The features evenly spaced by 1315 cm−1 are assigned to the C=C stretching vibration. Between 7.0 eV and 11.5 eV, several weak or very strong sharp features are observed. The 3b1→5p Rydberg transition is characterized by a short progression starting at 7.208 eV. A longer progression, assigned to 3b1→4d Rydberg transition, is observed up from 7.932 eV. Both Rydberg states converge to the X˜2B1 ionic ground state calculated at IEad=9.40 eV with quantum defects δ=2.51 and δ=0.96 respectively. The vibrational analysis provides vibrational wavenumbers ω1=1525±20 cm−1, ω2=975±40 cm−1, ω3=620±40 cm−1, ω4=355±20 cm−1 and ω5=185±30 cm−1 averaged over the 5p and 4d Rydberg states. An interaction has likely to be considered between the 6s and 4d Rydberg states. Above 11.5 eV, several strong sharp and broad bands are tentatively assigned to transitions to Rydberg states converging to excited ionic states of 1,1-Br2C2F2+. For one of these a vibrational structure is observed and a tentative assignment is proposed.

Vacuum UV photoabsorption spectroscopic and photoionization mass spectrometric study of geminal dibromoethylene (1,1-Br2C2H2) in the 5–15eV range. Experiment and theory

The vacuum UV photoabsorption spectrum (PAS) of 1,1-C2H2Br2 has been examined between 5 eV and 15 eV using the vacuum UV light of synchrotron radiation. For the first time the photoionization mass spectroscopy and efficiency of 1,1-C2H2Br2+ has been measured in the same energy range. A quantum chemical calculation is proposed for the investigation of the neutral and ionized states. The photoionization efficiency curve (PIEC) of 1,1-C2H2Br2+ provided the IEad(X˜2B1)= 9.617±0.005 eV. A vibrational structure gave ω3+=1336 cm−1 and most likely ω4+=483 cm−1. The PIEC of C2H2Br+ shows the lowest appearance energy to be at 11.14±0.02 eV. The onset at 11.56±0.01 eV likely corresponds to the excitation of Br in the 2P1/2 spin-orbit state. In the vacuum UV-PAS the broad band observed at 6.231 eV includes nσ→Rs, 2b1(π)→π* valence transitions and the 2b1→3 s Rydberg transition in agreement with the present calculations. An isolated weak continuum at 7.15 eV is assigned to the nπ→π* transition. The 2b1→3 s Rydberg transition is characterized by a short progression starting at 6.583 eV. A series of long progressions observed between 7.364 eV and 9.666 eV has been analyzed in terms of vibrational transitions to np- (δ= 0.544) and nd-type (δ= -0.04) Rydberg states all converging to the X˜2B1 ionic ground state. An analysis has been attempted providing average values of the vibrational wavenumbers ω3≈1300 cm−1 (or 162 meV), ω4≈480 cm−1 (or 60 meV) and ω5≈145 cm−1 (or 18 meV). By the same way several other Rydberg states were analyzed. For the first time the vacuum UV spectrum of 1,1-C2H2Br2 has been recorded above 10 eV and up to 15 eV. Several broad bands are tentatively assigned to transitions to Rydberg states converging to excited ionic states of 1,1-C2H2Br2+. For one of these a vibrational structure is observed and a tentative assignment is proposed.

Near-thermo-neutral electron recombination of titanium oxide ions.

While the dissociative recombination (DR) of ground-state molecular ions with low-energy free electrons is generally known to be exothermic, it has been predicted to be endothermic for a class of transition-metal oxide ions. To understand this unusual case, the electron recombination of titanium oxide ions (TiO+) with electrons has been experimentally investigated using the Cryogenic Storage Ring. In its low radiation field, the TiO+ ions relax internally to low rotational excitation (≲100 K). Under controlled collision energies down to ∼2 meV within the merged electron and ion beam configuration, fragment imaging has been applied to determine the kinetic energy released to Ti and O neutral reaction products. Detailed analysis of the fragment imaging data considering the reactant and product excitation channels reveals an endothermicity for the TiO+ dissociative electron recombination of (+4 ± 10) meV. This result improves the accuracy of the energy balance by a factor of 7 compared to that found indirectly from hitherto known molecular properties. Conversely, the present endothermicity yields improved dissociation energy values for D0(TiO) = (6.824 ± 0.010)eV and D0(TiO+) = (6.832 ± 0.010)eV. All thermochemistry values were compared to new coupled-cluster calculations and found to be in good agreement. Moreover, absolute rate coefficients for the electron recombination of rotationally relaxed ions have been measured, yielding an upper limit of 1 × 10-7 cm3 s-1 for typical conditions of cold astrophysical media. Strong variation of the DR rate with the TiO+ internal excitation is predicted. Furthermore, potential energy curves for TiO+ and TiO have been calculated using a multi-reference configuration interaction method to constrain quantum-dynamical paths driving the observed TiO+ electron recombination.

Ionic Liquid Induced p-Nitrophenol prototropism

The manuscript “Ionic Liquid Induced p-Nitrophenol Prototropism” deals with the acid-base properties of p-Nitrophenol molecule in the presence of two different Ionic Liquids (ILs). Prototropic equilibria of p-Nitrophenol (PNP) have been studied in water, ethanol, carbon tetrachloride, chloroform, cyclohexane and IL added aqueous solution with the help of Uv-vis absorbance spectroscopy. It was found that PNP mainly exists in neutral form when dissolved in ethanol, carbon tetrachloride, chloroform and cyclohexane. Interestingly, ground state ionization of PNP takes place in water and results into the formation of p-Nitrophenolate anion as a result of proton transfer to water and hence two absorbing species have been detected in the absorbance spectra. Inter-conversion of neutral to anionic and vice versa can be achieved with the addition of small amount of NaOH/HCl. Furthermore, in water/ethanol binary mixture both neutral and anionic forms exist. Interactions of surfactants sodium dodecyl sulfate (SDS) and cetrimonium bromide (CTAB) with neutral and ionic forms of PNP is also explored. To assess the potential role of ILs as a solubilizing media that facilitates proton-transfer reactions, p-Nitrophenol prototropism is investigated in water in the presence of small amount of added ILs. Interestingly, addition of small amount of hydrophilic IL, 1-butyl-3-methylimidazolium tetrafluoroborate [bmim][BF4] or hydrophobic IL, 1-butyl-3-methylimidazolium hexafluorophosphate [bmim][PF6] into PNP dissolved in high pH water causes protonation of the already present p-Nitrophenolate anion. Protonation of p-Nitrophenolate is attributed due to presence of acidic C2-H protons in [bmim]+ cations associated with both ILs. Furthermore, the extent of protonation induced by addition of [BF4]− based IL is found to be much pronounced as compared to [PF6]− based IL having same cation due to difference in hydrolytic properties of [BF4]− based ILs when compared with [PF6]− based ILs. These findings could contribute to the technological applications for detection, removal and sensing of environmentally hazardous p-Nitrophenol and its ionic forms from water. The results presented in this work lead to a better understanding of prototropic behavior of PNP in IL based media as well as different organic solvents based media.