Ion Molecule Research Articles

Level structure of hole two-center complex and related luminescence in semiconductors

Real semiconductors usually contain both donor and acceptor impurities. A finite compensation degree leads to the possibility of the single carrier to be bounded by two impurity centers. For such an electron complex (near a simple conduction band), the spectral problem resembles the hydrogen molecule ion problem (up to renormalization of the effective mass and dielectric screening). In $p$-type semiconductors, the spectral problem for a single hole in the field of two attracting centers (${A}_{2}^{\ensuremath{-}}$ complex) is more complicated due to the complex structure of the valence band. Here such a problem is presented for the case of the hole bounded at two shallow acceptors close to the ${\mathrm{\ensuremath{\Gamma}}}_{8}$ valence band edge (${\mathrm{A}}^{\mathrm{III}}{\mathrm{B}}^{\mathrm{V}}$ or group $\mathrm{IV}$ semiconductors). The multicomponent envelope functions are used to develop quantum chemistrylike approach (molecular orbital method). The variational approach is applied to calculate the level structure of the complex. The states of the complex are classified by the total angular momentum projection onto the intercenter axis and by the parity with respect to the intercenter permutation. The ground state has a total angular momentum projection of $\ifmmode\pm\else\textpm\fi{}1/2$ and a wave function that is symmetric with respect to the intercenter permutation. The energy levels are found as a function of the intercenter distance. A possible manifestation of ${A}_{2}^{\ensuremath{-}}$ complexes in acceptor-related luminescence is discussed.

Roles of the Zinc Ion and Water Molecule in the Active Site of the Copper-Zinc SOD Catalyst

In this work, we study the effect of a water molecule and a zinc ion on the catalytic activity of copper-zinc superoxide dismutase by computer simulation at the level of density functional theory using the PBE functional and the def2-SVPD and def2-TZVPD basis sets. Assessment is carried out in two directions. The first is a comparison of the main characteristics of electron transfer according to Marcus in the presence and absence of a water molecule in the active site. The second is the topological analysis of the electron density of the ligand environment of the copper ion according to Bader. It has been found that the presence of a water molecule and a zinc ion next to a copper ion has little effect on the primary stage of catalysis, the reduction of the copper ion. However, their presence significantly affects the course of the second stage of the catalytic cycle in the oxidation of copper. The water molecule is involved as a proton carrier. It may be present next to the copper ion during primary electron transfer. The water molecule leaves the first coordination sphere of copper after the initial electron transfer; otherwise, it forms a strong bond with the nitrogen atom, interrupting the electron transfer, according to the topological analysis. The presence of a water molecule near copper significantly impairs the secondary electron transfer, and the catalytic cycle is generally blocked.

Effect of Polymer Hydrophobicity in the Performance of Hybrid Gel Gas Sensors for E-Noses.

Relative humidity (RH) is a common interferent in chemical gas sensors, influencing their baselines and sensitivity, which can limit the performance of e-nose systems. Tuning the composition of the sensing materials is a possible strategy to control the impact of RH in gas sensors. Hybrid gel materials used as gas sensors contain self-assembled droplets of ionic liquid and liquid crystal molecules encapsulated in a polymeric matrix. In this work, we assessed the effect of the matrix hydrophobic properties in the performance of hybrid gel materials for VOC sensing in humid conditions (50% RH). We used two different polymers, the hydrophobic PDMS and the hydrophilic bovine gelatin, as polymeric matrices in hybrid gel materials containing imidazolium-based ionic liquids, [BMIM][Cl] and [BMIM][DCA], and the thermotropic liquid crystal 5CB. Better accuracy of VOC prediction is obtained for the hybrid gels composed of a PDMS matrix combined with the [BMIM][Cl] ionic liquid, and the use of this hydrophobic matrix reduces the effect of humidity on the sensing performance when compared to the gelatin counterpart. VOCs interact with all the moieties of the hybrid gel multicomponent system; thus, VOC correct classification depends not only on the polymeric matrix used, but also on the IL selected, which seems to be key to achieve VOCs discrimination at 50% RH. Thus, hybrid gels' tunable formulation offers the potential for designing complementary sensors for e-nose systems operable under different RH conditions.

Efficient Ligand Passivation Enables Ultrastable CsPbX3 Perovskite Nanocrystals in Fully Alcohol Environments

AbstractHalide perovskite nanocrystals (PNCs) have demonstrated their wide potential to fabricate efficient optoelectronic devices and to prepare promising photocatalysts for solar‐driven photo(electro)chemical reactions. However, their use in most of the practical applications is limited due to the instability of PNCs in polar environments. Here, the preparation of non‐encapsulated CsPbX3 nanocrystals dispersed in fully alcohol environments, with outstanding stability through surface defect passivation strategy is reported. By using didodecyldimethylammonium bromide (DDAB) during material post‐treatment, highly luminescent CsPbBr3 PNCs with remarkable stability in methanol/butanol medium up to 7 months with near‐unity photoluminescence quantum yield are achieved. This approach is extrapolated to stabilize iodine‐based CsPbBr3‐xIx and CsPbI3 PNCs, showing an improvement of their photoluminescence features and stability in these high polar alcohols up to 6 h. DDAB mediates the defect suppression through ligand exchange and avoids the full permeation of alcohol to be in contact with the PNCs. In this context, DDAB induces ionization of alcohol molecules to strengthen the surface passivation. The findings open the door to the development of long‐term stable CsPbX3 PNCs with high optical performance to be used in polar environments.

About the Formation of NH2OH+ from Gas Phase Reactions under Astrochemical Conditions

We present here an analysis of several possible reactive pathways toward the formation of hydroxylamine under astrochemical conditions. The analysis is based on ab initio quantum chemistry calculations. Twenty-one bimolecular ion-molecule reactions have been studied and their thermodynamics presented. Only one of these reactions is a viable direct route to hydroxylamine. We conclude that the contribution of gas-phase chemistry to hydroxylamine formation is probably negligible when compared to its formation via surface grain chemistry. However, we have found several plausible gas-phase reactions whose outcome is the hydroxylamine cation.

Epoxidation of Methyl Esters as Valuable Biomolecules: Monitoring of Reaction

The paper is focused on the epoxidation of methyl esters prepared from oil crops with various profiles of higher fatty acids, especially unsaturated, which are mainly contained in the non-edible linseed and Camelina sativa oil (second generation). The novelty consists in the separation and identification of all products with oxirane ring formed through a reaction and in the determination of time course. Through the epoxidation, many intermediates and final products were formed, i.e., epoxides with different number and/or different position of oxirane rings in carbon chain. For the determination, three main methods (infrared spectroscopy, high-pressure liquid chromatography and gas chromatography with mass spectrometry) were applied. Only gas chromatography enables the separation of individual epoxides, which were identified on the base of the mass spectra, molecule ion and time course of products. The determination of intermediates enables: (i) control of the epoxidation process, (ii) determination of the mixture of epoxides in detail and so the calculation of selectivity of each product. Therefore, the epoxidation will be more environmentally friendly especially for advanced applications of non-edible oil crops containing high amounts of unsaturated fatty acids.

Differentiating Toxic and Nontoxic Tricresyl Phosphate Isomers Using Ion–Molecule Reactions with Oxygen

Ortho-substituted isomers of tricresyl phosphates (TCPs) and their toxic metabolites (e.g., CBDP: cresyl saligenin phosphate) can cause neurotoxic effects in humans. When TCP is introduced to an atmospheric pressure chemical ionization source using gas chromatography, radical cations M•+ are formed by charge exchange. The mass spectrum of an ortho-substituted isomer displays two intense peaks that are absent in the spectra of non-ortho-substituted isomers, leading us to propose structure-diagnostic ion-molecule reactions between ions M•+ and oxygen species present in the source. However, the mechanisms of these reactions have not yet been established. In this study, we propose a mechanism and provide support through computational and experimental analyses using density functional theory and cyclic ion mobility-mass spectrometry. The mechanism consists of a multistep reaction starting with the rearrangement of the molecular ion into a distonic isomer followed by an oxidation step and then decomposition into [CBDP-H]+. This proposal is consistent with the results obtained from a series of isotopically labeled analogues. Cyclic ion mobility experiments with a tri-o-cresyl phosphate standard reveal the presence of at least two hydrogen shift isomers of the product ion [CBDP-H]+ that are connected by a low-lying barrier. The selectivity of the ion-molecule reactions toward ortho-substituted cresyl TCP isomers provides us with an identification tool that can select potentially neurotoxic triaryl phosphate esters present in complex mixtures that are produced in large volume by industry.

Ptychographic measurements of varying size and shape along zeolite channels.

Sub-angstrom resolution imaging of porous materials like zeolites is important to reveal their structure-property relationships involved in ion exchange, molecule adsorption and separation, and catalysis. Using multislice electron ptychography, we successfully measured the atomic structure of zeolite at sub-angstrom lateral resolution for 100-nanometer-thick samples. Both lateral and depth deformations of the straight channels are mapped, showing the three-dimensional structural inhomogeneity and flexibility. Since most zeolites in industrial applications are usually tens to hundreds of nanometers thick, the sub-angstrom resolution imaging and accurate measurements of depth-dependent local structures with electron ptychography at low-dose condition will find wide applications in porous materials close to their industrially relevant conditions.

New type of hydrogenlike charm-pion or charm-kaon matter

Borrowing the structures of the hydrogen atom, molecular ion, and diatomic molecule, we predict the nature of a new type of hydrogenlike charm-pion or charm-kaon matter that could be obtained by replacing the proton and electron in hydrogen matter with a charmed meson and a pion or a kaon, respectively. We find that the spectra of the atom, molecular ion, and diatomic molecule can be obtained simultaneously with the Coulomb potential for the hydrogen, the charm-pion, and the charm-kaon systems. The predicted charm-pion matter also allows us to explore the mass shift mediated by the strong interaction. For the charm-pion and charm-kaon systems, the strong interactions could lead to binding energy shifts. Our calculations suggests that the binding energy shifts in charm-pion systems are in the order of several to tens of eV. For the charm-kaon systems, the results are in the order of tens to hundreds of eV. Exploring hydrogenlike charm-pion matter must lead to new demands for high-precision experiments.

The occurrence of pristine and functionalized fullerenes as constituents of airborne aerosols

We investigated if pristine and functionalized fullerenes could be actual constituents of fine atmospheric aerosols. Comprehensive profiles of fullerenes from 1 µL extracts were made through matrix laser desorption ionization Time-of-Flight Mass Spectrometry (MALDI-MS) within a few minutes. The ion with m/z 720, corresponding to [C60]−•, was identified as fullerene after 1 µL of α-cyano-4-hydroxycinnamic acid matrix solution was spotted over the dried extracts. The ions with the m/z corresponding to C70, C76, C84, C100, C118, C128, and C130 were also attributed to other fullerene species detected within the samples. The ion m/z 878 was found to be the fullerene derivative diethyl methano[60]fullerene dicarboxylate. Since ions of fragmented fullerene molecules were not detected even at high laser energies, we considered the fullerenes’ occurring as original constituents of real atmospheric particle matrices instead of being formed as artifacts of the laser action on samples. Therefore, this protocol would be helpful in the understanding of the distribution of either pristine or functionalized fullerenes in the environment and their participation in atmospheric chemistry under typical conditions, as well as its application in vitro and in vivo (eco)toxicity studies.

Time-dependent multiconfiguration self-consistent-field and time-dependent optimized coupled-cluster methods for intense laser-driven multielectron dynamics

We reviewed the time-dependent multiconfiguration self-consistent-field (TD-MCSCF) method and the time-dependent optimized coupled-cluster (TD-OCC) method for first-principles simulations of high-field phenomena such as tunneling ionization and high-order harmonic generation in atoms and molecules irradiated by a strong laser field. These methods provide a flexible and systematically improvable description of the multielectron dynamics by expressing the all-electron wavefunction by configuration interaction expansion or coupled-cluster expansion, using time-dependent one-electron orbital functions. The time-dependent variational principle plays a key role in deriving these methods while satisfying gauge invariance and Ehrenfest theorem. The real-time/real-space implementation with an absorbing boundary condition enables the simulation of high-field processes involving multiple excitation and ionization. We present a detailed, comprehensive discussion of such features of the TD-MCSCF and TD-OCC methods.

Electron impact ionization of atoms and molecules: an improved BBK model

We present a new model to study the dynamics of electron impact ionization of atoms and molecules. In this model, the two outgoing electrons are both described by a Coulomb wave with variable charges Z(r) while the incident electron is described by a plane wave. The fully differential cross-section is then calculated in (e,2e) reactions for several atomic and molecular targets taking into account the post-collision interaction. Calculations are carried out for the coplanar asymmetric kinematics, and the results are compared with those from available experiments.

X-ray Diffraction Topography (Imaging) of Crystals Grown from Solution: A Short Review

A short review of X-ray topographic studies of crystals grown from solution is presented. The dislocation configurations characteristic of such crystals are described, and Klapper’s explanation in terms of minimization of the elastic energy of a dislocation per unit growth length is highlighted. It is shown that the principles apply to crystals grown not only from low temperature solution but also by hydrothermal growth and growth from fluxed melts. Recent studies of growth of protein crystals have found that they have similar dislocation configurations and characteristics to those of ionic and small organic molecule crystals grown from solution.

Selective accumulation of pharmaceutical residues from 6 different soils by plants: a comparative study on onion, radish, and spinach

The accumulation of six pharmaceuticals of different therapeutic uses has been thoroughly investigated and compared between onion, spinach, and radish plants grown in six soil types. While neutral molecules (e.g., carbamazepine (CAR) and some of its metabolites) were efficiently accumulated and easily translocated to the plant leaves (onion > radish > spinach), the same for ionic (both anionic and cationic) molecules seems to be minor to moderate. The maximum accumulation of CAR crosses 38,000 (onion), 42,000 (radish), and 7000 (spinach) ng g−1 (dry weight) respectively, in which the most majority of them happened within the plant leaves. Among the metabolites, the accumulation of carbamazepine 10,11-epoxide (EPC — a primary CAR metabolite) was approximately 19,000 (onion), 7000 (radish), and 6000 (spinach) ng g−1 (dry weight) respectively. This trend was considerably similar even when all these pharmaceuticals applied together. The accumulation of most other molecules (e.g., citalopram, clindamycin, clindamycin sulfoxide, fexofenadine, irbesartan, and sulfamethoxazole) was restricted to plant roots, except for certain cases (e.g., clindamycin and clindamycin sulfoxide in onion leaves). Our results clearly demonstrated the potential role of this accumulation process on the entrance of pharmaceuticals/metabolites into the food chain, which eventually becomes a threat to associated living biota.

Optimal Alkalinity Model of Ladle Furnace Slag for Bearing Steel Production Based on Ion–Molecule Coexistence Theory

The fatigue life of bearing steel is closely related to the total oxygen content (T(O)) of the liquid steel. In order to stably and effectively control the T(O) during the ladle furnace (LF) refining process, we established a calculation model of optimal alkalinity for the refining slag CaO–SiO2–Al2O3–MgO–FeO–CaF2 at 1853 K based on ion–molecule coexistence theory (IMCT). Here, the influencing factors are discussed. The results show that the maximum value of NFeO occurred when the optimal alkalinity was around five at varied FeO contents, and that the optimal alkalinity basically remained the same with changes in FeO content. With the increase of MgO content, the optimal alkalinity decreased. However, the change in the value of NFeO against the higher alkalinity was not obvious at a given MgO content. The effect of Al2O3 content on the optimal alkalinity was opposite to that of MgO. With the increasing Al2O3 content, the optimal alkalinity obviously increased, while the maximum value of NFeO occurred when the Al2O3 content varied from 35 wt% to 45 wt% at higher alkalinity. The higher w(CaO)/w(Al2O3) mass ratio had a distinct effect on the value of NFeO against alkalinity, while the effect of alkalinity on the value of NFeO was not obvious at a fixed CaF2 level. This optimal alkalinity model based on IMCT can provide a certain guiding role in the process of refining slag composition optimization and is conducive to effectively controlling total oxygen content in the refining process.

Theoretical Calculations of the Thermal Rate Coefficients for the Interstellar NH3+ + H2 → NH4+ + H Reaction on a New Δ-Machine Learning Potential Energy Surface

The NH3+ + H2 → NH4+ + H ion–molecule hydrogen-exchange reaction is important for understanding the mechanisms of ammonia formation in interstellar medium and circumstellar environments. The thermal rate coefficients of this reaction are calculated using the ring polymer molecular dynamics approach, which can account for the nuclear quantum effects, on a newly developed ab initio potential energy surface (PES). The PES was constructed by fitting a large number of ab initio points at the MP2/cc-pVDZ and CCSD(T)/cc-pVTZ levels using a Δ-machine learning approach. The obtained rate coefficients exhibited a minimum at T ∼ 130 K, and this characteristic temperature-dependent behavior qualitatively agreed with the experimental measurements. This study confirms that quantum tunneling plays a significant role in the reaction dynamics along with the existence of the metastable NH3+···H2 pre-reactive complex in the entrance channel of the PES.

Electron dynamics of molecular frustrated double ionization driven by strong laser fields* *Supported by the National Natural Science Foundation of China (Grant Nos. 12004323, 12074329, 12104389, 1174131 and 91850114), National Key R&D Program of China (2022YFE0134200) and Nanhu Scholars Program for Young Scholars of Xinyang Normal University, Natural Science Foundation of Jilin Province, China (Grant No. 20220101016JC), and the Open

We theoretically investigate the frustrated double ionization (FDI) of molecules with different alignment-dependence using a three-dimensional classical ensemble method. The numerical results show that the FDI probability decreases with increasing wavelength, which is similar to the wavelength dependence of the FDI probability of atoms. Tracing the classical trajectories reveals that the contributions to molecular FDI from single-recollision and multiple-recollision mechanisms are equal in the short wavelength regime. In the long wavelength regime, the single-recollision FDI channel dominates in FDI. The nature in which molecular FDI occurs is identified and explained.

Tribological mechanism of carbon group nanofluids on grinding interface under minimum quantity lubrication based on molecular dynamic simulation

Carbon group nanofluids can further improve the friction-reducing and anti-wear properties of minimum quantity lubrication (MQL). However, the formation mechanism of lubrication films generated by carbon group nanofluids on MQL grinding interfaces is not fully revealed due to lack of sufficient evidence. Here, molecular dynamic simulations for the abrasive grain/workpiece interface were conducted under nanofluid MQL, MQL, and dry grinding conditions. Three kinds of carbon group nanoparticles, i.e., nanodiamond (ND), carbon nanotube (CNT), and graphene nanosheet (GN), were taken as representative specimens. The [BMIM]BF4 ionic liquid was used as base fluid. The materials used as workpiece and abrasive grain were the single-crystal Ni-Fe-Cr series of Ni-based alloy and single-crystal cubic boron nitride (CBN), respectively. Tangential grinding force was used to evaluate the lubrication performance under the grinding conditions. The abrasive grain/workpiece contact states under the different grinding conditions were compared to reveal the formation mechanism of the lubrication film. Investigations showed the formation of a boundary lubrication film on the abrasive grain/workpiece interface under the MQL condition, with the ionic liquid molecules absorbing in the groove-like fractures on the grain wear’s flat face. The boundary lubrication film underwent a friction-reducing effect by reducing the abrasive grain/workpiece contact area. Under the nanofluid MQL condition, the carbon group nanoparticles further enhanced the tribological performance of the MQL technique that had benefited from their corresponding tribological behaviors on the abrasive grain/workpiece interface. The behaviors involved the rolling effect of ND, the rolling and sliding effects of CNT, and the interlayer shear effect of GN. Compared with the findings under the MQL condition, the tangential grinding forces could be further reduced by 8.5%, 12.0%, and 14.1% under the diamond, CNT, and graphene nanofluid MQL conditions, respectively.

Textural landscapes of VOC-sensitive chiral liquid crystal-based materials

Liquid crystal-based materials, in which liquid crystal molecules are confined and ordered in compartments, are dynamic materials yielding a variety of optical textures that can be tuned as a response to physical and chemical stimuli. While nematic and smectic-based gel materials have been reported as dynamic optical sensors to report volatile organic compounds (VOCs), chiral systems are less explored despite having the potential to yield extremely rich optical landscapes. Here, we report for the first time the confinement of chiral liquid crystal formulations by an interface formed by ionic liquid molecules. The resultant self-assembled ionic liquid/liquid crystal droplets are simultaneously immobilized on a gelatin matrix. The droplets feature a rich variety of unique topological states. We explored, by means of polarizing optical microscopy, the various droplet optical textures and categorized them with regard to their relative chirality parameter. We further investigated their optical response in the presence of gas analytes and discussed their potential utilization as dynamic liquid crystal-based optical VOC sensors. The newly generated soft materials with semi-selective VOC sensing capabilities can be further utilized in arrays of liquid crystal-based gas sensors for the analysis of complex gas samples using artificial olfaction approaches.

The 8‐Hydroxyquinolinium Cation as a Lead Structure for Efficient Color‐Tunable Ionic Small Molecule Emitting Materials

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