Ion probe analysis of artificially implanted ions in terrestrial samples and surface enhanced ions in lunar sample 76215,77
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Zinner, E.↗
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High-resolution ion mobility based on traveling wave structures for lossless ion manipulation resolves hidden lipid features
Abstract High-resolution ion mobility (resolving power > 200) coupled with mass spectrometry (MS) is a powerful analytical tool for resolving isobars and isomers in complex samples. High-resolution ion mobility is capable of discerning additional structurally distinct features, which are not observed with conventional resolving power ion mobility (IM, resolving power ~ 50) techniques such as traveling wave IM and drift tube ion mobility (DTIM). DTIM in particular is considered to be the “gold standard” IM technique since collision cross section (CCS) values are directly obtained through a first-principles relationship, whereas traveling wave IM techniques require an additional calibration strategy to determine accurate CCS values. In this study, we aim to evaluate the separation capabilities of a traveling wave ion mobility structures for lossless ion manipulation platform integrated with mass spectrometry analysis (SLIM IM-MS) for both lipid isomer standards and complex lipid samples. A cross-platform investigation of seven subclass-specific lipid extracts examined by both DTIM-MS and SLIM IM-MS showed additional features were observed for all lipid extracts when examined under high resolving power IM conditions, with the number of CCS-aligned features that resolve into additional peaks from DTIM-MS to SLIM IM-MS analysis varying between 5 and 50%, depending on the specific lipid sub-class investigated. Lipid CCS values are obtained from SLIM IM ( TW(SLIM) CCS) through a two-step calibration procedure to align these measurements to within 2% average bias to reference values obtained via DTIM ( DT CCS). A total of 225 lipid features from seven lipid extracts are subsequently identified in the high resolving power IM analysis by a combination of accurate mass-to-charge, CCS, retention time, and linear mobility-mass correlations to curate a high-resolution IM lipid structural atlas. These results emphasize the high isomeric complexity present in lipidomic samples and underscore the need for multiple analytical stages of separation operated at high resolution. Graphical abstract
Reardon, Allison R. (ORCID:0000000165830134)↗
Structural mapping and tuning of mixed halide ions in amorphous sulfides for fast Li-ion conduction and high deformability
Amorphous sulfides are among the most promising candidates for solid electrolytes (SEs) owing to their excellent deformability and acceptable Li-ion conductivity (σion) at room temperature. However, the complex atomic structure of these amorphous materials without long-range ordering results in a lack of structural understanding and difficulties in tuning material properties. Here, in this study, we performed structural mapping of glassy sulfide SEs composed of various anion clusters using a combinatorial atomic level analysis of synchrotron X-ray-based pair distribution function (PDF) and reverse Monte-Carlo (RMC) methods, demonstrating the potential to tune σ ion in glass SEs. First, we prepared a new glassy sulfide with a mixed anion framework of two halogens (Br and I) as atomic anions, with PS 4 3- molecular anions in a Li 2 S–P 2 S 5 -based glass SE. At a specific Br content, [(Li 2 S) 0.658 (LiI 0.9 LiBr 0.1 ) 0.342 ] 0.825 [P 2 S 5 ] 0.175 recorded a σ ion of 2.27 mS cm -1 , the highest value for any glass sulfides reported to date; however, its elastic modulus was still suppressed to 14.48 GPa. PDF and RMC calculations successfully provided structural mapping of anion clusters, including two halogens. Molecular dynamics simulations of each composition confirmed that flexible coordination caused by the rattling of small polarizable Br ions in the mixed halogens of glassy SEs contributed to the superior σ ion . Our results may provide new insights into the design of superior glassy SEs that play key roles in all-solid-state batteries requiring fast Li-ion conduction and high deformability.
36 MATERIALS SCIENCE↗
Topotactic Phase Transformation of Lithiated Spinel to Layered LiMn0.5Ni0.5O2: The Interaction of 3-D and 2-D Li-ion Diffusion
This study investigates the structural evolution of LiMn0.5Ni0.5O2 cathode materials for Li-ion batteries as a function of synthesis temperature and its effect on electrochemical performance. It is demonstrated that, as the synthesis temperature increases from 400 to 900 ?C, a gradual topotactic transformation occurs between a lithiated spinel structure, denoted herein as “lithium-excess spinel” LxS-LiMn0.5Ni0.5O2 (or LxS-LMNO), and the well-known layered LiMn0.5Ni0.5O2 structure prepared at high temperature, HT-LiMn0.5Ni0.5O2 (HT-LMNO). The electrochemical capacity of the LiMn0.5Ni0.5O2 electrodes follows a parabolic trend with increasing synthesis temperature, which is attributed primarily to the gradual transformation of 3-dimensional (3-D) to 2-dimensional (2-D) diffusion pathways for the Li ions. When synthesized at 400 °C, LxS-LiMn0.5Ni0.5O2 electrodes perform well, benefitting from the 3-D network of channels within the LxS structure. By contrast, when prepared at 500-700 °C, LiMn0.5Ni0.5O2 electrodes operate poorly, which is attributed to the formation of locally disordered structural arrangements that impede Li-ion diffusion. Such an increase in local disorder in the mid-temperature synthesis range is attributed to the structural frustration between the lithium-excess spinal and layered end-members. The transformation from the locally disordered to more ordered layered components between 700 °C and 900 °C enhances electrochemical performance. The study opens new avenues for designing next-generation Mn-rich cathode materials by fine-tuning the synthesis conditions as well as the composition and structure of LxS-LMNO electrodes.
energy storage↗
The impact of the electric field of metal ions on the vibrations and internal hydrogen bond strength in alkali metal ion di- and triglycine complexes
Using infrared predissociation spectroscopy of cryogenic ions, we revisit the vibrational spectra of alkali metal ion (Li+, Na+, K+) di- and triglycine complexes. We assign their most stable conformation, which involves metal ion coordination to all C=O groups and an internal NH⋯NH2 hydrogen bond in the peptide backbone. An analysis of the spectral shifts of the OH and C=O stretching vibrations across the different metal ions and peptide chain lengths shows that these are largely caused by the electric field of the metal ion, which varies in strength as a function of the square of the distance. The metal ion–peptide interaction also remotely modulates the strength of internal hydrogen bonding in the peptide backbone via the weakening of the amide C=O bond, resulting in a decrease in internal hydrogen bond strength from Li+ > Na+ > K+.
Chemistry↗
Exploring the impact of ions on oxygen K-edge X-ray absorption spectroscopy in NaCl solution using the GW-Bethe-Salpeter-equation approach
X-ray absorption spectroscopy (XAS) is a powerful experimental tool to probe the local structure in materials with the core hole excitations. Here, the oxygen K-edge XAS spectra of the NaCl solution and pure water are computed by using a recently developed GW-Bethe-Salpeter equation approach, based on configurations modeled by path-integral molecular dynamics with the deep-learning technique. The neural network is trained on ab initio data obtained with strongly constrained and appropriately normed density functional theory. The observed changes in the XAS features of the NaCl solution, compared to those of pure water, are in good agreement between experimental and theoretical results. We provided detailed explanations for these spectral changes that occur when NaCl is solvated in pure water. Specifically, the presence of solvating ion pairs leads to localization of electron-hole excitons. As a result, our theoretical XAS results support the theory that the effects of the solvating ions on the H-bond network are mainly confined within the first hydration shell of ions, however beyond the shell the arrangement of water molecules remains to be comparable to that observed in pure water.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Extraction of ion beam from laser ion source for direct plasma injection scheme
Laser ion sources are expected to be used in various applications of heavy ion beam technology. The plasma direct injection scheme (DPIS) is a method in which ion beams extracted from a laser ion source are directly injected into a radio frequency quadrupole (RFQ) linear accelerator. In this study, a new shape of the plasma electrode with a concave surface for the DPIS was proposed to inject a converging beam to a cavity of RFQ accelerator. This approach allows the use of a large-diameter extraction electrode, which is not limited by the aperture of the RFQ electrode rods. The DPIS, using the concave surface electrode, was employed to accelerate C 6+ ion beams. The results indicated that both the beam current and the number of ions increased nearly twice with the proposed electrode shape compared to values obtained with the conventional electrode. This enhancement corresponded to the increased extraction area of the beam.
43 PARTICLE ACCELERATORS↗
Experimental Measurements of Ion Diffusion Coefficients and Heating in a Multi-Ion-Species Plasma Shock
Collisional plasma shocks generated from supersonic flows are an important feature in many astrophysical and laboratory high-energy-density plasmas. Compared to single-ion-species plasma shocks, plasma shock fronts with multiple ion species contain additional structure, including interspecies ion separation driven by gradients in species concentration, temperature, pressure, and electric potential. We present time-resolved density and temperature measurements of two ion species in collisional plasma shocks produced by head-on merging of supersonic plasma jets, allowing determination of the ion diffusion coefficients. Here our results provide the first experimental validation of the fundamental inter-ion-species transport theory. The temperature separation, a higher-order effect reported here, is valuable for advancements in modeling HED and ICF experiments.
70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
Dual-band Ion-scale Waves in the Solar Wind: Statistical Properties and Comparison with Single-band Ion-scale Waves
We present a comprehensive statistical analysis of ion-scale waves including dual-band ion-scale waves (DBIWs) observed by the Parker Solar Probe in the solar wind. DBIWs are characterized by the simultaneous occurrence of distinct left- and right-handed polarized wave packets at higher and lower frequencies, respectively, in the spacecraft frame, implying the presence of bidirectionally propagating L-mode waves. We identify and compare DBIWs to single-band ion-scale waves (SBIWs) and investigate their spatial distributions, background magnetic field conditions, and associated inertial range turbulence characteristics. We find that DBIWs exhibit a strong preferential occurrence at heliocentric distances between 0.2 and 0.25 au (equivalently 43 and 54 R S ) in contrast to SBIWs, the occurrence rate of which peaks closer to the Sun and decreases with the heliocentric distance. DBIWs are also preferentially observed under conditions of strong Alfvénic turbulence, characterized by low magnetic compressibility and perpendicular-dominant fluctuations. These findings support a scenario in which stochastic ion heating via sufficiently large perpendicular Alfvénic fluctuation generates the ion temperature anisotropies required to excite bidirectional ion cyclotron waves. This work advances our understanding of kinetic wave generation in the solar wind and its connection to large-scale turbulence.
79 ASTRONOMY AND ASTROPHYSICS↗
Ion acoustic waves in a multi-ion plasma.
An exact treatment of the multispecies ion acoustic dispersion relation is given for an argon/helium plasma. Phase velocity and damping are obtained as a function of ion-electron temperature ratio and relative densities of the two species. There are two important modes in the plasma, with quite different phase velocities, which are referred to as principal heavy ion mode and principal light ion mode. Which of these is dominant depends on the relative densities of the two components, but, in general, the light ion mode becomes important for surprisingly small light ion contamination. Approximate analytic expressions are derived from damping rates and phase velocities and their domains of validity are investigated. Relevance of the results for the investigation of collisionless shocks is discussed.
Fried, B. D.↗
Electrostatic Propulsion Beam Divergence Effects on Spacecraft Surfaces. Volume 2, Addendum 1: Ion Time-of-flight Determinations of Doubly to Singly Ionized Mercury Ion Ratios from a Mercury Electron Bombardment Discharge
The analysis of ion exhaust beam current flow for multiply charged ion species and the application to propellant utilization for the thruster are discussed. The ion engine in use in the experiments is a twenty centimeter diameter electromagnet electron bombardment engine. The experimental technique to determine the multiply charged ion abundance ratios using ion time of flight is described. An analytical treatment of the discharge action in producing various ion species has been carried out.
Sellen, J. M., Jr.↗
Charge exchange of metastable 2D oxygen ions with molecular oxygen - A new source of thermospheric O2/+/ ions
Reactions involving metastable ions are difficult to study in the laboratory. Much new information on these reactions has been derived from satellite measurements of aeronomic parameters. In this paper, Atmosphere Explorer D data are used to study charge exchange of metastable O(+)(2D) ions with O2. Using direct measurements of the O2 at 200 km to compute O2 densities at 300 km and supporting ionic concentrations and temperature observations, we find the rate coefficient for this reaction to be 1 + or - 0.6 times 10 to the minus 9th cu cm/sec. The process constitutes a significant source of O2(+) ions in the F2 layer at times when the N2 and O2 densities are enhanced. This finding leads to the conclusion that charge exchange with O2 must be a major sink for O(+)(2D) and an important source of O2(+) ions in the E region, because of the increase in the O2 concentration/N2 concentration ratio with decreasing altitude. The results imply that 80% of all O(+) ions formed in the E region are converted to O2(+) and that only about 20% of the metastable O(+) ions are converted into N2(+) through charge exchange with N2.
Torr, D. G.↗
Transversely accelerated ions - An ionospheric source of hot magnetospheric ions
The paper considers observational data on transversely accelerated ion (TAI) events observed from the Isis 1 and 2 satellites. A source of hot magnetospheric ions was discovered in the auroral topside ionosphere, and a part of the cold ionospheric ion distribution is transversely accelerated within a source region as low as 1000 km. Subsequent to transverse acceleration, the ions are driven upward into the magnetosphere by the gradient B mirror force; they are observed by the soft particle spectrometers on the Isis 1 and 2 satellites, with sharply defined pitch angle distributions centered between 90 and 120 deg, and with energy distributions up to several hundred electron volts. Observations at 1400 km indicate that the transversely accelerated ion (TAI) events are predominantly a winter nightside auroral zone phenomenon, but in the summertime TAI events were observed at altitudes above 2750 km on the day-side within the cleft. Typical intensities exceeding 10 to the 8th power ions/sq cm s sr during TAI events suggest that they may be a significant source of hot ions for the magnetosphere.
Klumpar, D. M.↗
Diffuse ions produced by electromagnetic ion beam instabilities
The evolution of the electromagnetic ion beam instability driven by the reflected ion component backstreaming away from the earth's bow shock into the foreshock region is studied by means of computer simulation. The linear and quasi-linear stages of the instability are found to be in good agreement with known results for the resonant mode propagating parallel to the beam along the magnetic field and with theory developed in this paper for the nonresonant mode, which propagates antiparallel to the beam direction. The quasi-linear stage, which produces large amplitude delta B approximately B, sinusoidal transverse waves and 'intermediate' ion distributions, is terminated by a nonlinear phase in which strongly nonlinear, compressive waves and 'diffuse' ion distributions are produced. Additional processes by which the diffuse ions are accelerated to observed high energies are not addressed. The results are discussed in terms of the ion distributions and hydromagnetic waves observed in the foreshock of the earth's bow shock and of interplanetary shocks.
Winske, D.↗
Energization of ions in the auroral plasma by broadband waves - Generation of ion conics
Nonresonant heating of plasma ions flowing along geomagnetic field lines by VLF waves is shown to generate ion conics. Ions with energies of less than 1 eV are proven capable of resonance with ionospheric VLF waves excited by electron beams with energies over 100 eV at lower hybrid frequencies (LHF) of 1-1.01. The variation of resonant ion energy with LHF wave frequency is formulated and an expression is derived for the heating rate. The heating rate is then applied to model ion acceleration along a dipole geomagnetic field in terms of the power spectral density of broadband waves, i.e., the VLF noise. Attention is given to ion energization at lower altitudes than the auroral acceleration region and examples of conic acceleration are cited.
Singh, N.↗
Transport of ions in presence of induced electric field and electrostatic turbulence - Source of ions injected into ring current
The transport of ions from the polar ionosphere to the inner magnetosphere during stormtime conditions has been computed using a Monte Carlo diffusion code. The effect of the electrostatic turbulence assumed to be present during the substorm expansion phase was simulated by a process that accelerated the ions stochastically perpendicular to the magnetic field with a diffusion coefficient proportional to the energization rate of the ions by the induced electric field. This diffusion process was continued as the ions were convected from the plasma sheet boundary layer to the double-spiral injection boundary. Inward of the injection boundary, the ions were convected adiabatically. By using as input an O(+) flux of 2.8 x 10 to the 8th per sq cm per s (w greater than 10 eV) and an H(+) flux of 5.5 x 10 to the 8th per sq cm per s (w greater than 0.63 eV), the computed distribution functions of the ions in the ring current were found to be in good agreement, over a wide range in L (4 to 8), with measurements made with the ISEE-1 satellite during a storm. This O(+) flux and a large part of the H(+) flux are consistent with the DE satellite measurements of the polar ionospheric outflow during disturbed times.
Cladis, J. B.↗
Transverse acceleration of oxygen ions by electromagnetic ion cyclotron resonance with broad band left-hand polarized waves
Central plasma sheet (CPS) ion conics are oxygen-dominated, with peak energies ranging from tens to hundreds of eV centered around pitch-angles between 115 and 130 degrees. Because of the lack of correlation between the CPS conics and the observed currents and/or electron beam-like structures, it is not likely that all of these conics are generated by interactions with electrostatic ion cyclotron waves or lower hybrid waves. Instead, it is suggested that the observed intense broad band electric field fluctuations in the frequency range between 0 and 100 Hz can be responsible for the transverse energization of the ions through cyclotron resonance heating with the left-hand polarized electromagnetic waves. This process is much more efficient for heating the oxygen ions than hydrogen ions, thus providing a plausible explanation of the oxygen dominance in CPS conics. Simple algebraic expressions are given from which estimates of conic energy and pitch angle can be easily calculated. This suggested mechanism can also provide some preheating of the oxygen ions in the boundary plasma sheet (BPS) where discrete aurorae form.
Chang, T.↗
Hot ions observed by the Giotto ion mass spectrometer inside the Comet Halley contact surface
Just inside the contact surface (approx. 4700 km) the High Energy Range Spectrometer (HERS) sensor of the Giotto ion mass spectrometer detected a sudden, intense burst of ions that lasted until the HERS sensor ceased transmitting data at a distance 3000 km from comet Halley. During this interval ions with M/Q=1, 2, 12, 14, 16, 19, 24 and 28 were observed. The heavier ions appear in two populations (in the S/C frame): a very low energy, almost omnidirectional distribution, and a more energetic (approx. < ram speed) population coming from the ram direction. The low energy ions may belong to the natural Halley environment or be generated at the spacecraft by dust and gas bombardment. The ions may also be related to spacecraft charging processes on Giotto.
Goldstein, R.↗