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At least 289 records · Page 16Linked to original sources
PubMed2000

Improved ion transmission from atmospheric pressure to high vacuum using a multicapillary inlet and electrodynamic ion funnel interface

A heated multicapillary inlet and ion funnel interface was developed to couple an electrospray ionization (ESI) source to a high-vacuum stage for obtaining improved sensitivity in mass spectrometric applications. The inlet was constructed from an array of seven thin-wall stainless steel tubes soldered into a central hole of a cylindrical heating block. An electrodynamic ion funnel was used in the interface region to more effectively capture, focus, and transmit ions from the multicapillary inlet. The interface of seven capillary inlets with the ion funnel showed more than 7 times higher transmission efficiency compared to that of a single capillary inlet with the ion funnel and a 23-fold greater transmission efficiency than could be obtained using the standard orifice-skimmer interface of a triple-quadrupole MS. The multiple-capillary inlet and ion funnel interface showed an overall 10% ion transmission efficiency and approximately 3-4% overall detection efficiency of ions from solution based (i.e., prior to electrospray). The improved performance was achieved under conditions where ESI operation is robust and results in a significant increase in dynamic range.

Journal Article↗
PubMed1993

Enhanced mass resolving power, sensitivity, and selectivity in laser desorption Fourier transform ion cyclotron resonance mass spectrometry by ion axialization and cooling.

Ion cooling and axialization produced by azimuthal quadrupolar excitation in the presence of ion-neutral collisions are applied to laser desorption Fourier transform ion cyclotron resonance mass spectrometry (LD/FT/ICR-MS). With this technique, the large kinetic and internal energies of ions generated by laser desorption processes can be cooled effectively by collisions of ions with neutral argon atoms (at > 5 x 10(-7) Torr). After sufficient cooling in the source compartment of a dual ion trap, the axialized ions may be transferred to the analyzer compartment for detection at much lower pressure (and thus much higher mass resolving power). Enhancements in both FT/ICR mass resolving power and sensitivity are observed; moreover, ion isolation with high selectivity at high pressure is also demonstrated.

Argon↗
PubMed1996

Three-dimensional motional stabilization in the trapping field of an open-ended trapped-ion cell: application to the remeasurement experiment in Fourier transform ion cyclotron resonance mass spectrometry.

Three-dimensional motional stabilization of radial trajectories of low-mass organic ions in an open cell using only a dc trapping field is applied to the FT-ICR remeasurement experiment. More than 300 remeasurement cycles are observed with 99.59% remeasurement efficiency for benzene (m/z 78) using a high-pressure helium buffer gas. The enhancement in remeasurement efficiency is due to collisional stabilization of the guiding center of ion motion by dynamic motional averaging in the axial position-dependent radial electric field. Such dc-induced radial stabilization is in contrast to the stability produced by application of radio frequency fields characteristic of quadrupolar axialization or rf-only mode operation. The same effect is produced because ions experience a radial "pseudopotential" during axial oscillation as in time-varying fields. Trajectory simulations for ions oscillating in an open cell trapping well above a z-amplitude critical threshold energy of 0.60 eV (in a potential well of 0.84 V) indicate that radially stabilized trapping motion is achieved because the outward-directed radial electric field existing near the cell center line is compensated by an opposing inward-directed radial electric field at extended z-amplitude. Sufficient axial kinetic energy permits ion penetration into the inward-directed radial electric field regions, enabling > 50% residence time of each trapping oscillation period in regions inducing radial stability, thereby inhibiting magnetron radius growth. A high-pressure, low-mass buffer gas such as helium provides the requisite increase in the axial amplitude of the ion cloud, similar to the mechanism observed for axial excitation of low-mass ions observed in collision-induced dissociation. The result is radial stability at high pressure, even after multiple remeasurement cycles. An optimized excitation radius of 12.5% of the cell radius yields maximum remeasurement efficiency with a 500 ms relaxation delay between excitation events. Summed signal intensity decreases with increased trap potential due to the greater radial electric field and reduced axial expansion of the ion cloud and also decreases with buffer gas mass in response to greater radial scattering.

Fourier Analysis↗
PubMed1996

Matrix-assisted laser desorption ion trap mass spectrometry: efficient isolation and effective fragmentation of peptide ions.

Effective analysis of the sequence of peptides using matrix-assisted laser desorption/ionization (MALDI) tandem ion trap mass spectrometry requires efficient mass isolation and the ability to induce extensive sequence-specific fragmentation. The present paper describes a new excitation scheme, which we term red-shifted off-resonance large-amplitude excitation (RSORLAE), that can deposit higher amounts of internal energy in ions than is feasible with conventional resonant excitation. The new method provides an effective means for inducing fragmentation of MALDI-produced peptide ions with m/z values up to 3500. Prior to excitation, it is necessary to isolate ions of interest with high efficiency. We demonstrate that isolation efficiencies of > 95% can be achieved by careful design of the rf scan functions used during ion isolation. In particular, sudden transitions in the amplitude of the rf field (from low to high amplitudes) must be avoided. The combined improvements in the efficiency for ion isolation and the efficacy of ion activation make MALDI tandem ion trap mass spectrometry a practical tool for the characterization of proteins with high sensitivity.

Amino Acid Sequence↗
PubMed2004

Not ions alone: barriers to ion permeation in nanopores and channels.

A hydrophobic pore of subnanometer dimensions can appear impermeable to an ion even though its radius is still much wider than that of the ion. Pores of molecular dimensions can be found, for instance, in carbon nanotubes, zeolites, or ion channel proteins. We quantify this barrier to ion permeation by calculating the potential of mean force from umbrella-sampled molecular dynamics simulations and compare them to continuum-electrostatic Poisson-Boltzmann calculations. The latter fail to describe the ion barrier because they do not account for the properties of water in the pore. The barrier originates from the energetic cost to desolvate the ion. Even in wide pores, which could accommodate an ion and its hydration shell, a barrier of several kT remains because the liquid water phase is not stable in the hydrophobic pore. Thus, the properties of the solvent play a crucial role in determining permeation properties of ions in confinement at the molecular scale.

Journal Article↗
PubMed2004

Kinetic theory of radio frequency quadrupole ion traps. I. Trapping of atomic ions in a pure atomic gas.

A kinetic theory based on the Boltzmann equation is developed for the trapping of atomic ions in a radio-frequency quadrupole ion trap containing enough neutral atoms that ion-neutral collisions cannot be ignored. The collisions are treated at the same level of sophistication and detail as is used to deal with the time- and space-dependent electric fields in the trap. As a result, microscopic definitions are obtained for the damping and stochastic forces that originate from such collisions. These definitions contrast with corresponding phenomenological terms added ad hoc in previous treatments to create damped Mathieu and Langevin equations, respectively. Furthermore, the theory indicates that either collisional cooling or heating of the ions is possible, depending upon details of the ion-neutral mass ratios and interaction potential. The kinetic theory is not dependent on any special assumptions about the electric field strengths, the ion-neutral interaction potentials, or the ion-neutral mass ratio. It also provides an ab initio way to describe the ion kinetic energies, temperatures, and other properties by a series of successive approximations.

Journal Article↗
PubMed2006

Dynamics of lithium ions in bismuthate glasses: influence of strontium ions.

The influence of strontium ions on the relaxation dynamics of lithium ions in bismuthate glasses has been investigated in the frequency range of 10 Hz to 2 MHz. We have observed that the conductivity increases and the activation energy decreases with the increase of SrO content in the glass compositions with fixed Li2O content. We have also observed that the conductivity increases and the activation energy decreases when Sr2+ ions are replaced by Li+ ions, keeping the glass former content fixed. We have shown that the estimated mobile ion concentration is almost independent of temperature and SrO content in the compositions. We have further shown that a fraction of total lithium ions are mobile for all glass compositions. The results have been interpreted on the basis of the modification of the bismuthate network by the addition of SrO, which enhances the mobility of Li ions, without altering the mobile Li+ ion concentration. We have also shown that the conductivity relaxation in these glasses is independent of temperature and composition, and the nonexponential parameter is less than that for the lithium bismuthate glasses without SrO.

Journal Article↗
PubMed1989

The role of hydrated divalent metal ions in the bridging of two anionic groups. An ab initio quantum chemical and molecular mechanics study of dimethyl phosphate and formate bridged by calcium and magnesium ions.

Ab initio quantum chemical (Gaussian82) and molecular mechanics (AMBER2.0) computational techniques are employed to investigate the interaction of two anions (formate an dimethylphosphate) and a central divalent metal cation (magnesium or calcium). These systems are models for the essential GDP binding unit of the G-proteins (e.g., EF-Tu or the ras oncogene proteins) and for protein/phospholipid interactions, both of which are mediated by divalent metal cations. Various levels of hydration are utilized to examine coordination of differences between magnesium and calcium ions. Two different orientations of formate and dimethyl phosphate in direct ion contact with a magnesium ion and two waters of hydration were energy minimized with both quantum and molecular mechanics techniques. The structures and energy differences between the two orientations determined by either of the computational techniques are similar. Magnesium ion has a strong propensity to assume six coordination whereas calcium ion preferentially assumes a coordination greater than six. Likewise, water molecules attached to magnesium ion are held more rigidly than those of calcium ion, thus calcium ion is more accommodating in the exchange of water for negative ligands.

Calcium↗
PubMed2002

Ion-acoustic compressive and rarefactive double layers in a warm multicomponent plasma with negative ions.

Propagation of ion-acoustic double layers has been studied in plasma consisting of warm positive- and negative-ion species with different masses, concentrations, and charge states along with electrons with two-electron temperature distributions. It is found that there exist two critical concentrations of negative ions, alpha(R) and alpha(Q). One of them (alpha(R)) generally decides the existence of the double layer, whereas the other one (alpha(Q)) decides the nature of the double layer. It is found that the system supports ion-acoustic double layers only when the negative-ion concentration (alpha) is greater than the critical concentration alpha(R). It is also found that below the critical concentration alpha(Q), compressive double layers exist and above it rarefactive double layers exist. For some values of cold-electron concentrations (mu) it is found that if the temperature of the negative-ion species is higher than the positive-ion species, then the system supports compressive double layers for all values of alpha lying in the range 0<alpha<alpha(Q). The dependence of the critical concentrations on the temperatures of the two-ion species and on the concentration of cold electrons has also been investigated.

Journal Article↗
PubMed2004

Energy loss of ions and ion clusters in a disordered electron gas.

The various aspects of the correlated stopping power of pointlike and extended ions moving in a disordered degenerate electron gas have been analytically and numerically studied. Within the linear response theory we have made a systematic and comprehensive investigation of correlated stopping power, vicinage function, and related quantities for protons and extended ions, as well as for their clusters. The disorder, which leads to a damping of plasmons and quasiparticles in the electron gas, is taken into account through a relaxation time approximation in the linear response function. The stopping power for an arbitrary extended ion with a single bound electron is calculated in both the low- and high velocity limits. Our analytical results show that in a high velocity limit the main logarithmic contribution to the stopping power for an extended ion is significantly modified and for instance, in the case of He+, Li2+, and Be3+ ions must behave as ln ( A v(5) ), ln ( A v(3.25) ), and ln ( A v(2.77) ), respectively where v is the ion velocity. This behavior may be contrasted with the usual ln ( v(2) ) dependence for a point ion projectile. It is shown that the factor A which depends on the damping can be significantly reduced by increasing the latter. In order to highlight the effects of damping we present a comparison of our analytical and numerical results, in the case of both pointlike and extended ions, obtained for a nonzero damping with those for a vanishing damping.

Journal Article↗
PubMed1996

Use-dependent blockers and exit rate of the last ion from the multi-ion pore of a K+ channel.

Quaternary ammonium blockers inhibit many voltage-activated potassium (K+) channels from the intracellular side. When applied to Drosophila Shaker potassium channels expressed in mammalian cells, these rapidly reversible blockers produced use-dependent inhibition through an unusual mechanism--they promoted an intrinsic conformational change known as C-type inactivation, from which recovery is slow. The blockers did so by cutting off potassium ion flow to a site in the pore, which then emptied at a rate of 10(5) ions per second. This slow rate probably reflected the departure of the last ion from the multi-ion pore: Permeation of ions (at 10(7) per second) occurs rapidly because of ion-ion repulsion, but the last ion to leave would experience no such repulsion.

Binding Sites↗
PubMed2005

Rapid analysis of polychlorinated biphenyls in the gas phase with resonance-enhanced two-photon ionization: optimal injection of ions into the ion-trap storage/time-of-flight mass spectrometer.

LI-IT-TOFMS (laser ionization/ion-trap storage/time-of-flight mass spectrometry) is expected to be a powerful tool for environmental monitoring. In the research reported here, real-time LI-IT-TOFMS measurements were carried out on gaseous 2-4 chlorinated PCBs in order to evaluate the applicability of an environmental monitoring method. With respect to ion-trap storage for PCBs, we found that the effect was due to the driving RF voltage on the ring electrode in the ion trap. For PCBs ions produced by laser irradiation, we observed that it was more efficient to reach the center of the ion trap by using a gated RF voltage rather than by using a continuous RF voltage. The ion trajectories in the ion trap were simulated by SIMION 7.0. We found that the voltage of the exit end cap electrode affected both the number of ions trapped and the orbit of ions inside the trap cell. Optimization of this parameter was performed using both simulated and experimental results. The achievable PCBs sensitivity for real-time (1 min) measurement using the LI-IT-TOFMS method was found to be in the pptV range (<0.01 mg/m3N) by means of a comparison with the conventional gas sampling/GS-MS method. A satisfactory proportional relationship was confirmed between the laser-based and conventional results.

Environmental Monitoring↗
PubMed2004

Orthogonal time-of-flight secondary ion mass spectrometric analysis of peptides using large gold clusters as primary ions.

Secondary ion mass spectrometry (SIMS) for biomolecular analysis is greatly enhanced by the instrumental combination of orthogonal extraction time-of-flight mass spectrometry with massive gold cluster primary ion bombardment. Precursor peptide molecular ion yield enhancements of 1000, and signal-to-noise improvements of up to 20, were measured by comparing SIMS spectra obtained using Au(+) and massive Au(400) (4+) cluster primary ion bombardment of neat films of the neuropeptide fragment dynorphin 1-7. Remarkably low damage cross-sections were also measured from dynorphin 1-7 and gramicidin S during prolonged bombardment with 40 keV Au(400) (4+). For gramicidin S, the molecular ion yield increases slightly as a function of Au(400) (4+) beam fluence up to at least 2 x 10(13) Au(400) (4+)/cm(2). This is in marked contrast to the rapid decrease observed when bombarding with ions such as Au(5) (+) and Au(9) (+). When gramicidin S is impinged with Au(5) (+), the molecular ion yield decreases by a factor of 10 after a fluence of only 8 x 10(12) ions/cm(2). Comparison of these damage cross-sections implies that minimal surface damage occurs during prolonged Au(400) (4+) bombardment. Several practical analytical implications are drawn from these observations.

Dynorphins↗
PubMed2004

Tissue molecular ion imaging by gold cluster ion bombardment.

The use of gold cluster focused ion beams produced by a liquid metal ion gun in a TOF-SIMS mass spectrometer is shown to dramatically enhance secondary ion emission of phospholipids and peptides. The method has been successfully tested with cells grown onto plastic slips and with mouse brain slices, without any treatment of the samples. Very reliable time-of-flight mass spectra are acquired with a low primary ion dose of a few 10(7) ions, and high lateral resolution molecular ion images are obtained for heavy ions of great biological interest. This approach offers new opportunities in pharmacological and biological research fields by localizing compounds of interest such as drugs or metabolites in tissues.

Animals↗
PubMed1997

Stabilization of ion selectivity filter by pore loop ion pairs in an inwardly rectifying potassium channel.

Ion selectivity is critical for the biological functions of voltage-dependent cation channels and is achieved by specific ion binding to a pore region called the selectivity filter. In voltage-gated K+, Na+ and Ca2+ channels, the selectivity filter is formed by a short polypeptide loop (called the H5 or P region) between the fifth and sixth transmembrane segments, donated by each of the four subunits or internal homologous domains forming the channel. While mutagenesis studies on voltage-gated K+ channels have begun to shed light on the structural organization of this pore region, little is known about the physical and chemical interactions that maintain the structural stability of the selectivity filter. Here we show that in an inwardly rectifying K+ (IRK) channel, IRK1, short range interactions of an ion pair in the H5 pore loop are crucial for pore structure and ion permeation. The two residues, a glutamate and an arginine, appear to form exposed salt bridges in the tetrameric channel. Alteration or disruption of such ion pair interactions dramatically alters ion selectivity and permeation. Since this ion pair is conserved in all IRK channels, it may constitute a general mechanism for maintaining the stability of the pore structure in this channel superfamily.

Amino Acid Sequence↗
PubMed1999

Intraneuronal ion distribution during experimental oxygen/glucose deprivation. Routes of ion flux as targets of neuroprotective strategies.

Ischemic neuronal injury appears to be mediated by disruption of subcellular ion distribution and, therefore, prevention of ion relocation might be neuroprotective. X-ray microanalysis was used to measure concentrations of Na, K, Ca and other elements in subcellular compartments (e.g., mitochondria) of CA1 neurons from oxygen/glucose-deprived (OGD) hippocampal slices. Results showed that OGD produced progressive loss of ion regulation in CA1 cells. Post-OGD reperfusion with normal media exacerbated the initial ion deregulation. To study neuroprotective mechanisms, we determined the ability of hypothermia (31 degrees C) or ion channel blockade to retard intraneuronal ion disruption induced by OGD/reperfusion. Whereas Ca2+ channel blockade (omega-conotoxin MVIIC, 3 microM) was ineffective, hypothermia and Na+ channel blockers (tetrodotoxin, TTX, 1 microM; lidocaine, 200 microM) reduced ion deregulation in subneuronal compartments. Blockade of glutamate receptors (AMPA, 10 microM; the non-NMDA receptor antagonist CNQX, 10 microM/100 microM glycine; the NMDA receptor antagonist CCP, 100 microM) during OGD/reperfusion provided nearly complete protection. These findings provide a foundation for identifying potential pharmacotherapeutic approaches and for discerning corresponding mechanisms of neuroprotection.

Animals↗
PubMed1998

Ion transport in chondrocytes: membrane transporters involved in intracellular ion homeostasis and the regulation of cell volume, free [Ca2+] and pH.

Chondrocytes exist in an unusual and variable ionic and osmotic environment in the extracellular matrix of cartilage and are responsible for maintaining the delicate equilibrium between extracellular matrix synthesis and degradation. The mechanical performance of cartilage relies on the biochemical properties of the matrix. Alterations to the ionic and osmotic extracellular environment of chondrocytes have been shown to influence the volume, intracellular pH and ionic content of the cells, which in turn modify the synthesis and degradation of extracellular matrix macromolecules. Physiological ion homeostasis is fundamental to the routine functioning of cartilage and the factors that control the integrity of this highly evolved and specialized tissue. Ion transport in cartilage is relatively unexplored and the biochemical properties and molecular identity of membrane transport mechanisms employed by chondrocytes in the control of intracellular ion concentrations and pH is not fully defined and this review focuses on these processes. Chondrocytes have been shown to express voltage and stretch activated ion channels, passive exchangers and ATP dependent ion pumps. In addition, recent studies of transport systems in chondrocytes have demonstrated the presence of isozyme diversity that includes Na+/H+ exchange (NHE1, NHE3), Na+, K(+)-ATPase (several isoforms) and others each of which possess considerably different kinetic properties and modes of regulation. This multitude of isozyme diversity indicates the highly specialized handling of ions and protons in order to accomplish a fine regulation of their transmembrane fluxes. The complexities of these transport systems and their patterns of isoform expression underscore the subtlety of ion homeostasis and pH regulation in normal cartilage. Perturbations in these mechanisms may affect the physiological turnover of cartilage and thus increase the susceptibility to degenerative joint disease.

Animals↗
PubMed2005

Local structures of ions at ion-exchange resin/solution interface.

The local structures of Cl- and Br- in anion-exchange resins have been studied by X-ray absorption fine structure (XAFS), and separation selectivity is discussed on the basis of results. When two different anion-exchange resins having trimethylammonium and dimethylammonium groups as anion-exchange groups are employed for ion-exchange experiments, slightly higher Br- selectivity has been obtained with the former. XAFS has indicated that the average hydration numbers for a given anion is not affected by the structure of the ion-exchange group, but that the extent of ion-association between the anion and the ion-exchange groups depends on the type of the ion-exchange group. Shorter interaction distance (and in turn stronger ion-association) has been confirmed for the dimethylammonium-type resin, and is consistent with lower Br- selectivity of this resin.

Anion Exchange Resins↗