Correlating Resolving Power, Resolution, and Collision Cross Section: Unifying Cross-Platform Assessment of Separation Efficiency in Ion Mobility Spectrometry.

PubMed

Dodds, James N; May, Jody C; McLean, John A

2017-11-21

Here we examine the relationship among resolving power (R p ), resolution (R pp ), and collision cross section (CCS) for compounds analyzed in previous ion mobility (IM) experiments representing a wide variety of instrument platforms and IM techniques. Our previous work indicated these three variables effectively describe and predict separation efficiency for drift tube ion mobility spectrometry experiments. In this work, we seek to determine if our previous findings are a general reflection of IM behavior that can be applied to various instrument platforms and mobility techniques. Results suggest IM distributions are well characterized by a Gaussian model and separation efficiency can be predicted on the basis of the empirical difference in the gas-phase CCS and a CCS-based resolving power definition (CCS/ΔCCS). Notably traveling wave (TWIMS) was found to operate at resolutions substantially higher than a single-peak resolving power suggested. When a CCS-based R p definition was utilized, TWIMS was found to operate at a resolving power between 40 and 50, confirming the previous observations by Giles and co-workers. After the separation axis (and corresponding resolving power) is converted to cross section space, it is possible to effectively predict separation behavior for all mobility techniques evaluated (i.e., uniform field, trapped ion mobility, traveling wave, cyclic, and overtone instruments) using the equations described in this work. Finally, we are able to establish for the first time that the current state-of-the-art ion mobility separations benchmark at a CCS-based resolving power of >300 that is sufficient to differentiate analyte ions with CCS differences as small as 0.5%.

Time-resolved VUV spectroscopy in the EXTRAP-T2 reversed field pinch

NASA Astrophysics Data System (ADS)

Hedqvist, Anders; Rachlew-Källne, Elisabeth

1998-09-01

Time-resolved VUV spectroscopy has been used to investigate the effects of impurities in a reversed field pinch operating with a resistive shell. Results of electron temperature, impurity ion densities, particle confinement time and 0741-3335/40/9/004/img1 together with a description of the interpretation and the equipment are presented.

Development of a New Time-Resolved Laser-Induced Fluorescence Technique

NASA Astrophysics Data System (ADS)

Durot, Christopher; Gallimore, Alec

2012-10-01

We are developing a time-resolved laser-induced fluorescence (LIF) technique to interrogate the ion velocity distribution function (VDF) of EP thruster plumes down to the microsecond time scale. Better measurements of dynamic plasma processes will lead to improvements in simulation and prediction of thruster operation and erosion. We present the development of the new technique and results of initial tests. Signal-to-noise ratio (SNR) is often a challenge for LIF studies, and it is only more challenging for time-resolved measurements since a lock-in amplifier cannot be used with a long time constant. The new system uses laser modulation on the order of MHz, which enables the use of electronic filtering and phase-sensitive detection to improve SNR while preserving time-resolved information. Statistical averaging over many cycles to further improve SNR is done in the frequency domain. This technique can have significant advantages, including (1) larger spatial maps enabled by shorter data acquisition time and (2) the ability to average data without creating a phase reference by modifying the thruster operating condition with a periodic cutoff in discharge current, which can modify the ion velocity distribution.

Time-Resolved Magnetic Field Effects Distinguish Loose Ion Pairs from Exciplexes

PubMed Central

2013-01-01

We describe the experimental investigation of time-resolved magnetic field effects in exciplex-forming organic donor–acceptor systems. In these systems, the photoexcited acceptor state is predominantly deactivated by bimolecular electron transfer reactions (yielding radical ion pairs) or by direct exciplex formation. The delayed fluorescence emitted by the exciplex is magnetosensitive if the reaction pathway involves loose radical ion pair states. This magnetic field effect results from the coherent interconversion between the electronic singlet and triplet radical ion pair states as described by the radical pair mechanism. By monitoring the changes in the exciplex luminescence intensity when applying external magnetic fields, details of the reaction mechanism can be elucidated. In this work we present results obtained with the fluorophore-quencher pair 9,10-dimethylanthracene/N,N-dimethylaniline (DMA) in solvents of systematically varied permittivity. A simple theoretical model is introduced that allows discriminating the initial state of quenching, viz., the loose ion pair and the exciplex, based on the time-resolved magnetic field effect. The approach is validated by applying it to the isotopologous fluorophore-quencher pairs pyrene/DMA and pyrene-d10/DMA. We detect that both the exciplex and the radical ion pair are formed during the initial quenching stage. Upon increasing the solvent polarity, the relative importance of the distant electron transfer quenching increases. However, even in comparably polar media, the exciplex pathway remains remarkably significant. We discuss our results in relation to recent findings on the involvement of exciplexes in photoinduced electron transfer reactions. PMID:24041160

From Supercomputer Modeling to Highest Mass Resolution in FT-ICR.

PubMed

N Nikolaev, Evgene; N Vladimirov, Gleb; Jertz, Roland; Baykut, Gökhan

2013-01-01

Understanding of behavior of ion ensembles inside FT-ICR cell based on the computer simulation of ion motion gives rise to the new ideas of cell designs. The recently introduced novel FT-ICR cell based on a Penning ion trap with specially shaped excitation and detection electrodes prevents distortion of ion cyclotron motion phases (normally caused by non-ideal electric trapping fields) by averaging the trapping DC electric field during the ion motion in the ICR cell. Detection times of 5 min resulting in resolving power close to 40,000,000 have been reached for reserpine at m/z 609 at a magnetic field of only 7 Tesla. Fine structures of resolved 13Cn isotopic cluster groups could be measured for molecular masses up to 5.7 kDa (insulin) with resolving power of 4,000,000 at 7 Tesla. Based on resolved fine structure patterns atomic compositions can be directly determined using a new developed algorithm for fine structure processing. Mass spectra of proteins and multimers of proteins reaching masses up to 186 kDa (enolase tetramer) could be measured with isotopic resolution. For instance, at 7 Tesla resolving power of 800,000 was achieved for enolase dimer (96 kDa) and 500,000 for molecular masses above 100 kDa. Experimental data indicate that there is practically no limit for the resolving power of this ICR cell except by collisional damping in the ultrahigh vacuum chamber.

Observation of inhibited electron-ion coupling in strongly heated graphite

PubMed Central

White, T. G.; Vorberger, J.; Brown, C. R. D.; Crowley, B. J. B.; Davis, P.; Glenzer, S. H.; Harris, J. W. O.; Hochhaus, D. C.; Le Pape, S.; Ma, T.; Murphy, C. D.; Neumayer, P.; Pattison, L. K.; Richardson, S.; Gericke, D. O.; Gregori, G.

2012-01-01

Creating non-equilibrium states of matter with highly unequal electron and lattice temperatures (Tele≠Tion) allows unsurpassed insight into the dynamic coupling between electrons and ions through time-resolved energy relaxation measurements. Recent studies on low-temperature laser-heated graphite suggest a complex energy exchange when compared to other materials. To avoid problems related to surface preparation, crystal quality and poor understanding of the energy deposition and transport mechanisms, we apply a different energy deposition mechanism, via laser-accelerated protons, to isochorically and non-radiatively heat macroscopic graphite samples up to temperatures close to the melting threshold. Using time-resolved x ray diffraction, we show clear evidence of a very small electron-ion energy transfer, yielding approximately three times longer relaxation times than previously reported. This is indicative of the existence of an energy transfer bottleneck in non-equilibrium warm dense matter. PMID:23189238

In-SITU, Time-resolved Raman Spectro-micro-topography of an Operating Lithium Ion Battery

NASA Technical Reports Server (NTRS)

Luo, Yu; Cai, Wen-Bin; Xing, Xue-Kun; Scherson, Daniel A.

2003-01-01

A Raman microscope has been coupled to a computer-controlled, two-dimensional linear translator attached to a custom-designed, sealed optical chamber to allow in situ acquisition of space-, and time-resolved spectra of an operating thin graphite/LiCoO2 Li-ion battery. This unique arrangement made it possible to collect continuously series of Raman spectra from a sharply defined edge of the battery exposing the anode (A), separator (S), and cathode (C), during charge and discharge, while the device was moved back and forth under the fixed focused laser beam along an axis normal to the layered A/S/C plane. Clear spectral evidence was obtained for changes in the amount of Li(+) within particles of graphite in the anode, and, to a lesser extent, of LiCoO2 in the cathode, during battery discharge both as a function of position and time. Analysis of time-resolved Raman spectro-micro-topography (SMT) measurements of the type described in this work are expected to open new prospects for assessing the validity of theoretical models aimed at simulating the flow of Li(+) within Li-ion batteries under operating conditions.

Investigations on the photoreactions of phenothiazine and phenoxazine in presence of 9-cyanoanthracene by using steady state and time resolved spectroscopic techniques.

PubMed

Bardhan, Munmun; Mandal, Paulami; Tzeng, Wen-Bih; Ganguly, Tapan

2010-09-01

By using electrochemical, steady state and time resolved (fluorescence lifetime and transient absorption) spectroscopic techniques, detailed investigations were made to reveal the mechanisms of charge separation or forward electron transfer reactions within the electron donor phenothiazine (PTZH) or phenoxazine (PXZH) and well known electron acceptor 9-cyanoanthracene (CNA). The transient absorption spectra suggest that the charge separated species formed in the excited singlet state resulted from intermolecular photoinduced electron transfer reactions within the donor PTZH (or PXZH) and CNA acceptor relaxes to the corresponding triplet state. Though alternative mechanisms of via formations of contact neutral radical by H-transfer reaction have been proposed but the observed results obtained from the time resolved measurements indicate that the regeneration of ground state reactants is primarily responsible due to direct recombination of triplet contact ion-pair (CIP) or solvent-separated ion-pair (SSIP).

Voltage sweep ion mobility spectrometry.

PubMed

Davis, Eric J; Williams, Michael D; Siems, William F; Hill, Herbert H

2011-02-15

Ion mobility spectrometry (IMS) is a rapid, gas-phase separation technique that exhibits excellent separation of ions as a standalone instrument. However, IMS cannot achieve optimal separation power with both small and large ions simultaneously. Similar to the general elution problem in chromatography, fast ions are well resolved using a low electric field (50-150 V/cm), whereas slow drifting molecules are best separated using a higher electric field (250-500 V/cm). While using a low electric field, IMS systems tend to suffer from low ion transmission and low signal-to-noise ratios. Through the use a novel voltage algorithm, some of these effects can be alleviated. The electric field was swept from low to high while monitoring a specific drift time, and the resulting data were processed to create a 'voltage-sweep' spectrum. If an optimal drift time is calculated for each voltage and scanned simultaneously, a spectrum may be obtained with optimal separation throughout the mobility range. This increased the resolving power up to the theoretical maximum for every peak in the spectrum and extended the peak capacity of the IMS system, while maintaining accurate drift time measurements. These advantages may be extended to any IMS, requiring only a change in software.

Effect of gas filling pressure and operation energy on ion and neutron emission in a medium energy plasma focus device

NASA Astrophysics Data System (ADS)

Niranjan, Ram; Rout, R. K.; Srivastava, Rohit; Kaushik, T. C.

2018-03-01

The effects of gas filling pressure and operation energy on deuterium ions and neutrons have been studied in a medium energy plasma focus device, MEPF-12. The deuterium gas filling pressure was varied from 1 to 10 mbar at an operation energy of 9.7 kJ. Also, the operation energy was varied from 3.9 to 9.7 kJ at a deuterium gas filling pressure of 4 mbar. Time resolved emission of deuterium ions was measured using a Faraday cup. Simultaneously, time integrated and time resolved emissions of neutrons were measured using a silver activation detector and plastic scintillator detector, respectively. Various characteristics (fluence, peak density, and most probable energy) of deuterium ions were estimated using the Faraday cup signal. The fluence was found to be nearly independent of the gas filling pressure and operation energy, but the peak density and most probable energy of deuterium ions were found to be varying. The neutron yield was observed to be varying with the gas filling pressure and operation energy. The effect of ions on neutrons emission was observed at each operation condition.

Ultra High Resolution Linear Ion Trap Orbitrap Mass Spectrometer (Orbitrap Elite) Facilitates Top Down LC MS/MS and Versatile Peptide Fragmentation Modes*

PubMed Central

Michalski, Annette; Damoc, Eugen; Lange, Oliver; Denisov, Eduard; Nolting, Dirk; Müller, Mathias; Viner, Rosa; Schwartz, Jae; Remes, Philip; Belford, Michael; Dunyach, Jean-Jacques; Cox, Juergen; Horning, Stevan; Mann, Matthias; Makarov, Alexander

2012-01-01

Although only a few years old, the combination of a linear ion trap with an Orbitrap analyzer has become one of the standard mass spectrometers to characterize proteins and proteomes. Here we describe a novel version of this instrument family, the Orbitrap Elite, which is improved in three main areas. The ion transfer optics has an ion path that blocks the line of sight to achieve more robust operation. The tandem MS acquisition speed of the dual cell linear ion trap now exceeds 12 Hz. Most importantly, the resolving power of the Orbitrap analyzer has been increased twofold for the same transient length by employing a compact, high-field Orbitrap analyzer that almost doubles the observed frequencies. An enhanced Fourier Transform algorithm—incorporating phase information—further doubles the resolving power to 240,000 at m/z 400 for a 768 ms transient. For top-down experiments, we combine a survey scan with a selected ion monitoring scan of the charge state of the protein to be fragmented and with several HCD microscans. Despite the 120,000 resolving power for SIM and HCD scans, the total cycle time is within several seconds and therefore suitable for liquid chromatography tandem MS. For bottom-up proteomics, we combined survey scans at 240,000 resolving power with data-dependent collision-induced dissociation of the 20 most abundant precursors in a total cycle time of 2.5 s—increasing protein identifications in complex mixtures by about 30%. The speed of the Orbitrap Elite furthermore allows scan modes in which complementary dissociation mechanisms are routinely obtained of all fragmented peptides. PMID:22159718

In-depth study of in-trap high-resolution mass separation by transversal ion ejection from a multi-reflection time-of-flight device.

PubMed

Fischer, Paul; Knauer, Stefan; Marx, Gerrit; Schweikhard, Lutz

2018-01-01

The recently introduced method of ion separation by transversal ejection of unwanted species in electrostatic ion-beam traps and multi-reflection time-of-flight devices has been further studied in detail. As this separation is performed during the ion storage itself, there is no need for additional external devices such as ion gates or traps for either pre- or postselection of the ions of interest. The ejection of unwanted contaminant ions is performed by appropriate pulses of the potentials of deflector electrodes. These segmented ring electrodes are located off-center in the trap, i.e., between one of the two ion mirrors and the central drift tube, which also serves as a potential lift for capturing incoming ions and axially ejecting ions of interest after their selection. The various parameters affecting the selection effectivity and resolving power are illustrated with tin-cluster measurements, where isotopologue ion species provide mass differences down to a single atomic mass unit at ion masses of several hundred. Symmetric deflection voltages of only 10 V were found sufficient for the transversal ejection of ion species with as few as three deflection pulses. The duty cycle, i.e., the pulse duration with respect to the period of ion revolution, has been varied, resulting in resolving powers of up to several tens of thousands for this selection technique.

In-depth study of in-trap high-resolution mass separation by transversal ion ejection from a multi-reflection time-of-flight device

NASA Astrophysics Data System (ADS)

Fischer, Paul; Knauer, Stefan; Marx, Gerrit; Schweikhard, Lutz

2018-01-01

The recently introduced method of ion separation by transversal ejection of unwanted species in electrostatic ion-beam traps and multi-reflection time-of-flight devices has been further studied in detail. As this separation is performed during the ion storage itself, there is no need for additional external devices such as ion gates or traps for either pre- or postselection of the ions of interest. The ejection of unwanted contaminant ions is performed by appropriate pulses of the potentials of deflector electrodes. These segmented ring electrodes are located off-center in the trap, i.e., between one of the two ion mirrors and the central drift tube, which also serves as a potential lift for capturing incoming ions and axially ejecting ions of interest after their selection. The various parameters affecting the selection effectivity and resolving power are illustrated with tin-cluster measurements, where isotopologue ion species provide mass differences down to a single atomic mass unit at ion masses of several hundred. Symmetric deflection voltages of only 10 V were found sufficient for the transversal ejection of ion species with as few as three deflection pulses. The duty cycle, i.e., the pulse duration with respect to the period of ion revolution, has been varied, resulting in resolving powers of up to several tens of thousands for this selection technique.

Time-resolved laser spectroscopy of multiply ionized atoms: natural radiative lifetimes in Ce IV.

PubMed

Zhang, Z G; Svanberg, S; Quinet, P; Palmeri, P; Biémont, E

2001-12-31

Radiative lifetimes have been measured for two excited levels of Ce IV using the time-resolved laser-induced fluorescence technique. Ce3+ ions were produced in a laser-induced plasma. In the measurements, a suitable magnetic field was applied to reduce the recombination between electrons and the ions and thus the background light from the recombination, and special care was exercised to avoid flight-out-of-view effects on the lifetime measurements for the high-velocity ions. The experimental lifetime results, tau = 30(2) ns for the level 49 737 cm(-1) and tau = 30(3) ns for the level 52 226 cm(-1), were compared with relativistic Hartree-Fock calculations (tau = 30.5 and 30.0 ns) indicating a particularly excellent agreement.

Depth-Resolved Cathodoluminescence of Thorium Dioxide

DTIC Science & Technology

2013-03-01

exhibited more of an energy dependency than the cut and polished sample. However, in a companion study, ime of flight secondary ion mass spectrometry...Ion Mass Spectrometry (TOF SIMS) ......................17 2.7 Atomic Force Microscope (AFM...1 TOF SIMS……….Time of Flight Secondary Ion Mass Spectroscopy……………….62 1 DEPTH

Time-Resolved Chemical Mapping in Light-Emitting Electrochemical Cells.

PubMed

Jafari, Mohammad Javad; Liu, Jiang; Engquist, Isak; Ederth, Thomas

2017-01-25

An understanding of the doping and ion distributions in light-emitting electrochemical cells (LECs) is required to approach a realistic conduction model which can precisely explain the electrochemical reactions, p-n junction formation, and ion dynamics in the active layer and to provide relevant information about LECs for systematic improvement of function and manufacture. Here, Fourier-transform infrared (FTIR) microscopy is used to monitor anion density profile and polymer structure in situ and for time-resolved mapping of electrochemical doping in an LEC under bias. The results are in very good agreement with the electrochemical doping model with respect to ion redistribution and formation of a dynamic p-n junction in the active layer. We also physically slow ions by decreasing the working temperature and study frozen-junction formation and immobilization of ions in a fixed-junction LEC device by FTIR imaging. The obtained results show irreversibility of the ion redistribution and polymer doping in a fixed-junction device. In addition, we demonstrate that infrared microscopy is a useful tool for in situ characterization of electroactive organic materials.

Multidimensional Separation of Natural Products Using Liquid Chromatography Coupled to Hadamard Transform Ion Mobility Mass Spectrometry

NASA Astrophysics Data System (ADS)

Liu, Wenjie; Zhang, Xing; Knochenmuss, Richard; Siems, William F.; Hill, Herbert H.

2016-05-01

A high performance liquid chromatograph (HPLC)was interfaced to an atmospheric drift tube ion mobility time of flight mass spectrometry. The power of multidimensional separation was demonstrated using chili pepper extracts. The ambient pressure drift tube ion mobility provided high resolving powers up to 166 for the HPLC eluent. With implementation of Hadamard transform (HT), the duty cycle for the ion mobility drift tube was increased from less than 1% to 50%, and the ion transmission efficiency was improved by over 200 times compared with pulsed mode, improving signal to noise ratio 10 times. HT ion mobility and TOF mass spectrometry provide an additional dimension of separation for complex samples without increasing the analysis time compared with conventional HPLC.

Information hidden in the velocity distribution of ions and the exact kinetic Bohm criterion

NASA Astrophysics Data System (ADS)

Tsankov, Tsanko V.; Czarnetzki, Uwe

2017-05-01

Non-equilibrium distribution functions of electrons and ions play an important role in plasma physics. A prominent example is the kinetic Bohm criterion. Since its first introduction it has been controversial for theoretical reasons and due to the lack of experimental data, in particular on the ion distribution function. Here we resolve the theoretical as well as the experimental difficulties by an exact solution of the kinetic Boltzmann equation including charge exchange collisions and ionization. This also allows for the first time non-invasive measurement of spatially resolved ion velocity distributions, absolute values of the ion and electron densities, temperatures, and mean energies as well as the electric field and the plasma potential in the entire plasma. The non-invasive access to the spatially resolved distribution functions of electrons and ions is applied to the problem of the kinetic Bohm criterion. Theoretically a so far missing term in the criterion is derived and shown to be of key importance. With the new term the validity of the kinetic criterion at high collisionality and its agreement with the fluid picture are restored. All findings are supported by experimental data, theory and a numerical model with excellent agreement throughout.

Picosecond time-resolved measurements of dense plasma line shifts

DOE PAGES

Stillman, C. R.; Nilson, P. M.; Ivancic, S. T.; ...

2017-06-13

Picosecond time-resolved x-ray spectroscopy is used to measure the spectral line shift of the 1s2p–1s 2 transition in He-like Al ions as a function of the instantaneous plasma conditions. The plasma temperature and density are inferred from the Al He α complex using a nonlocal-thermodynamic-equilibrium atomic physics model. The experimental spectra show a linearly increasing red shift for electron densities of 1 to 5 × 10 23 cm –3. Furthermore, the measured line shifts are broadly consistent with a generalized analytic line-shift model based on calculations of a self-consistent field ion sphere model.

Picosecond time-resolved measurements of dense plasma line shifts

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stillman, C. R.; Nilson, P. M.; Ivancic, S. T.

Picosecond time-resolved x-ray spectroscopy is used to measure the spectral line shift of the 1s2p–1s 2 transition in He-like Al ions as a function of the instantaneous plasma conditions. The plasma temperature and density are inferred from the Al He α complex using a nonlocal-thermodynamic-equilibrium atomic physics model. The experimental spectra show a linearly increasing red shift for electron densities of 1 to 5 × 10 23 cm –3. Furthermore, the measured line shifts are broadly consistent with a generalized analytic line-shift model based on calculations of a self-consistent field ion sphere model.

Numerical simulation of the kinetic effects in the solar wind

NASA Astrophysics Data System (ADS)

Sokolov, I.; Toth, G.; Gombosi, T. I.

2017-12-01

Global numerical simulations of the solar wind are usually based on the ideal or resistive MagnetoHydroDynamics (MHD) equations. Within a framework of MHD the electric field is assumed to vanish in the co-moving frame of reference (ideal MHD) or to obey a simple and non-physical scalar Ohm's law (resistive MHD). The Maxwellian distribution functions are assumed, the electron and ion temperatures may be different. Non-disversive MHD waves can be present in this numerical model. The averaged equations for MHD turbulence may be included as well as the energy and momentum exchange between the turbulent and regular motion. With the use of explicit numerical scheme, the time step is controlled by the MHD wave propagtion time across the numerical cell (the CFL condition) More refined approach includes the Hall effect vie the generalized Ohm's law. The Lorentz force acting on light electrons is assumed to vanish, which gives the expression for local electric field in terms of the total electric current, the ion current as well as the electron pressure gradient and magnetic field. The waves (whistlers, ion-cyclotron waves etc) aquire dispersion and the short-wavelength perturbations propagate with elevated speed thus strengthening the CFL condition. If the grid size is sufficiently small to resolve ion skindepth scale, then the timestep is much shorter than the ion gyration period. The next natural step is to use hybrid code to resolve the ion kinetic effects. The hybrid numerical scheme employs the same generalized Ohm's law as Hall MHD and suffers from the same constraint on the time step while solving evolution of the electromagnetic field. The important distiction, however, is that by sloving particle motion for ions we can achieve more detailed description of the kinetic effect without significant degrade in the computational efficiency, because the time-step is sufficient to resolve the particle gyration. We present the fisrt numerical results from coupled BATS-R-US+ALTOR code as applied to kinetic simulations of the solar wind.

Selective time-resolved binding of copper(II) by pyropheophorbide-a methyl ester.

PubMed

Ghosh, Indrajit; Saleh, Na'il; Nau, Werner M

2010-05-01

The complexation behavior of pyropheophorbide-a methyl ester (PPME) with transition metal ions as well as other biologically relevant metal ions has been investigated in water-DMF (2 : 1 v/v) solution. PPME was found to selectively complex Cu(2+) ions, which leads to a distinct change in its absorption spectrum as well as efficient fluorescence quenching. The degree of fluorescence quenching by Cu(2+) depended on concentration and time. Upon addition of Cu(2+), the fluorescence showed a time-resolved decay on the time scale of minutes to hours, with the decay rate being dependent on the cation concentration. Fitting according to a bimolecular reaction rate law provided a rate constant of 650 +/- 90 M(-1) s(-1) at 298 K for metallochlorin formation. The potential implications of Cu(2+) binding for the use of PPME in photodynamic therapy are discussed, along with its use as a fluorescent sensor for detection of micromolar concentrations of Cu(2+).

Multi-Pass Quadrupole Mass Analyzer

NASA Technical Reports Server (NTRS)

Prestage, John D.

2013-01-01

Analysis of the composition of planetary atmospheres is one of the most important and fundamental measurements in planetary robotic exploration. Quadrupole mass analyzers (QMAs) are the primary tool used to execute these investigations, but reductions in size of these instruments has sacrificed mass resolving power so that the best present-day QMA devices are still large, expensive, and do not deliver performance of laboratory instruments. An ultra-high-resolution QMA was developed to resolve N2 +/CO+ by trapping ions in a linear trap quadrupole filter. Because N2 and CO are resolved, gas chromatography columns used to separate species before analysis are eliminated, greatly simplifying gas analysis instrumentation. For highest performance, the ion trap mode is used. High-resolution (or narrow-band) mass selection is carried out in the central region, but near the DC electrodes at each end, RF/DC field settings are adjusted to allow broadband ion passage. This is to prevent ion loss during ion reflection at each end. Ions are created inside the trap so that low-energy particles are selected by low-voltage settings on the end electrodes. This is beneficial to good mass resolution since low-energy particles traverse many cycles of the RF filtering fields. Through Monte Carlo simulations, it is shown that ions are reflected at each end many tens of times, each time being sent back through the central section of the quadrupole where ultrahigh mass filtering is carried out. An analyzer was produced with electrical length orders of magnitude longer than its physical length. Since the selector fields are sized as in conventional devices, the loss of sensitivity inherent in miniaturizing quadrupole instruments is avoided. The no-loss, multi-pass QMA architecture will improve mass resolution of planetary QMA instruments while reducing demands on the RF electronics for high-voltage/high-frequency production since ion transit time is no longer limited to a single pass. The QMA-based instrument will thus give way to substantial reductions of the mass of flight instruments.

Multiple-reflection time-of-flight mass spectrometry for in situ applications

NASA Astrophysics Data System (ADS)

Dickel, T.; Plaß, W. R.; Lang, J.; Ebert, J.; Geissel, H.; Haettner, E.; Jesch, C.; Lippert, W.; Petrick, M.; Scheidenberger, C.; Yavor, M. I.

2013-12-01

Multiple-reflection time-of-flight mass spectrometers (MR-TOF-MS) have recently been installed at different low-energy radioactive ion beam facilities. They are used as isobar separators with high ion capacity and as mass spectrometers with high mass resolving power and accuracy for short-lived nuclei. Furthermore, MR-TOF-MS have a huge potential for applications in other fields, such as chemistry, biology, medicine, space science, and homeland security. The development, commissioning and results of an MR-TOF-MS is presented, which serves as proof-of-principle to show that very high mass resolving powers (∼105) can be achieved in a compact device (length ∼30 cm). Based on this work, an MR-TOF-MS for in situ application has been designed. For the first time, this device combines very high mass resolving power (>105), mobility, and an atmospheric pressure inlet in one instrument. It will enable in situ measurements without sample preparation at very high mass accuracy. Envisaged applications of this mobile MR-TOF-MS are discussed.

Electron and ion dynamics study of iron in warm dense matter regime by time-resolved XAS measurements and from first-principles

NASA Astrophysics Data System (ADS)

Ogitsu, T.; Fernandez-Paãella, A.; Correa, A.; Engelhorn, K.; Barbrel, B.; Prendergast, D. G.; Pemmaraju, D.; Beckwith, M.; Kraus, D.; Hamel, S.; Cho, B. I.; Jin, L.; Wong, J.; Heinman, P.; Collins, G. W.; Falcone, R.; Ping, Y.

2016-10-01

We present a study of the electron-phonon coupling of warm dense iron upon femtosecond laser excitation by time-resolved x-ray absorption near edge spectroscopy (XANES). The dynamics of iron in electron-ion non-equilibrium conditions was studied using ab-initio density-functional-theory (DFT) simulations combined with the Two Temperature Model (TTM) where spatial inhomogeneity of electron (and ion) temperature(s) due to short ballistic electron transport length in iron was explicitly taken into consideration. Detailed comparison between our simulation results and experiments indicates that the ion temperature dependence on specific heat and on electron-phonon coupling also plays a relevant role in modeling the relaxation dynamics of electrons and ions. These results are the first experimental evidence of the suppression of the electron-phonon coupling factor of a transition metal at electron temperatures ranging 5000- 10000 K. This work was performed under DOE contract DE-AC52-07NA27344 with support from OFES Early Career program and LLNL LDRD program.

Implementation of Dipolar Resonant Excitation for Collision Induced Dissociation with Ion Mobility/Time-of-Flight MS

PubMed Central

Webb, Ian K.; Chen, Tsung-Chi; Danielson, William F.; Ibrahim, Yehia M.; Tang, Keqi; Anderson, Gordon A.; Smith, Richard D.

2014-01-01

An ion mobility/time-of-flight mass spectrometer (IMS/TOF MS) platform that allows for resonant excitation collision induced dissociation (CID) is presented. Highly efficient, mass-resolved fragmentation without additional excitation of product ions was accomplished and over-fragmentation common in beam-type CID experiments was alleviated. A quadrupole ion guide was modified to apply a dipolar AC signal across a pair of rods for resonant excitation. The method was characterized with singly protonated methionine enkephalin and triply protonated peptide angiotensin I, yielding maximum CID efficiencies of 44% and 84%, respectively. The Mathieu qx,y parameter was set at 0.707 for these experiments to maximize pseudopotential well depths and CID efficiencies. Resonant excitation CID was compared to beam-type CID for the peptide mixture. The ability to apply resonant waveforms in mobility-resolved windows is demonstrated with a peptide mixture yielding fragmentation over a range of mass-to-charge (m/z) ratios within a single IMS-MS analysis. PMID:24470195

The Influence of Drift Gas Composition on the Separation Mechanism in Traveling Wave Ion Mobility Spectrometry: Insight from Electrodynamic Simulations

PubMed Central

May, Jody C.; McLean, John A.

2013-01-01

The influence of three different drift gases (helium, nitrogen, and argon) on the separation mechanism in traveling wave ion mobility spectrometry is explored through ion trajectory simulations which include considerations for ion diffusion based on kinetic theory and the electrodynamic traveling wave potential. The model developed for this work is an accurate depiction of a second-generation commercial traveling wave instrument. Three ion systems (cocaine, MDMA, and amphetamine) whose reduced mobility values have previously been measured in different drift gases are represented in the simulation model. The simulation results presented here provide a fundamental understanding of the separation mechanism in traveling wave, which is characterized by three regions of ion motion: (1) ions surfing on a single wave, (2) ions exhibiting intermittent roll-over onto subsequent waves, and (3) ions experiencing a steady state roll-over which repeats every few wave cycles. These regions of ion motion are accessed through changes in the gas pressure, wave amplitude, and wave velocity. Resolving power values extracted from simulated arrival times suggest that momentum transfer in helium gas is generally insufficient to access regions (2) and (3) where ion mobility separations occur. Ion mobility separations by traveling wave are predicted to be effectual for both nitrogen and argon, with slightly lower resolving power values observed for argon as a result of band-broadening due to collisional scattering. For the simulation conditions studied here, the resolving power in traveling wave plateaus between regions (2) and (3), with further increases in wave velocity contributing only minor improvements in separations. PMID:23888124

The Influence of Drift Gas Composition on the Separation Mechanism in Traveling Wave Ion Mobility Spectrometry: Insight from Electrodynamic Simulations.

PubMed

May, Jody C; McLean, John A

2003-06-01

The influence of three different drift gases (helium, nitrogen, and argon) on the separation mechanism in traveling wave ion mobility spectrometry is explored through ion trajectory simulations which include considerations for ion diffusion based on kinetic theory and the electrodynamic traveling wave potential. The model developed for this work is an accurate depiction of a second-generation commercial traveling wave instrument. Three ion systems (cocaine, MDMA, and amphetamine) whose reduced mobility values have previously been measured in different drift gases are represented in the simulation model. The simulation results presented here provide a fundamental understanding of the separation mechanism in traveling wave, which is characterized by three regions of ion motion: (1) ions surfing on a single wave, (2) ions exhibiting intermittent roll-over onto subsequent waves, and (3) ions experiencing a steady state roll-over which repeats every few wave cycles. These regions of ion motion are accessed through changes in the gas pressure, wave amplitude, and wave velocity. Resolving power values extracted from simulated arrival times suggest that momentum transfer in helium gas is generally insufficient to access regions (2) and (3) where ion mobility separations occur. Ion mobility separations by traveling wave are predicted to be effectual for both nitrogen and argon, with slightly lower resolving power values observed for argon as a result of band-broadening due to collisional scattering. For the simulation conditions studied here, the resolving power in traveling wave plateaus between regions (2) and (3), with further increases in wave velocity contributing only minor improvements in separations.

Accelerated High-Resolution Differential Ion Mobility Separations Using Hydrogen

PubMed Central

Shvartsburg, Alexandre A.; Smith, Richard D.

2011-01-01

The resolving power of differential ion mobility spectrometry (FAIMS) was dramatically increased recently by carrier gases comprising up to 75% He or various vapors, enabling many new applications. However, the need for resolution of complex mixtures is virtually open-ended and many topical analyses demand yet finer separations. Also, the resolving power gains are often at the expense of speed, in particular making high-resolution FAIMS incompatible with online liquid-phase separations. Here, we report FAIMS employing hydrogen, specifically in mixtures with N2 containing up to 90% H2. Such compositions raise the mobilities of all ions and thus the resolving power beyond that previously feasible, while avoiding the electrical breakdown inevitable in He-rich mixtures. The increases in resolving power and ensuing peak resolution are especially significant at H2 fractions above ~50%. Higher resolution can be exchanged for acceleration of the analyses by up to ~4 times, at least. For more mobile species such as multiply-charged peptides, this exchange is presently forced by the constraints of existing FAIMS devices, but future designs optimized for H2 should consistently improve resolution for all analytes. PMID:22074292

High-performance multiple-reflection time-of-flight mass spectrometers for research with exotic nuclei and for analytical mass spectrometry

NASA Astrophysics Data System (ADS)

Plaß, Wolfgang R.; Dickel, Timo; Ayet San Andres, Samuel; Ebert, Jens; Greiner, Florian; Hornung, Christine; Jesch, Christian; Lang, Johannes; Lippert, Wayne; Majoros, Tamas; Short, Devin; Geissel, Hans; Haettner, Emma; Reiter, Moritz P.; Rink, Ann-Kathrin; Scheidenberger, Christoph; Yavor, Mikhail I.

2015-11-01

A class of multiple-reflection time-of-flight mass spectrometers (MR-TOF-MSs) has been developed for research with exotic nuclei at present and future accelerator facilities such as GSI and FAIR (Darmstadt), and TRIUMF (Vancouver). They can perform highly accurate mass measurements of exotic nuclei, serve as high-resolution, high-capacity mass separators and be employed as diagnostics devices to monitor the production, separation and manipulation of beams of exotic nuclei. In addition, a mobile high-resolution MR-TOF-MS has been developed for in situ applications in analytical mass spectrometry ranging from environmental research to medicine. Recently, the MR-TOF-MS for GSI and FAIR has been further developed. A novel RF quadrupole-based ion beam switchyard has been developed that allows merging and splitting of ion beams as well as transport of ions into different directions. It efficiently connects a test and reference ion source and an auxiliary detector to the system. Due to an increase in the kinetic energy of the ions in the time-of-flight analyzer of the MR-TOF-MS, a given mass resolving power is now achieved in less than half the time-of-flight. Conversely, depending on the time-of-flight, the mass resolving power has been increased by a factor of more than two.

Evaluating the accuracy of recent electron transport models at predicting Hall thruster plasma dynamics

NASA Astrophysics Data System (ADS)

Cappelli, Mark; Young, Christopher

2016-10-01

We present continued efforts towards introducing physical models for cross-magnetic field electron transport into Hall thruster discharge simulations. In particular, we seek to evaluate whether such models accurately capture ion dynamics, both averaged and resolved in time, through comparisons with measured ion velocity distributions which are now becoming available for several devices. Here, we describe a turbulent electron transport model that is integrated into 2-D hybrid fluid/PIC simulations of a 72 mm diameter laboratory thruster operating at 400 W. We also compare this model's predictions with one recently proposed by Lafluer et al.. Introducing these models into 2-D hybrid simulations is relatively straightforward and leverages the existing framework for solving the electron fluid equations. The models are tested for their ability to capture the time-averaged experimental discharge current and its fluctuations due to ionization instabilities. Model predictions are also more rigorously evaluated against recent laser-induced fluorescence measurements of time-resolved ion velocity distributions.

Heavy Ion Current Transients in SiGe HBTs

NASA Technical Reports Server (NTRS)

Pellish, Jonathan A.; Reed, Robert A.; Vizkelethy, Gyorgy; McMorrow, Dale; Ferlet-Cavrois, Veronique; Baggio, Jacques; Paillet, Philipe; Duhanel, Olivier; Phillips, Stanley D.; Sutton, Akil K.;

Time-resolved determination of Fe(II) ions using cysteine-bridged Mn-doped ZnS quantum dots as a phosphorimetric probe.

PubMed

Jing, Wenjie; Lu, Yuexiang; Wang, Feiyang; He, Liuying; Sun, Jingwei; Liu, Yueying

2018-05-12

A time-resolved phosphorescence (TRP) is applied to the highly sensitive determination of Fe(II) ions. The method is based on the use of a phosphorescent probe consisting of cysteine-bridged Mn-doped ZnS quantum dots (Mn/ZnS QDs). The presence of cysteine enhances the phosphorescence of the QDs and also increases the efficiency of quenching caused by Fe(II) ions. This results in strongly improved selectivity for Fe(II). The linear response is obtained in the concentration range of 50-1000 nM with a 19 nM detection limit. Phosphorescence is recorded at excitation/emission peaks of 301/602 nm. The interference of short-lived fluorescent and scattering background from the biological fluids is eliminated by using the TRP mode with a delay time of 200 μs. The determination of Fe(II) in human serum samples spiked at a 150 nM level gave a 92.4% recovery when using the TRP mode, but only 52.4% when using steady-state phosphorescence. This demonstrates that this probe along with TRP detection enables highly sensitive and accurate determination of Fe(II) in serum. Graphical abstract Schematic of a novel phosphorescent method for the detection of Fe 2+ ions based on cysteine-bridged Mn-doped ZnS quantum dots. The sensitivity of this assay greatly increases due to the addition of cysteine. Interferences by short-lived auto-fluorescence and the scattering light from the biological fluids is eliminated by using time-resolved phosphorescence mode.

Time-resolved ion imaging at free-electron lasers using TimepixCam.

PubMed

Fisher-Levine, Merlin; Boll, Rebecca; Ziaee, Farzaneh; Bomme, Cédric; Erk, Benjamin; Rompotis, Dimitrios; Marchenko, Tatiana; Nomerotski, Andrei; Rolles, Daniel

2018-03-01

The application of a novel fast optical-imaging camera, TimepixCam, to molecular photoionization experiments using the velocity-map imaging technique at a free-electron laser is described. TimepixCam is a 256 × 256 pixel CMOS camera that is able to detect and time-stamp ion hits with 20 ns timing resolution, thus making it possible to record ion momentum images for all fragment ions simultaneously and avoiding the need to gate the detector on a single fragment. This allows the recording of significantly more data within a given amount of beam time and is particularly useful for pump-probe experiments, where drifts, for example, in the timing and pulse energy of the free-electron laser, severely limit the comparability of pump-probe scans for different fragments taken consecutively. In principle, this also allows ion-ion covariance or coincidence techniques to be applied to determine angular correlations between fragments.

The 2nd order focusing sector field type TOF mass analyzer with an orthogonal ion acceleration for LC-IMS-MS.

PubMed

Poteshin, S S; Zarakovsky, A I

2017-03-15

Original orthogonal acceleration (OA) electrostatic sector time of flight (TOF) mass analyzer is proposed those allows the second order focusing of time of flight by initial ions position. Resolving power aberration limit exceeding 80,000 FW (full width mass peak) was shown to be obtainable for mass analyzer with the total length of flight L=133.2cm, the average ion energy 3700V and the ion energy spread of 2.5% on the entrance of sector field. Copyright © 2016 Elsevier B.V. All rights reserved.

Numerical studies of fast ion slowing down rates in cool magnetized plasma using LSP

NASA Astrophysics Data System (ADS)

Evans, Eugene S.; Kolmes, Elijah; Cohen, Samuel A.; Rognlien, Tom; Cohen, Bruce; Meier, Eric; Welch, Dale R.

2016-10-01

In MFE devices, rapid transport of fusion products from the core into the scrape-off layer (SOL) could perform the dual roles of energy and ash removal. The first-orbit trajectories of most fusion products from small field-reversed configuration (FRC) devices will traverse the SOL, allowing those particles to deposit their energy in the SOL and be exhausted along the open field lines. Thus, the fast ion slowing-down time should affect the energy balance of an FRC reactor and its neutron emissions. However, the dynamics of fast ion energy loss processes under the conditions expected in the FRC SOL (with ρe <λDe) are analytically complex, and not yet fully understood. We use LSP, a 3D electromagnetic PIC code, to examine the effects of SOL density and background B-field on the slowing-down time of fast ions in a cool plasma. As we use explicit algorithms, these simulations must spatially resolve both ρe and λDe, as well as temporally resolve both Ωe and ωpe, increasing computation time. Scaling studies of the fast ion charge (Z) and background plasma density are in good agreement with unmagnetized slowing down theory. Notably, Z-scaling represents a viable way to dramatically reduce the required CPU time for each simulation. This work was supported, in part, by DOE Contract Number DE-AC02-09CH11466.

Time-resolved delayed luminescence image microscopy using an europium ion chelate complex.

PubMed Central

Marriott, G.; Heidecker, M.; Diamandis, E. P.; Yan-Marriott, Y.

1994-01-01

Improvements and extended applications of time-resolved delayed luminescence imaging microscopy (TR-DLIM) in cell biology are described. The emission properties of europium ion complexed to a fluorescent chelating group capable of labeling proteins are exploited to provide high contrast images of biotin labeled ligands through detection of the delayed emission. The streptavidin-based macromolecular complex (SBMC) employs streptavidin cross-linked to thyroglobulin multiply labeled with the europium-fluorescent chelate. The fluorescent chelate is efficiently excited with 340-nm light, after which it sensitizes europium ion emission at 612 nm hundreds of microseconds later. The SBMC complex has a high quantum yield orders of magnitude higher than that of eosin, a commonly used delayed luminescent probe, and can be readily seen by the naked eye, even in specimens double-labeled with prompt fluorescent probes. Unlike triplet-state phosphorescent probes, sensitized europium ion emission is insensitive to photobleaching and quenching by molecular oxygen; these properties have been exploited to obtain delayed luminescence images of living cells in aerated medium thus complementing imaging studies using prompt fluorescent probes. Since TR-DLIM has the unique property of rejecting enormous signals that originate from scattered light, autofluorescence, and prompt fluorescence it has been possible to resolve double emission images of living amoeba cells containing an intensely stained lucifer yellow in pinocytosed vesicles and membrane surface-bound SBMC-labeled biotinylated concanavalin A. Images of fixed cells represented in terms of the time decay of the sensitized emission show the lifetime of the europium ion emission is sensitive to the environment in which it is found. Through the coupling of SBMC to streptavidin,a plethora of biotin-based tracer molecules are available for immunocytochemical studies. Images FIGURE 1 FIGURE 2 FIGURE 3 FIGURE 4 FIGURE 5 FIGURE 6 FIGURE 7 PMID:7811952

Flexible attosecond beamline for high harmonic spectroscopy and XUV/near-IR pump probe experiments requiring long acquisition times

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weber, S. J., E-mail: sebastien.weber@cea.fr; Manschwetus, B.; Billon, M.

2015-03-15

We describe the versatile features of the attosecond beamline recently installed at CEA-Saclay on the PLFA kHz laser. It combines a fine and very complete set of diagnostics enabling high harmonic spectroscopy (HHS) through the advanced characterization of the amplitude, phase, and polarization of the harmonic emission. It also allows a variety of photo-ionization experiments using magnetic bottle and COLTRIMS (COLd Target Recoil Ion Momentum Microscopy) electron spectrometers that may be used simultaneously, thanks to a two-foci configuration. Using both passive and active stabilization, special care was paid to the long term stability of the system to allow, using bothmore » experimental approaches, time resolved studies with attosecond precision, typically over several hours of acquisition times. As an illustration, applications to multi-orbital HHS and electron-ion coincidence time resolved spectroscopy are presented.« less

MASS SPECTROMETER

DOEpatents

White, F.A.

1960-08-23

A mass spectrometer is designed with a first adjustable magnetic field for resolving an ion beam into beams of selected masses, a second adjustable magnetic field for further resolving the ion beam from the first field into beams of selected masses, a thin foil disposed in the path of the beam between the first and second magnets to dissociate molecular ions incident thereon, an electrostatic field for further resolving the ion beam from the second field into beams of selected masses, and a detector disposed adjacent to the electrostatic field to receive the ion beam.

TimepixCam: a fast optical imager with time-stamping

NASA Astrophysics Data System (ADS)

Fisher-Levine, M.; Nomerotski, A.

2016-03-01

We describe a novel fast optical imager, TimepixCam, based on an optimized silicon pixel sensor with a thin entrance window, read out by a Timepix ASIC. TimepixCam is able to record and time-stamp light flashes in excess of 1,000 photons with high quantum efficiency in the 400-1000nm wavelength range with 20ns timing resolution, corresponding to an effective rate of 50 Megaframes per second. The camera was used for imaging ions impinging on a microchannel plate followed by a phosphor screen. Possible applications include spatial and velocity map imaging of ions in time-of-flight mass spectroscopy; coincidence imaging of ions and electrons, and other time-resolved types of imaging spectroscopy.

Accurate Drift Time Determination by Traveling Wave Ion Mobility Spectrometry: The Concept of the Diffusion Calibration.

PubMed

Kune, Christopher; Far, Johann; De Pauw, Edwin

2016-12-06

Ion mobility spectrometry (IMS) is a gas phase separation technique, which relies on differences in collision cross section (CCS) of ions. Ionic clouds of unresolved conformers overlap if the CCS difference is below the instrumental resolution expressed as CCS/ΔCCS. The experimental arrival time distribution (ATD) peak is then a superimposition of the various contributions weighted by their relative intensities. This paper introduces a strategy for accurate drift time determination using traveling wave ion mobility spectrometry (TWIMS) of poorly resolved or unresolved conformers. This method implements through a calibration procedure the link between the peak full width at half-maximum (fwhm) and the drift time of model compounds for wide range of settings for wave heights and velocities. We modified a Gaussian equation, which achieves the deconvolution of ATD peaks where the fwhm is fixed according to our calibration procedure. The new fitting Gaussian equation only depends on two parameters: The apex of the peak (A) and the mean drift time value (μ). The standard deviation parameter (correlated to fwhm) becomes a function of the drift time. This correlation function between μ and fwhm is obtained using the TWIMS calibration procedure which determines the maximum instrumental ion beam diffusion under limited and controlled space charge effect using ionic compounds which are detected as single conformers in the gas phase. This deconvolution process has been used to highlight the presence of poorly resolved conformers of crown ether complexes and peptides leading to more accurate CCS determinations in better agreement with quantum chemistry predictions.

Ultrafast Physics Behind the Nonradiative Relaxation Process of Chromium Ions in Forsterite Crystals.

NASA Astrophysics Data System (ADS)

Demos, Stavros Gregorios

The nonradiative relaxation following photoexcitation has been studied in Cr^{4+} -doped forsterite (Mg_2SiO _4) using picosecond laser excitation and ultrasensitive photon counting detection. The experimental techniques utilized were time resolved antiStokes Raman scattering and up-converted hot and ordinary luminescence. The up-converted hot luminescence technique allowed the investigation of the upper state nonradiative relaxation of the excited state manifold of Cr^{4+ }-doped forsterite. The excitation involves the absorption of two photons per photoexcited ion in a two-step absorption. Discrete peaks are observed in the hot up-converted luminescence spectrum and are attributed to the population of nonequilibrium vibronic levels during the deexcitation of the ions by phonon emission. This work reveals that the phonon modes participating in the initial steps of the nonradiative relaxation of the photoexcited ions have energies 218 +/- 20, 325 +/- 20, 365 +/- 20 and 513 +/- 12 cm^ {-1}. The shape of the luminescence spectral envelope suggests two electronic bottlenecks at ~2.1 and ~2.45 eV associated with slower rates of vibrational relaxation at different parts of the excited state manifold. Time resolved measurements indicated that the average time for phonon emission is of the order of hundreds of fs. Information on the nonequilibrium phonon dynamics of the 225, 335 and 370 cm^{-1} modes of forsterite has been obtained using time resolved Raman scattering. Laser pulses of 450 fs in duration and 590 nm in wavelength were used to excite the Cr ions 2.1 eV above the ground state. The probe pulses (obtained from the same laser) are monitoring the nonequilibrium phonon population through the intensity of the antiStokes Raman lines at various pump-probe delay times. Experiments were performed at room and liquid nitrogen temperatures. The observed nonequilibrium phonon populations are associated with the overall complex nonradiative decay following the excitation of the impurity Cr^{4+} ions. Using rate equations to describe the electron -lattice system, the nonradiative relaxation time and the phonon lifetimes were estimated by fitting to the experimental data. The nonradiative relaxation time is estimated to be in the order of few ps while the phonon lifetimes are of the order of 10 ps. Best fit suggests the presence of an electronic bottleneck immediately after photoexcitation with an estimated lifetime of 3 ps at room temperature.

Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy

DOE PAGES

Hassan, Asra; Zhang, Xiaoyi; Liu, Xiaohan; ...

2017-08-28

Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report the results of time-resolved X-ray absorption studies on copper-doped cadmium sulfide nanoparticles that provide an explicit description of the electronic dynamics of the dopants. The interaction of a dopant ion and an excess charge carrier is unambiguously observed via monitoring the oxidation state. The experimental data combined with DFT calculations demonstrate that dopant bonding to the host matrix is modulated by its interaction with charge carriers. Additionally, the transient photoluminescence and the kinetics of dopantmore » oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.« less

Charge Carriers Modulate the Bonding of Semiconductor Nanoparticle Dopants As Revealed by Time-Resolved X-ray Spectroscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hassan, Asra; Zhang, Xiaoyi; Liu, Xiaohan

Understanding the electronic structure of doped semiconductors is essential to realize advancements in electronics and in the rational design of nanoscale devices. Here, we report the results of time-resolved X-ray absorption studies on copper-doped cadmium sulfide nanoparticles that provide an explicit description of the electronic dynamics of the dopants. The interaction of a dopant ion and an excess charge carrier is unambiguously observed via monitoring the oxidation state. The experimental data combined with DFT calculations demonstrate that dopant bonding to the host matrix is modulated by its interaction with charge carriers. Additionally, the transient photoluminescence and the kinetics of dopantmore » oxidation reveal the presence of two types of surface-bound ions that create mid-gap states.« less

High dynamic range bio-molecular ion microscopy with the Timepix detector.

PubMed

Jungmann, Julia H; MacAleese, Luke; Visser, Jan; Vrakking, Marc J J; Heeren, Ron M A

2011-10-15

Highly parallel, active pixel detectors enable novel detection capabilities for large biomolecules in time-of-flight (TOF) based mass spectrometry imaging (MSI). In this work, a 512 × 512 pixel, bare Timepix assembly combined with chevron microchannel plates (MCP) captures time-resolved images of several m/z species in a single measurement. Mass-resolved ion images from Timepix measurements of peptide and protein standards demonstrate the capability to return both mass-spectral and localization information of biologically relevant analytes from matrix-assisted laser desorption ionization (MALDI) on a commercial ion microscope. The use of a MCP-Timepix assembly delivers an increased dynamic range of several orders of magnitude. The Timepix returns defined mass spectra already at subsaturation MCP gains, which prolongs the MCP lifetime and allows the gain to be optimized for image quality. The Timepix peak resolution is only limited by the resolution of the in-pixel measurement clock. Oligomers of the protein ubiquitin were measured up to 78 kDa. © 2011 American Chemical Society

Space-resolved measurements of neutrons and ions emitted by a plasma focus

NASA Astrophysics Data System (ADS)

Jaeger, U.

1980-05-01

Space-resolved measurements of neutrons and of accelerated charged particles emitted by a plasma focus device are presented. The neutron source was measured with one and two dimensional paraffin collimators. The spatial resolution is 5 mn along the axis and the radius, with a time resolution of 10 ns. In order to make quantitative statements about the neutron yield, neutron scattering, absorption, and nuclear reactions were taken into account. Part of the neutron measurement was carried out together with time and space resolved measurements of the electron density to study possible correlations between n sub e and y sub n.

MAVEN SupraThermal and Thermal Ion Compostion (STATIC) Instrument

NASA Astrophysics Data System (ADS)

McFadden, J. P.; Kortmann, O.; Curtis, D.; Dalton, G.; Johnson, G.; Abiad, R.; Sterling, R.; Hatch, K.; Berg, P.; Tiu, C.; Gordon, D.; Heavner, S.; Robinson, M.; Marckwordt, M.; Lin, R.; Jakosky, B.

2015-12-01

The MAVEN SupraThermal And Thermal Ion Compostion (STATIC) instrument is designed to measure the ion composition and distribution function of the cold Martian ionosphere, the heated suprathermal tail of this plasma in the upper ionosphere, and the pickup ions accelerated by solar wind electric fields. STATIC operates over an energy range of 0.1 eV up to 30 keV, with a base time resolution of 4 seconds. The instrument consists of a toroidal "top hat" electrostatic analyzer with a 360° × 90° field-of-view, combined with a time-of-flight (TOF) velocity analyzer with 22.5° resolution in the detection plane. The TOF combines a -15 kV acceleration voltage with ultra-thin carbon foils to resolve H+, He^{++}, He+, O+, O2+, and CO2+ ions. Secondary electrons from carbon foils are detected by microchannel plate detectors and binned into a variety of data products with varying energy, mass, angle, and time resolution. To prevent detector saturation when measuring cold ram ions at periapsis (˜10^{1 1} eV/cm2 s sr eV), while maintaining adequate sensitivity to resolve tenuous pickup ions at apoapsis (˜103 eV/cm2 s sr eV), the sensor includes both mechanical and electrostatic attenuators that increase the dynamic range by a factor of 103. This paper describes the instrument hardware, including several innovative improvements over previous TOF sensors, the ground calibrations of the sensor, the data products generated by the experiment, and some early measurements during cruise phase to Mars.

Watching electrons tunnel

NASA Astrophysics Data System (ADS)

Moser, Simon

2008-03-01

To get insight to time resolved inner atomic or molecular processes, laser pulses of few femtoseconds or even attoseconds are needed. These short light pulse techniques ask for broad frequency spectra, control of dispersion and control of phase. Hence, linear optics fails and nonlinear optics in high electromagnetic fields is needed to satisfy the amount of control that is needed. One recent application of attosecond laser pulses is time resolved visualization of tunnel ionization in atoms applied to high electromagnetic fields. Here, Ne atom electrons are excited by an extreme ultraviolet attosecond laser pulse. After a while, a few cycles nearly infrared femtosecond laser pulse is applied to the atom causing tunnel ionization. The ion yield distribution can be measured as function of the delay time between excitation and ionization and so deliver insight to the time resolved mechanisms.

Exploding Pusher Targets for Electron-Ion Coupling Measurements

NASA Astrophysics Data System (ADS)

Whitley, Heather D.; Pino, Jesse; Schneider, Marilyn; Shepherd, Ronnie; Benedict, Lorin; Bauer, Joseph; Graziani, Frank; Garbett, Warren

2015-11-01

Over the past several years, we have conducted theoretical investigations of electron-ion coupling and electronic transport in plasmas. In the regime of weakly coupled plasmas, we have identified models that we believe describe the physics well, but experimental data is still needed to validate the models. We are currently designing spectroscopic experiments to study electron-ion equilibration and/or electron heat transport using exploding pusher (XP) targets for experiments at the National Ignition Facility. Two platforms are being investigated: an indirect drive XP (IDXP) with a plastic ablator and a polar-direct drive XP (PDXP) with a glass ablator. The fill gas for both designs is D2. We propose to use a higher-Z dopant, such as Ar, as a spectroscopic tracer for time-resolved electron and ion temperature measurements. We perform 1D simulations using the ARES hydrodynamic code, in order to produce the time-resolved plasma conditions, which are then post-processed with CRETIN to assess the feasibility of a spectroscopic measurement. We examine target performance with respect to variations in gas fill pressure, ablator thickness, atom fraction of the Ar dopant, and drive energy, and assess the sensitivity of the predicted spectra to variations in the models for electron-ion equilibration and thermal conductivity. Prepared by LLNL under Contract DE-AC52-07NA27344. LLNL-ABS-675219.

Ultra-high-mass mass spectrometry with charge discrimination using cryogenic detectors

DOEpatents

Frank, Matthias; Mears, Carl A.; Labov, Simon E.; Benner, W. Henry

1999-01-01

An ultra-high-mass time-of-flight mass spectrometer using a cryogenic particle detector as an ion detector with charge discriminating capabilities. Cryogenic detectors have the potential for significantly improving the performance and sensitivity of time-of-flight mass spectrometers, and compared to ion multipliers they exhibit superior sensitivity for high-mass, slow-moving macromolecular ions and can be used as "stop" detectors in time-of-flight applications. In addition, their energy resolving capability can be used to measure the charge state of the ions. Charge discrimination is very valuable in all time-of-flight mass spectrometers. Using a cryogenically-cooled Nb-Al.sub.2 O.sub.3 -Nb superconductor-insulator-superconductor (SIS) tunnel junction (STJ) detector operating at 1.3 K as an ion detector in a time-of-flight mass spectrometer for large biomolecules it was found that the STJ detector has charge discrimination capabilities. Since the cryogenic STJ detector responds to ion energy and does not rely on secondary electron production, as in the conventionally used microchannel plate (MCP) detectors, the cryogenic detector therefore detects large molecular ions with a velocity-independent efficiency approaching 100%.

Lithium ion beam divergence on SABRE extraction ion diode experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hanson, D.L.; Cuneo, M.E.; Johnson, D.J.

Intense lithium beams are of particular interest for light ion inertial confinement fusion applications because lithium ions can be accelerated at high voltage in a single charge state (Li{sup +}) with a high mass-to-charge ratio and appropriate range for efficient focusing and heating of a hohlraum ICF target. Scaling to ion power densities adequate to drive high gain pellet implosions (600 TW at 30 MeV) will require a large number of beams transported, temporally bunched, and focused onto a target, with the necessary target standoff to ensure survival of the driver modules. For efficient long distance transport and focusing tomore » a small pellet, lithium beam divergence must be reduced to about 12 mrad or less (depending on the transport scheme). To support the eventual development of a light ion driver module for ICF applications, the authors are currently working to improve the composition, uniformity, and divergence of lithium ion beams produced by both passive LiF and active laser-generated lithium ion sources on extraction applied-B ion diodes on the SABRE accelerator (1 TW, 5 MV, 250 kA). While lithium beam divergence accounting and control are an essential goal of these experiments, divergence measurements for lithium beams present some unique problems not encountered to the same degree in divergence measurements on proton sources. To avoid these difficulties, the authors have developed a large aperture ion imaging diagnostic for time-resolved lithium divergence measurements. The authors will report on the operation of this lithium beam divergence diagnostic and on results of time-resolved divergence measurements in progress for passive LiF ion sources and laser-produced active lithium sources operated in diode configurations designed to control divergence growth. Comparisons will also be made with time-integrated divergence results obtained with small entrance aperture ultracompact pinhole cameras.« less

Measurement of electron-ion relaxation in warm dense copper

DOE PAGES

Cho, B. I.; Ogitsu, T.; Engelhorn, K.; ...

2016-01-06

Experimental investigation of electron-ion coupling and electron heat capacity of copper in warm and dense states are presented. From time-resolved x-ray absorption spectroscopy, the temporal evolution of electron temperature is obtained for non-equilibrium warm dense copper heated by an intense femtosecond laser pulse. Electron heat capacity and electron-ion coupling are inferred from the initial electron temperature and its decrease over 10 ps. As a result, data are compared with various theoretical models.

Energetics and Dynamics of Dissociation of Deprotonated Peptides: Fragmentation of Angiotensin Analogs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laskin, Julia; Yang, Zhibo

2011-12-01

We present a first study of the energetics and dynamics of dissociation of deprotonated peptides using time- and collision-energy resolved surface-induced dissociation (SID) experiments. SID of four model peptides: RVYIHPF, HVYIHPF, DRVYIHPF, and DHVYIHPF was studied using a specially designed Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS) configured for studying ion-surface collisions. Energy and entropy effects for the overall decomposition of the precursor ion were deduced by modeling the time- and collision energy-resolved survival curves using an RRKM based approach developed in our laboratory. The results were compared to the energetics and dynamics of dissociation of the correspondingmore » protonated species. We demonstrate that acidic peptides are less stable in the negative mode because of the low threshold associated with the kinetically hindered loss of H2O from [M-H]- ions. Comparison between the two basic peptides indicates that the lower stability of the [M-H]- ion of RVYIHPF as compared to HVYIHPF towards fragmentation is attributed to the differences in fragmentation mechanisms. Specifically, threshold energy associated with losses of NH3 and NHCNH from RVYIHPF is lower than the barrier for backbone fragmentation that dominates gas-phase decomposition of HVYIHPF. The results provide a first quantitative comparison between the energetics and dynamics of dissociation of [M+H]+ and [M-H]- ions of acidic and basic peptides.« less

Spatial and Temporal Extent of Ion Spectral Structures at the Inner Edge of the Plasma Sheet

NASA Astrophysics Data System (ADS)

Ferradas, C.; Reeves, G. D.; Zhang, J.; Spence, H. E.; Kistler, L. M.; Larsen, B.; Skoug, R. M.; Funsten, H. O.

2017-12-01

Several ion spectral structures are observed near the inner edge of the plasma sheet and constitute the signatures of ion drift and loss in the highly dynamic environment of the inner magnetosphere. Their study helps us understand ion access and losses in this region. Several studies have found that these structures vary with geomagnetic activity, local time, and ion species, but their spatial and temporal extent remain undetermined. We use data from the Helium, Oxygen, Proton, and Electron (HOPE) mass spectrometers onboard the Van Allen Probes to analyze the spectral structures in the energy range of 1- 50 keV. HOPE measurements on both Van Allen Probes spacecraft enable us to resolve the extent of these ion structures in space and time. As the structures respond to changes in the convection electric field on a variety of time scales, the lapping of the two spacecraft on time scales of minutes to hours helps determine their spatial and temporal evolution.

Time-resolved pulsed hydrogen/deuterium exchange mass spectrometry probes gaseous proteins structural kinetics.

PubMed

Rajabi, Khadijeh

2015-01-01

A pulsed hydrogen/deuterium exchange (HDX) method has been developed for rapid monitoring of the exchange kinetics of protein ions with D2O a few milliseconds after electrospray ionization (ESI). The stepwise gradual evolution of HDX of multiply charged protein ions was monitored using the pulsed HDX mass spectrometry technique. Upon introducing a very short pulse of D2O (in the μs to ms time scale) into the linear ion trap (LIT) of a time-of-flight (TOF) mass spectrometer, bimodal distributions were detected for the ions of cytochrome c and ubiquitin. Mechanistic details of HDX reactions for ubiquitin and cytochrome c in the gas phase were uncovered and the structural transitions were followed by analyzing the kinetics of HDX.

Characterization of compounds by time-of-flight measurement utilizing random fast ions

DOEpatents

Conzemius, R.J.

1989-04-04

An apparatus is described for characterizing the mass of sample and daughter particles, comprising a source for providing sample ions; a fragmentation region wherein a fraction of the sample ions may fragment to produce daughter ion particles; an electrostatic field region held at a voltage level sufficient to effect ion-neutral separation and ion-ion separation of fragments from the same sample ion and to separate ions of different kinetic energy; a detector system for measuring the relative arrival times of particles; and processing means operatively connected to the detector system to receive and store the relative arrival times and operable to compare the arrival times with times detected at the detector when the electrostatic field region is held at a different voltage level and to thereafter characterize the particles. Sample and daughter particles are characterized with respect to mass and other characteristics by detecting at a particle detector the relative time of arrival for fragments of a sample ion at two different electrostatic voltage levels. The two sets of particle arrival times are used in conjunction with the known altered voltage levels to mathematically characterize the sample and daughter fragments. In an alternative embodiment the present invention may be used as a detector for a conventional mass spectrometer. In this embodiment, conventional mass spectrometry analysis is enhanced due to further mass resolving of the detected ions. 8 figs.

Characterization of compounds by time-of-flight measurement utilizing random fast ions

DOEpatents

Conzemius, Robert J.

1989-01-01

An apparatus for characterizing the mass of sample and daughter particles, comprising a source for providing sample ions; a fragmentation region wherein a fraction of the sample ions may fragment to produce daughter ion particles; an electrostatic field region held at a voltage level sufficient to effect ion-neutral separation and ion-ion separation of fragments from the same sample ion and to separate ions of different kinetic energy; a detector system for measuring the relative arrival times of particles; and processing means operatively connected to the detector system to receive and store the relative arrival times and operable to compare the arrival times with times detected at the detector when the electrostatic field region is held at a different voltage level and to thereafter characterize the particles. Sample and daughter particles are characterized with respect to mass and other characteristics by detecting at a particle detector the relative time of arrival for fragments of a sample ion at two different electrostatic voltage levels. The two sets of particle arrival times are used in conjunction with the known altered voltage levels to mathematically characterize the sample and daughter fragments. In an alternative embodiment the present invention may be used as a detector for a conventional mass spectrometer. In this embodiment, conventional mass spectrometry analysis is enhanced due to further mass resolving of the detected ions.

High-Field Asymmetric-Waveform Ion Mobility Spectrometry and Electron Detachment Dissociation of Isobaric Mixtures of Glycosaminoglycans

NASA Astrophysics Data System (ADS)

Kailemia, Muchena J.; Park, Melvin; Kaplan, Desmond A.; Venot, Andre; Boons, Geert-Jan; Li, Lingyun; Linhardt, Robert J.; Amster, I. Jonathan

2014-02-01

High-field asymmetric waveform ion mobility spectrometry (FAIMS) is shown to be capable of resolving isomeric and isobaric glycosaminoglycan negative ions and to have great utility for the analysis of this class of molecules when combined with Fourier transform ion cyclotron resonance mass spectrometry (FTICR-MS) and tandem mass spectrometry. Electron detachment dissociation (EDD) and other ion activation methods for tandem mass spectrometry can be used to determine the sites of labile sulfate modifications and for assigning the stereochemistry of hexuronic acid residues of glycosaminoglycans (GAGs). However, mixtures with overlapping mass-to-charge values present a challenge, as their precursor species cannot be resolved by a mass analyzer prior to ion activation. FAIMS is shown to resolve two types of mass-to-charge overlaps. A mixture of chondroitin sulfate A (CSA) oligomers with 4-10 saccharides units produces ions of a single mass-to-charge by electrospray ionization, as the charge state increases in direct proportion to the degree of polymerization for these sulfated carbohydrates. FAIMS is shown to resolve the overlapping charge. A more challenging type of mass-to-charge overlap occurs for mixtures of diastereomers. FAIMS is shown to separate two sets of epimeric GAG tetramers. For the epimer pairs, the complexity of the separation is reduced when the reducing end is alkylated, suggesting that anomers are also resolved by FAIMS. The resolved components were activated by EDD and the fragment ions were analyzed by FTICR-MS. The resulting tandem mass spectra were able to distinguish the two epimers from each other.

A Survey of the High Order Multiplicity of Nearby Solar-Type Binary Stars with Robo-AO

DTIC Science & Technology

2015-01-20

auxiliary images are not used for astrometry or photometry , but are helpful for verifying compan- ion detection and for resolving the 180◦ ambiguity of...pair Ba,Bb was resolved by Robo-AO three times at 0.′′16 with Δi = 0.87m, Δr = 0.97m, and Δz = 0.52m. This corresponds to a mass for Bb of ∼0.6M. We...known quintuple system. The component E (STF 2032AE, E=HIP 79551=GJ 615.2C) is resolved here at 0.′′4 (but not for the first time : Ea,Eb=YSC 152

Surface-induced dissociation: a unique tool for studying energetics and kinetics of the gas-phase fragmentation of large ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laskin, Julia

2015-01-01

Surface-induced dissociation (SID) is valuable tool for investigating activation and dissociation of large ions in tandem mass spectrometry. This account summarizes key findings from studies of the energetics and mechanisms of complex ion dissociation, in which SID experiments were combined with Rice-Ramsperger-Kassel-Marcus (RRKM) modeling of the experimental data. These studies used time- and collision-energy-resolved SID experiments and SID combined with resonant ejection of selected fragment ions on a specially designed Fourier transform ion cyclotron resonance mass spectrometer (FT-ICR MS). Fast ion activation by collision with a surface combined with the long and variable timescale of a FT-ICR MS is perfectlymore » suited for studying the energetics and dynamics of complex ion dissociation in the gas phase. Modeling of time- and collision-energy-resolved SID enables accurate determination of energy and entropy effects in the dissociation process. It has been demonstrated that entropy effects play an important role in determining the dissociation rates of both covalent and non-covalent bonds in large gaseous ions. SID studies have provided important insights on the competition between charge-directed and charge-remote fragmentation in even-electron peptide ions and the role of charge and radical site on the energetics of the dissociation of odd-electron peptide ions. Furthermore, this work examined factors that affect the strength of non-covalent binding, as well as the competition between covalent and non-covalent bond cleavages and between proton and electron transfer in model systems. Finally, SID studies have been used to understand the factors affecting nucleation and growth of clusters in solution and the gas phase.« less

Time-resolved ion imaging at free-electron lasers using TimepixCam

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fisher-Levine, Merlin; Boll, Rebecca; Ziaee, Farzaneh

In this paper, the application of a novel fast optical-imaging camera, TimepixCam, to molecular photoionization experiments using the velocity-map imaging technique at a free-electron laser is described. TimepixCam is a 256 × 256 pixel CMOS camera that is able to detect and time-stamp ion hits with 20 ns timing resolution, thus making it possible to record ion momentum images for all fragment ions simultaneously and avoiding the need to gate the detector on a single fragment. This allows the recording of significantly more data within a given amount of beam time and is particularly useful for pump–probe experiments, where drifts,more » for example, in the timing and pulse energy of the free-electron laser, severely limit the comparability of pump–probe scans for different fragments taken consecutively. Finally, in principle, this also allows ion–ion covariance or coincidence techniques to be applied to determine angular correlations between fragments.« less

Time-resolved ion imaging at free-electron lasers using TimepixCam

DOE PAGES

Fisher-Levine, Merlin; Boll, Rebecca; Ziaee, Farzaneh; ...

2018-02-20

In this paper, the application of a novel fast optical-imaging camera, TimepixCam, to molecular photoionization experiments using the velocity-map imaging technique at a free-electron laser is described. TimepixCam is a 256 × 256 pixel CMOS camera that is able to detect and time-stamp ion hits with 20 ns timing resolution, thus making it possible to record ion momentum images for all fragment ions simultaneously and avoiding the need to gate the detector on a single fragment. This allows the recording of significantly more data within a given amount of beam time and is particularly useful for pump–probe experiments, where drifts,more » for example, in the timing and pulse energy of the free-electron laser, severely limit the comparability of pump–probe scans for different fragments taken consecutively. Finally, in principle, this also allows ion–ion covariance or coincidence techniques to be applied to determine angular correlations between fragments.« less

Travelling-wave ion mobility and negative ion fragmentation of high mannose N-glycans

PubMed Central

Harvey, David J.; Scarff, Charlotte A.; Edgeworth, Matthew; Struwe, Weston B.; Pagel, Kevin; Thalassinos, Konstantinos; Crispin, Max; Scrivens, Jim

2016-01-01

The isomeric structure of high-mannose N-glycans can significantly impact biological recognition events. Here, the utility of travelling-wave ion mobility-mass spectrometry (TW IM-MS)for isomer separation of high-mannose N-glycans is investigated. Negative ion fragmentation using collision-induced dissociation (CID) gave more informative spectra than positive ion spectra with mass-different fragment ions characterizing many of the isomers. Isomer separation by ion mobility in both ionization modes was generally limited, with the arrival time distributions (ATD) often showing little sign of isomers. However, isomers could be partially resolved by plotting extracted fragment ATDs of the diagnostic fragment ions from the negative ion spectra and the fragmentation spectra of the isomers could be extracted by using ions from limited areas of the ATD peak. In some cases, asymmetric ATDs were observed but no isomers could be detected by fragmentation. In these cases, it was assumed that conformers were being separated. Collision cross sections (CCSs) of the isomers in positive and negative fragmentation mode were estimated from TW IM-MS data using dextran glycans as calibrant. More complete CCS data were achieved in negative ion mode by utilizing the diagnostic fragment ions. Examples of isomer separations are shown for N-glycans released from the well-characterized glycoproteins chicken ovalbumin, porcine thyroglobulin and gp120 from the human immunodeficiency virus. In addition to the cross sectional data, details of the negative ion collision-induced dissociation (CID) spectra of all resolved isomers are discussed. PMID:26956389

Imaging thermal plasma mass and velocity analyzer

NASA Astrophysics Data System (ADS)

Yau, Andrew W.; Howarth, Andrew

2016-07-01

We present the design and principle of operation of the imaging ion mass and velocity analyzer on the Enhanced Polar Outflow Probe (e-POP), which measures low-energy (1-90 eV/e) ion mass composition (1-40 AMU/e) and velocity distributions using a hemispherical electrostatic analyzer (HEA), a time-of-flight (TOF) gate, and a pair of toroidal electrostatic deflectors (TED). The HEA and TOF gate measure the energy-per-charge and azimuth of each detected ion and the ion transit time inside the analyzer, respectively, providing the 2-D velocity distribution of each major ionospheric ion species and resolving the minor ion species under favorable conditions. The TED are in front of the TOF gate and optionally sample ions at different elevation angles up to ±60°, for measurement of 3-D velocity distribution. We present examples of observation data to illustrate the measurement capability of the analyzer, and show the occurrence of enhanced densities of heavy "minor" O++, N+, and molecular ions and intermittent, high-velocity (a few km/s) upward and downward flowing H+ ions in localized regions of the quiet time topside high-latitude ionosphere.

Millimeter-Wave Time Resolved Studies of the Formation and Decay of CO^+

NASA Astrophysics Data System (ADS)

Oesterling, Lee; Herbst, Eric; de Lucia, Frank

1998-04-01

Since the rate constants for ion-molecule interactions are typically much larger than neutral-neutral interactions, understanding ion-molecule interactions is essential to interpreting radio astronomical spectra from interstellar clouds and modeling the processes which lead to the formation of stars in these regions. We have developed a cell which allows us to study ion-molecule interactions in gases at low temperatures and pressures by using an electron gun technique to create ions. By centering our millimeter-wave source on a rotational resonance and gating the electron beam on and off, we are able to study the time-dependent rotational state distribution of the ion during its formation and decay, and so learn about excitation and relaxation processes as functions of temperature, pressure, electron beam energy, and electron beam current.

Femtosecond-laser-induced nonadiabatic alignment in photoexcited pyrimidine

NASA Astrophysics Data System (ADS)

Li, Shuai; Ling, Fengzi; Wang, Yanmei; Long, Jinyou; Deng, Xulan; Jin, Bing; Zhang, Bing

2017-09-01

The rotational wave-packet dynamics in electronically excited pyrimidine induced by a femtosecond laser pulse at 321.5 nm has been studied by time-resolved mass spectroscopy and photoelectron velocity-map imaging. The rotational revival features at 81.3 ps, which are the direct manifestation of field-free nonadiabatic alignment, are clearly observed in both the time-dependent ion yields and photoelectron angular distributions. In particular, the out-of-phase recurrences in the parent-ion and fragment-ions transients indicate the different directions of the ionization transition-dipole moments for the generation of the parent ion and fragment ions. By tuning the polarization of the probe light parallel or perpendicular to that of the pump light, we demonstrate the potential application of nonadiabatic alignment to manipulate the branching ratio of photoionization products.

Control of femtosecond laser driven retro-Diels-Alder-like reaction of dicyclopentadiene

PubMed Central

Das, Dipak Kumar; Goswami, Tapas; Goswami, Debabrata

2013-01-01

Using femtosecond time resolved degenerate pump-probe mass spectrometry coupled with simple linearly chirped frequency modulated pulse, we elucidate that the dynamics of retro-Diels-Alder-like reaction of diclopentadiene (DCPD) to cyclopentadiene (CPD) in supersonic molecular beam occurs in ultrafast time scale. Negatively chirped pulse enhances the ion yield of CPD, as compared to positively chirped pulse. This indicates that by changing the frequency (chirp) of the laser pulse we can control the ion yield of a chemical reaction. PMID:23814449

Optical Orientation of Mn2+ Ions in GaAs in Weak Longitudinal Magnetic Fields

NASA Astrophysics Data System (ADS)

Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Sapega, V. F.; Yakovlev, D. R.; Bayer, M.

2011-04-01

We report on optical orientation of Mn2+ ions in bulk GaAs subject to weak longitudinal magnetic fields (B≤100mT). A manganese spin polarization of 25% is directly evaluated by using spin-flip Raman scattering. The dynamical Mn2+ polarization occurs due to the s-d exchange interaction with optically oriented conduction band electrons. Time-resolved photoluminescence reveals a nontrivial electron spin dynamics, where the oriented Mn2+ ions tend to stabilize the electron spins.

Optical orientation of Mn2+ ions in GaAs in weak longitudinal magnetic fields.

PubMed

Akimov, I A; Dzhioev, R I; Korenev, V L; Kusrayev, Yu G; Sapega, V F; Yakovlev, D R; Bayer, M

2011-04-08

We report on optical orientation of Mn2+ ions in bulk GaAs subject to weak longitudinal magnetic fields (B≤100  mT). A manganese spin polarization of 25% is directly evaluated by using spin-flip Raman scattering. The dynamical Mn2+ polarization occurs due to the s-d exchange interaction with optically oriented conduction band electrons. Time-resolved photoluminescence reveals a nontrivial electron spin dynamics, where the oriented Mn2+ ions tend to stabilize the electron spins.

BRIEF COMMUNICATION: Fast-ion redistribution due to sawtooth crash in the TEXTOR tokamak measured by collective Thomson scattering

NASA Astrophysics Data System (ADS)

Nielsen, S. K.; Bindslev, H.; Salewski, M.; Bürger, A.; Delabie, E.; Furtula, V.; Kantor, M.; Korsholm, S. B.; Leipold, F.; Meo, F.; Michelsen, P. K.; Moseev, D.; Oosterbeek, J. W.; Stejner, M.; Westerhof, E.; Woskov, P.; TEXTOR Team

2010-09-01

Here we present collective Thomson scattering measurements of 1D fast-ion velocity distribution functions in neutral beam heated TEXTOR plasmas with sawtooth oscillations. Up to 50% of the fast ions in the centre are redistributed as a consequence of a sawtooth crash. We resolve various directions to the magnetic field. The fast-ion distribution is found to be anisotropic as expected. For a resolved angle of 39° to the magnetic field we find a drop in the fast-ion distribution of 20-40%. For a resolved angle of 83° to the magnetic field the drop is no larger than 20%.

Time-dependent nonlinear Jaynes-Cummings dynamics of a trapped ion

NASA Astrophysics Data System (ADS)

Krumm, F.; Vogel, W.

2018-04-01

In quantum interaction problems with explicitly time-dependent interaction Hamiltonians, the time ordering plays a crucial role for describing the quantum evolution of the system under consideration. In such complex scenarios, exact solutions of the dynamics are rarely available. Here we study the nonlinear vibronic dynamics of a trapped ion, driven in the resolved sideband regime with some small frequency mismatch. By describing the pump field in a quantized manner, we are able to derive exact solutions for the dynamics of the system. This eventually allows us to provide analytical solutions for various types of time-dependent quantities. In particular, we study in some detail the electronic and the motional quantum dynamics of the ion, as well as the time evolution of the nonclassicality of the motional quantum state.

Background-free beta-decay half-life measurements by in-trap decay and high-resolution MR-ToF mass analysis

NASA Astrophysics Data System (ADS)

Wolf, R. N.; Atanasov, D.; Blaum, K.; Kreim, S.; Lunney, D.; Manea, V.; Rosenbusch, M.; Schweikhard, L.; Welker, A.; Wienholtz, F.; Zuber, K.

2016-06-01

In-trap decay in ISOLTRAP's radiofrequency quadrupole (RFQ) ion beam cooler and buncher was used to determine the lifetime of short-lived nuclides. After various storage times, the remaining mother nuclides were mass separated from accompanying isobaric contaminations by the multi-reflection time-of-flight mass separator (MR-ToF MS), allowing for a background-free ion counting. A feasibility study with several online measurements shows that the applications of the ISOLTRAP setup can be further extended by exploiting the high resolving power of the MR-ToF MS in combination with in-trap decay and single-ion counting.

Direct measurement of the transition from edge to core power coupling in a light-ion helicon source

NASA Astrophysics Data System (ADS)

Piotrowicz, P. A.; Caneses, J. F.; Showers, M. A.; Green, D. L.; Goulding, R. H.; Caughman, J. B. O.; Biewer, T. M.; Rapp, J.; Ruzic, D. N.

2018-05-01

We present time-resolved measurements of an edge-to-core power transition in a light-ion (deuterium) helicon discharge in the form of infra-red camera imaging of a thin stainless steel target plate on the Proto-Material Exposure eXperiment device. The time-resolved images measure the two-dimensional distribution of power deposition in the helicon discharge. The discharge displays a mode transition characterized by a significant increase in the on-axis electron density and core power coupling, suppression of edge power coupling, and the formation of a fast-wave radial eigenmode. Although the self-consistent mechanism that drives this transition is not yet understood, the edge-to-core power transition displays characteristics that are consistent with the discharge entering a slow-wave anti-resonant regime. RF magnetic field measurements made across the plasma column, together with the power deposition results, provide direct evidence to support the suppression of the slow-wave in favor of core plasma production by the fast-wave in a light-ion helicon source.

Quantitative study of energy-transfer mechanism in Eu,O-codoped GaN by time-resolved photoluminescence spectroscopy

NASA Astrophysics Data System (ADS)

Inaba, Tomohiro; Kojima, Takanori; Yamashita, Genki; Matsubara, Eiichi; Mitchell, Brandon; Miyagawa, Reina; Eryu, Osamu; Tatebayashi, Jun; Ashida, Masaaki; Fujiwara, Yasufumi

2018-04-01

In order to investigate the excitation processes in Eu,O-codoped GaN (GaN:Eu,O), the time-resolved photoluminescence signal including the rising part is analyzed. A rate equation is developed based upon a model for the excitation processes in GaN:Eu to fit the experimental data. The non-radiative recombination rate of the trap state in the GaN host, the energy transfer rate between the Eu3+ ions and the GaN host, the radiative transition probability of Eu3+ ion, as well as the ratio of the number of luminescent sites (OMVPE 4α and OMVPE 4β), are simultaneously determined. It is revealed and quantified that radiative transition probability of the Eu ion is the bottleneck for the enhancement of light output from GaN:Eu. We also evaluate the effect of the growth conditions on the luminescent efficiency of GaN:Eu quantitatively, and find the correlation between emission intensity of GaN:Eu and the fitting parameters introduced in our model.

Direct measurement of the transition from edge to core power coupling in a light-ion helicon source

DOE PAGES

Piotrowicz, Pawel A.; Caneses, Juan F.; Showers, Melissa A.; ...

2018-05-02

Here, we present time-resolved measurements of an edge-to-core power transition in a light-ion (deuterium) helicon discharge in the form of infra-red camera imaging of a thin stainless steel target plate on the Proto-Material Exposure eXperiment device. The time-resolved images measure the two-dimensional distribution of power deposition in the helicon discharge. The discharge displays a mode transition characterized by a significant increase in the on-axis electron density and core power coupling, suppression of edge power coupling, and the formation of a fast-wave radial eigenmode. Although the self-consistent mechanism that drives this transition is not yet understood, the edge-to-core power transition displaysmore » characteristics that are consistent with the discharge entering a slow-wave anti-resonant regime. RF magnetic field measurements made across the plasma column, together with the power deposition results, provide direct evidence to support the suppression of the slow-wave in favor of core plasma production by the fast-wave in a light-ion helicon source.« less

Direct measurement of the transition from edge to core power coupling in a light-ion helicon source

DOE Office of Scientific and Technical Information (OSTI.GOV)

Piotrowicz, Pawel A.; Caneses, Juan F.; Showers, Melissa A.

Here, we present time-resolved measurements of an edge-to-core power transition in a light-ion (deuterium) helicon discharge in the form of infra-red camera imaging of a thin stainless steel target plate on the Proto-Material Exposure eXperiment device. The time-resolved images measure the two-dimensional distribution of power deposition in the helicon discharge. The discharge displays a mode transition characterized by a significant increase in the on-axis electron density and core power coupling, suppression of edge power coupling, and the formation of a fast-wave radial eigenmode. Although the self-consistent mechanism that drives this transition is not yet understood, the edge-to-core power transition displaysmore » characteristics that are consistent with the discharge entering a slow-wave anti-resonant regime. RF magnetic field measurements made across the plasma column, together with the power deposition results, provide direct evidence to support the suppression of the slow-wave in favor of core plasma production by the fast-wave in a light-ion helicon source.« less

Observation and modeling of interspecies ion separation in inertial confinement fusion implosions via imaging x-ray spectroscopy

DOE PAGES

Joshi, Tirtha Raj; Hakel, Peter; Hsu, Scott C.; ...

2017-03-22

In this article, we report the first direct experimental evidence of interspecies ion separation in direct-drive inertial confinement fusion experiments performed at the OMEGA laser facility via spectrally, temporally, and spatially resolved imaging x-ray-spectroscopy data [S. C. Hsu et al., Europhys. Lett. 115, 65001 (2016)]. These experiments were designed based on the expectation that interspecies ion thermo-diffusion would be the strongest for species with a large mass and charge difference. The targets were spherical plastic shells filled with D2 and a trace amount of Ar (0.1% or 1% by atom). Ar K-shell spectral features were observed primarily between the timemore » of first-shock convergence and slightly before the neutron bang time, using a time- and space-integrated spectrometer, a streaked crystal spectrometer, and two gated multi-monochromatic x-ray imagers fielded along quasi-orthogonal lines of sight. Detailed spectroscopic analyses of spatially resolved Ar K-shell lines reveal the deviation from the initial 1% Ar gas fill and show both Ar-concentration enhancement and depletion at different times and radial positions of the implosion. The experimental results are interpreted using radiation-hydrodynamic simulations that include recently implemented, first-principles models of interspecies ion diffusion. Lastly, the experimentally inferred Ar-atom fraction profiles agree reasonably with calculated profiles associated with the incoming and rebounding first shock.« less

Mobility-Resolved Ion Selection in Uniform Drift Field Ion Mobility Spectrometry/Mass Spectrometry: Dynamic Switching in Structures for Lossless Ion Manipulations

DOE PAGES

Webb, Ian K.; Garimella, Sandilya V. B.; Tolmachev, Aleksey V.; ...

2014-09-15

A Structures for Lossless Ion Manipulations (SLIM) module that allows ion mobility separations and the switching of ions between alternative drift paths is described. The SLIM switch component has a “Tee” configuration and allows switching of ions between a linear path and a 90-degree bend. By controlling switching times, ions can be deflected to an alternative channel as a function of their mobilities. In the initial evaluation the switch is used in a static mode and shown compatible with high performance ion mobility separations at 4 torr. In the “dynamic mode” we show that mobility-selected ions can be switched intomore » the alternative channel, and that various ion species can be independently selected based on their mobilities for time-of-flight mass spectrometer (TOF MS) IMS detection and mass analysis. Ultimately, this development also provides the basis for e.g. the selection of specific mobilities for storage and accumulation, and key modules for the assembly of SLIM devices enabling much more complex sequences of ion manipulations.« less

Dipole Excitation With A Paul Ion Trap Mass Spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

MacAskill, J. A.; Madzunkov, S. M.; Chutjian, A.

Preliminary results are presented for the use of an auxiliary radiofrequency (rf) excitation voltage in combination with a high purity, high voltage rf generator to perform dipole excitation within a high precision Paul ion trap. These results show the effects of the excitation frequency over a continuous frequency range on the resultant mass spectra from the Paul trap with particular emphasis on ion ejection times, ion signal intensity, and peak shapes. Ion ejection times are found to decrease continuously with variations in dipole frequency about several resonant values and show remarkable symmetries. Signal intensities vary in a complex fashion withmore » numerous resonant features and are driven to zero at specific frequency values. Observed intensity variations depict dipole excitations that target ions of all masses as well as individual masses. Substantial increases in mass resolution are obtained with resolving powers for nitrogen increasing from 114 to 325.« less

Time-resolved and Depth-dependent Photo-Degradation of Marine Dissolved Organic Matter Analyzed by Semi-continuous EEM Fluorescence Monitoring

NASA Astrophysics Data System (ADS)

Gonsior, M.; Timko, S.; Conte, M. H.; Schmitt-Kopplin, P.

2016-02-01

Ten liter water samples were collected at the Bermuda Atlantic Time Series Station (BATS) at 200 m intervals down to a maximum depth of 4530 m and solid-phase extracted. The methanol extracts were dried and re-dissolved in pure water and then used to determine the time-resolved photo-degradation of marine dissolved organic matter to be able to determine kinetic data. Excitation Emission Matrix (EEM) fluorescence spectra were recorded every 20 minutes using a custom-built flow-through photo-degradation system during 20 h of solar simulated light exposure. The resulting EEM spectra were modeled using Parallel Factor Analysis (PARAFAC) and results revealed reproducible and significant changes in the photo-degradation of marine FDOM originating from different depths. A five component model was fitted and the terrestrial-like components showed the expected high photo-reactivity, but surprisingly, the traditional marine-like peak showed slight photo-production in the surface layer, which might be the reason for its prevalence in the open ocean. Surface ocean waters were depleted in the highly photo-degradable components while protein-like fluorescent components were enriched, which was in agreement with previous studies. Ultrahigh resolution mass spectrometry confirmed unique aliphatic molecular ions in the Surface Ocean and hydrogen-deficient molecules at depth. Multivariate statistical analyses revealed strong correlations between unsaturated/aromatic molecular ions and depth, where aliphatic molecular ions were more prevalent in the Surface Ocean and aromatic molecular ions at depth. Strong correlations were also found between hydrogen-deficient molecular ions and the humic-like fluorescent components. The rapid photo-degradation of the deep-sea FDOM and the surface oceans relative depletion of aromatic molecular ions suggested that deep-ocean FDOM may be too photochemically labile to survive meridional overturning circulation.

A new hybrid electrospray Fourier transform mass spectrometer: design and performance characteristics.

PubMed

O'connor, Peter B; Pittman, Jason L; Thomson, Bruce A; Budnik, Bogdan A; Cournoyer, Jason C; Jebanathirajah, Judith; Lin, Cheng; Moyer, Susanne; Zhao, Cheng

2006-01-01

A new hybrid electrospray quadrupole Fourier transform mass spectrometry (FTMS) instrument design is shown and characterized. This instrument involves coupling an electrospray source and mass-resolving quadrupole, ion accumulation, and collision cell linear ion trap system developed by MDS Sciex with a home-built ion guide and ion cyclotron resonance (ICR) cell. The iterative progression of this design is shown. The final design involves a set of hexapole ion guides to transfer the ions from the accumulation/collision trap through the magnetic field gradient and into the cell. These hexapole ion guides are separated by a thin gate valve and two conduction limits to maintain the required <10(-9) mbar vacuum for FTICR. Low-attomole detection limits for a pure peptide are shown, 220 000 resolving power in broadband mode and 820 000 resolving power in narrow-band mode are demonstrated, and mass accuracy in the <2 ppm range is routinely available provided the signal is abundant, cleanly resolved, and internally calibrated. This instrument design provides high experimental flexibility, allowing Q2 CAD, SORI-CAD, IRMPD, and ECD experiments with selected ion accumulation as well as experiments such as nozzle skimmer dissociation. Initial top-down mass spectrometry experiments on a protein is shown using ECD.

Highly time-resolved imaging of combustion and pyrolysis product concentrations in solid fuel combustion: NO formation in a burning cigarette.

PubMed

Zimmermann, Ralf; Hertz-Schünemann, Romy; Ehlert, Sven; Liu, Chuan; McAdam, Kevin; Baker, Richard; Streibel, Thorsten

2015-02-03

The highly dynamic, heterogeneous combustion process within a burning cigarette was investigated by a miniaturized extractive sampling probe (microprobe) coupled to photoionization mass spectrometry using soft laser single photon ionization (SPI) for online real-time detection of molecular ions of combustion and pyrolysis products. Research cigarettes smoked by a smoking machine are used as a reproducible model system for solid-state biomass combustion, which up to now is not addressable by current combustion-diagnostic tools. By combining repetitively recorded online measurement sequences from different sampling locations in an imaging approach, highly time- and space-resolved quantitative distribution maps of, e.g., nitrogen monoxide, benzene, and oxygen concentrations were obtained at a near microscopic level. The obtained quantitative distribution maps represent a time-resolved, movie-like imaging of the respective compound's formation and destruction zones in the various combustion and pyrolysis regions of a cigarette during puffing. Furthermore, spatially resolved kinetic data were ascertainable. The here demonstrated methodology can also be applied to various heterogenic combustion/pyrolysis or reaction model systems, such as fossil- or biomass-fuel pellet combustion or to a positional resolved analysis of heterogenic catalytic reactions.

Femtosecond manipulation of spins, charges, and ions in nanostructures, thin films, and surfaces

PubMed Central

Carbone, F.; Hengsberger, M.; Castiglioni, L.; Osterwalder, J.

2017-01-01

Modern ultrafast techniques provide new insights into the dynamics of ions, charges, and spins in photoexcited nanostructures. In this review, we describe the use of time-resolved electron-based methods to address specific questions such as the ordering properties of self-assembled nanoparticles supracrystals, the interplay between electronic and structural dynamics in surfaces and adsorbate layers, the light-induced control of collective electronic modes in nanowires and thin films, and the real-space/real-time evolution of the skyrmion lattice in topological magnets. PMID:29308416

On the Surface Mapping using Individual Cluster Impacts

PubMed Central

Fernandez-Lima, F.A.; Eller, M.J.; DeBord, J.D.; Verkhoturov, S.V.; Della-Negra, S.; Schweikert, E.A.

2011-01-01

This paper describes the advantages of using single impacts of large cluster projectiles (e.g. C60 and Au400) for surface mapping and characterization. The analysis of co-emitted time-resolved photon spectra, electron distributions and characteristic secondary ions shows that they can be used as surface fingerprints for target composition, morphology and structure. Photon, electron and secondary ion emission increases with the projectile cluster size and energy. The observed, high abundant secondary ion emission makes cluster projectiles good candidates for surface mapping of atomic and fragment ions (e.g., yield >1 per nominal mass) and molecular ions (e.g., few tens of percent in the 500 < m/z < 1500 range). PMID:22393269

A Particle X-ray Temporal Diagnostic (PXTD) for studies of kinetic, multi-ion effects, and ion-electron equilibration rates in Inertial Confinement Fusion plasmas at OMEGA (invited)

NASA Astrophysics Data System (ADS)

Sio, H.; Frenje, J. A.; Katz, J.; Stoeckl, C.; Weiner, D.; Bedzyk, M.; Glebov, V.; Sorce, C.; Gatu Johnson, M.; Rinderknecht, H. G.; Zylstra, A. B.; Sangster, T. C.; Regan, S. P.; Kwan, T.; Le, A.; Simakov, A. N.; Taitano, W. T.; Chacòn, L.; Keenan, B.; Shah, R.; Sutcliffe, G.; Petrasso, R. D.

2016-11-01

A Particle X-ray Temporal Diagnostic (PXTD) has been implemented on OMEGA for simultaneous time-resolved measurements of several nuclear products as well as the x-ray continuum produced in High Energy Density Plasmas and Inertial Confinement Fusion implosions. The PXTD removes systematic timing uncertainties typically introduced by using multiple instruments, and it has been used to measure DD, DT, D3He, and T3He reaction histories and the emission history of the x-ray core continuum with relative timing uncertainties within ±10-20 ps. This enables, for the first time, accurate and simultaneous measurements of the x-ray emission histories, nuclear reaction histories, their time differences, and measurements of Ti(t) and Te(t) from which an assessment of multiple-ion-fluid effects, kinetic effects during the shock-burn phase, and ion-electron equilibration rates can be made.

A Particle X-ray Temporal Diagnostic (PXTD) for studies of kinetic, multi-ion effects, and ion-electron equilibration rates in Inertial Confinement Fusion plasmas at OMEGA (invited)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sio, H.; Frenje, J. A.; Katz, J.

Here, a Particle X-ray Temporal Diagnostic (PXTD) has been implemented on OMEGA for simultaneous time-resolved measurements of several nuclear products as well as the x-ray continuum produced in High Energy Density Plasmas and Inertial Confinement Fusion implosions. The PXTD removes systematic timing uncertainties typically introduced by using multiple instruments, and it has been used to measure DD, DT, D 3He, and T 3He reaction histories and the emission history of the x-ray core continuum with relative timing uncertainties within ±10-20 ps. This enables, for the first time, accurate and simultaneous measurements of the x-ray emission histories, nuclear reaction histories, theirmore » time differences, and measurements of T i(t) and T e(t) from which an assessment of multiple-ion-fluid effects, kinetic effects during the shock-burn phase, and ion-electron equilibration rates can be made.« less

A Particle X-ray Temporal Diagnostic (PXTD) for studies of kinetic, multi-ion effects, and ion-electron equilibration rates in Inertial Confinement Fusion plasmas at OMEGA (invited)

DOE PAGES

Sio, H.; Frenje, J. A.; Katz, J.; ...

2016-09-14

Here, a Particle X-ray Temporal Diagnostic (PXTD) has been implemented on OMEGA for simultaneous time-resolved measurements of several nuclear products as well as the x-ray continuum produced in High Energy Density Plasmas and Inertial Confinement Fusion implosions. The PXTD removes systematic timing uncertainties typically introduced by using multiple instruments, and it has been used to measure DD, DT, D 3He, and T 3He reaction histories and the emission history of the x-ray core continuum with relative timing uncertainties within ±10-20 ps. This enables, for the first time, accurate and simultaneous measurements of the x-ray emission histories, nuclear reaction histories, theirmore » time differences, and measurements of T i(t) and T e(t) from which an assessment of multiple-ion-fluid effects, kinetic effects during the shock-burn phase, and ion-electron equilibration rates can be made.« less

A chemometric approach for characterization of serum transthyretin in familial amyloidotic polyneuropathy type I (FAP-I) by electrospray ionization-ion mobility mass spectrometry.

PubMed

Pont, Laura; Sanz-Nebot, Victoria; Vilaseca, Marta; Jaumot, Joaquim; Tauler, Roma; Benavente, Fernando

2018-05-01

In this study, we describe a chemometric data analysis approach to assist in the interpretation of the complex datasets from the analysis of high-molecular mass oligomeric proteins by ion mobility mass spectrometry (IM-MS). The homotetrameric protein transthyretin (TTR) is involved in familial amyloidotic polyneuropathy type I (FAP-I). FAP-I is associated with a specific TTR mutant variant (TTR(Met30)) that can be easily detected analyzing the monomeric forms of the mutant protein. However, the mechanism of protein misfolding and aggregation onset, which could be triggered by structural changes in the native tetrameric protein, remains under investigation. Serum TTR from healthy controls and FAP-I patients was purified under non-denaturing conditions by conventional immunoprecipitation in solution and analyzed by IM-MS. IM-MS allowed separation and characterization of several tetrameric, trimeric and dimeric TTR gas ions due to their differential drift time. After an appropriate data pre-processing, multivariate curve resolution alternating least squares (MCR-ALS) was applied to the complex datasets. A group of seven independent components being characterized by their ion mobility profiles and mass spectra were resolved to explain the observed data variance in control and patient samples. Then, principal component analysis (PCA) and partial least squares discriminant analysis (PLS-DA) were considered for exploration and classification. Only four out of the seven resolved components were enough for an accurate differentiation. Furthermore, the specific TTR ions identified in the mass spectra of these components and the resolved ion mobility profiles provided a straightforward insight into the most relevant oligomeric TTR proteoforms for the disease. Copyright © 2018 Elsevier B.V. All rights reserved.

The role of upstream distal electrodes in mitigating electrochemical degradation of ionic liquid ion sources

NASA Astrophysics Data System (ADS)

Brikner, Natalya; Lozano, Paulo C.

2012-11-01

Ionic liquid ion sources produce molecular ions from micro-tip emitters wetted with room-temperature molten salts. When a single ion polarity is extracted, counterions accumulate and generate electrochemical reactions that limit the source lifetime. The dynamics of double layer formation are reviewed and distal electrode contacts are introduced to resolve detrimental electrochemical decomposition effects at the micro-tip apex. By having the emitter follow the ionic liquid potential, operation can be achieved for an extended period of time with no apparent degradation of the material, indicating that electrochemistry can be curtailed and isolated to the upstream distal electrode.

Angular distribution of ions and extreme ultraviolet emission in laser-produced tin droplet plasma

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chen, Hong; Duan, Lian; Lan, Hui

Angular-resolved ion time-of-flight spectra as well as extreme ultraviolet radiation in laser-produced tin droplet plasma are investigated experimentally and theoretically. Tin droplets with a diameter of 150 μm are irradiated by a pulsed Nd:YAG laser. The ion time-of-flight spectra measured from the plasma formed by laser irradiation of the tin droplets are interpreted in terms of a theoretical elliptical Druyvesteyn distribution to deduce ion density distributions including kinetic temperatures of the plasma. The opacity of the plasma for extreme ultraviolet radiation is calculated based on the deduced ion densities and temperatures, and the angular distribution of extreme ultraviolet radiation is expressedmore » as a function of the opacity using the Beer–Lambert law. Our results show that the calculated angular distribution of extreme ultraviolet radiation is in satisfactory agreement with the experimental data.« less

Angular distribution of ions and extreme ultraviolet emission in laser-produced tin droplet plasma

NASA Astrophysics Data System (ADS)

Chen, Hong; Wang, Xinbing; Duan, Lian; Lan, Hui; Chen, Ziqi; Zuo, Duluo; Lu, Peixiang

2015-05-01

Angular-resolved ion time-of-flight spectra as well as extreme ultraviolet radiation in laser-produced tin droplet plasma are investigated experimentally and theoretically. Tin droplets with a diameter of 150 μm are irradiated by a pulsed Nd:YAG laser. The ion time-of-flight spectra measured from the plasma formed by laser irradiation of the tin droplets are interpreted in terms of a theoretical elliptical Druyvesteyn distribution to deduce ion density distributions including kinetic temperatures of the plasma. The opacity of the plasma for extreme ultraviolet radiation is calculated based on the deduced ion densities and temperatures, and the angular distribution of extreme ultraviolet radiation is expressed as a function of the opacity using the Beer-Lambert law. Our results show that the calculated angular distribution of extreme ultraviolet radiation is in satisfactory agreement with the experimental data.

CRF-PEPICO: Double velocity map imaging photoelectron photoion coincidence spectroscopy for reaction kinetics studies

NASA Astrophysics Data System (ADS)

Sztáray, Bálint; Voronova, Krisztina; Torma, Krisztián G.; Covert, Kyle J.; Bodi, Andras; Hemberger, Patrick; Gerber, Thomas; Osborn, David L.

2017-07-01

Photoelectron photoion coincidence (PEPICO) spectroscopy could become a powerful tool for the time-resolved study of multi-channel gas phase chemical reactions. Toward this goal, we have designed and tested electron and ion optics that form the core of a new PEPICO spectrometer, utilizing simultaneous velocity map imaging for both cations and electrons, while also achieving good cation mass resolution through space focusing. These optics are combined with a side-sampled, slow-flow chemical reactor for photolytic initiation of gas-phase chemical reactions. Together with a recent advance that dramatically increases the dynamic range in PEPICO spectroscopy [D. L. Osborn et al., J. Chem. Phys. 145, 164202 (2016)], the design described here demonstrates a complete prototype spectrometer and reactor interface to carry out time-resolved experiments. Combining dual velocity map imaging with cation space focusing yields tightly focused photoion images for translationally cold neutrals, while offering good mass resolution for thermal samples as well. The flexible optics design incorporates linear electric fields in the ionization region, surrounded by dual curved electric fields for velocity map imaging of ions and electrons. Furthermore, the design allows for a long extraction stage, which makes this the first PEPICO experiment to combine ion imaging with the unimolecular dissociation rate constant measurements of cations to detect and account for kinetic shifts. Four examples are shown to illustrate some capabilities of this new design. We recorded the threshold photoelectron spectrum of the propargyl and the iodomethyl radicals. While the former agrees well with a literature threshold photoelectron spectrum, we have succeeded in resolving the previously unobserved vibrational structure in the latter. We have also measured the bimolecular rate constant of the CH2I + O2 reaction and observed its product, the smallest Criegee intermediate, CH2OO. Finally, the second dissociative photoionization step of iodocyclohexane ions, the loss of ethylene from the cyclohexyl cation, is slow at threshold, as illustrated by the asymmetric threshold photoionization time-of-flight distributions.

Highly charged ion beams and their applications

NASA Astrophysics Data System (ADS)

Marler, Joan

2018-01-01

While much previous work with highly charged ions has been performed with the ions in the plasma state in which they were formed, beams of highly charged ions hold promise for exciting new experiments. Specifically low energy beams with a high degree of charge state purity are a prerequisite for momentum resolved cross section measurements and for efficient loading of highly charged ions into UHV traps for spectroscopy. The Clemson University facility is optimized for the delivery of such beams of highly charged ions with low kinetic energies. Near term experiments include energy resolved charge exchange with neutral targets.

EUV emission spectra in collisions of highly charged tantalum ions with nitrogen and oxygen molecules

NASA Astrophysics Data System (ADS)

Tanuma, Hajime; Numadate, Naoki; Uchikura, Yoshiyuki; Shimada, Kento; Akutsu, Takuto; Long, Elaine; O'Sullivan, Gerry

2017-10-01

We have performed ion beam collision experiments using multiply charged tantalum ions and observed EUV (extreme ultra-violet) emission spectra in collisions of ions with molecular targets, N2 and O2. Broad UTAs (un-resolved transition arrays) from multiply charged Ta ions were observed, and the mean wavelengths of the UTAs shifted and became shorter at higher charge statea of Ta ions. These UTAs may be attributed to the 4f-5d and 4f-5g transitions. Not only the UTA emission from incident ions, but also the sharp emission lines from multiply charged fragment atomic ions were observed. Production of temporary highly charged molecular ions, their kinetic energy and fragmentation processes have been investigated with coincident detection technique. However, the observation of emission from the fragments might be for the first time. The formation mechanisms of the multiply charged fragment atomic ions from target molecules are discussed.

New beam line for time-of-flight medium energy ion scattering with large area position sensitive detector

NASA Astrophysics Data System (ADS)

Linnarsson, M. K.; Hallén, A.; Åström, J.; Primetzhofer, D.; Legendre, S.; Possnert, G.

2012-09-01

A new beam line for medium energy ion mass scattering (MEIS) has been designed and set up at the Ångström laboratory, Uppsala University, Sweden. This MEIS system is based on a time-of-flight (ToF) concept and the electronics for beam chopping relies on a 4 MHz function generator. Repetition rates can be varied between 1 MHz and 63 kHz and pulse widths below 1 ns are typically obtained by including beam bunching. A 6-axis goniometer is used at the target station. Scattering angle and energy of backscattered ions are extracted from a time-resolved and position-sensitive detector. Examples of the performance are given for three kinds of probing ions, 1H+, 4He+, and 11B+. Depth resolution is in the nanometer range and 1 and 2 nm thick Pt layers can easily be resolved. Mass resolution between nearby isotopes can be obtained as illustrated by Ga isotopes in GaAs. Taking advantage of the large size detector, a direct imaging (blocking pattern) of crystal channels are shown for hexagonal, 4H-SiC. The ToF-MEIS system described in this paper is intended for use in semiconductor and thin film areas. For example, depth profiling in the sub nanometer range for device development of contacts and dielectric interfaces. In addition to applied projects, fundamental studies of stopping cross sections in this medium energy range will also be conducted.

Absorption Mode FT-ICR Mass Spectrometry Imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smith, Donald F.; Kilgour, David P.; Konijnenburg, Marco

2013-12-03

Fourier transform ion cyclotron resonance mass spectrometry offers the highest mass resolving power for molecular imaging experiments. This high mass resolving power ensures that closely spaced peaks at the same nominal mass are resolved for proper image generation. Typically higher magnetic fields are used to increase mass resolving power. However, a gain in mass resolving power can also be realized by phase correction of the data for absorption mode display. In addition to mass resolving power, absorption mode offers higher mass accuracy and signal-to-noise ratio over the conventional magnitude mode. Here we present the first use of absorption mode formore » Fourier transform ion cyclotron resonance mass spectrometry imaging. The Autophaser algorithm is used to phase correct each spectrum (pixel) in the image and then these parameters are used by the Chameleon work-flow based data processing software to generate absorption mode ?Datacubes? for image and spectral viewing. Absorption mode reveals new mass and spatial features that are not resolved in magnitude mode and results in improved selected ion image contrast.« less

Ion behaviour in pulsed plasma regime by means of Time-resolved energy mass spectroscopy (TREMS) applied to an industrial radiofrequency Plasma Immersion Ion Implanter PULSION registered

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carrere, M.; Kaeppelin, V.; Torregrosa, F.

2006-11-13

In order to face the requirements for P+/N junctions requested for < 45 nm ITRS nodes, new doping techniques are studied. Among them Plasma Immersion Ion Implantation (PIII) has been largely studied. IBS has designed and developed its own PIII machine named PULSION registered . This machine is using a pulsed plasma. As other modem technological applications of low pressure plasma, PULSION registered needs a precise control over plasma parameters in order to optimise process characteristics. In order to improve pulsed plasma discharge devoted to PIII, a nitrogen pulsed plasma has been studied in the inductively coupled plasma (ICP) ofmore » PULSION registered and an argon pulsed plasma has been studied in the helicon discharge of the laboratory reactor of LPIIM (PHYSIS). Measurements of the Ion Energy Distribution Function (IEDF) with EQP300 (Hidden) have been performed in both pulsed plasma. This study has been done for different energies which allow to reconstruct the IEDF resolved in time (TREMS). By comparing these results, we found that the beginning of the plasma pulse, named ignition, exhaust at least three phases, or more. All these results allowed us to explain plasma dynamics during the pulse while observing transitions between capacitive and inductive coupling. This study leads in a better understanding of changes in discharge parameters as plasma potential, electron temperature, ion density.« less

Tunable single and double emission semiconductor nanocrystal quantum dots: a multianalyte sensor

NASA Astrophysics Data System (ADS)

Ratnesh, Ratneshwar Kumar; Singh Mehata, Mohan

2018-07-01

We have prepared stable colloidal CdTe and CdTe/ZnS core–shell quantum dots (QDs) using hot injection chemical route. The developed CdTe QDs emit tunable single and dual photoluminescence (PL) bands, originating from the direct band edge and the surface state of QDs, as evident by the steady-state and time-resolved spectroscopy. The developed CdTe and CdTe/ZnS QDs act as optical sensors for the detection of metal ions (e.g., Fe2+ and Pb2+) in the feed water. The PL quenching in the presence of analytes has been examined by both the steady-state and time-resolved PL spectroscopy. The linear Stern–Volmer (S–V) plots obtained for PL intensity and lifetime as a function of metal ion concentration demonstrates the diffusion-mediated collisional quenching as a dominant mechanism together with the possibility of fluorescence resonance energy transfer. Thus, the prepared core and core–shell QDs which cover a broad spectral range of white light with high quantum yield (QY) are highly sensitive to the detection of metal ions in feed water and are also important for biological applications (Ratnesh and Mehata 2017 Spectrochim. Acta A: Mol. Biomol. Spectro. 179 201–10).

Rocket-borne time-of-flight mass spectrometry

NASA Technical Reports Server (NTRS)

Reiter, R. F.

1976-01-01

Theoretical and numerical analyses are made of planar, cylindrical and spherical-electrode two-field time-of-flight mass spectrometers in order to optimize their operating conditions. A method is introduced which can improve the resolving power of these instruments by a factor of 7.5. Potential barrier gating in time-of-flight mass spectrometers is also analyzed. Experimental studies of a miniature cylindrical-electrode and a hemispherical-electrode time-of-flight mass spectrometer are presented. Their sensitivity and ability to operate at D-region pressures with an open source make them ideal instruments for D-region ion composition measurements. A sounding rocket experiment package carrying a cylindrical electrode time-of-flight mass spectrometer was launched. The data indicate that essentially 100% of the positive electric charge on positive ions is carried by ions with mass-to-charge ratios greater than 500 below an altitude of 92 km. These heavy charge carriers were present at altitudes up to about 100 km.

Detection of aqueous phase chemical warfare agent degradation products by negative mode ion mobility time-of-flight mass spectrometry [IM(tof)MS].

PubMed

Steiner, Wes E; Harden, Charles S; Hong, Feng; Klopsch, Steve J; Hill, Herbert H; McHugh, Vincent M

2006-02-01

The use of negative ion monitoring mode with an atmospheric pressure ion mobility orthogonal reflector time-of-flight mass spectrometer [IM(tof)MS] to detect chemical warfare agent (CWA) degradation products from aqueous phase samples has been determined. Aqueous phase sampling used a traditional electrospray ionization (ESI) source for sample introduction and ionization. Certified reference materials (CRM) of CWA degradation products for the detection of Schedule 1, 2, or 3 toxic chemicals or their precursors as defined by the chemical warfare convention (CWC) treaty verification were used in this study. A mixture of six G-series nerve related CWA degradation products (EMPA, IMPA, EHEP, IHEP, CHMPA, and PMPA) and their related collision induced dissociation (CID) fragment ions (MPA and EPA) were found in each case to be clearly resolved and detected using the IM(tof)MS instrument in negative ion monitoring mode. Corresponding ions, masses, drift times, K(o) values, and signal intensities for each of the CWA degradation products are reported.

Rates and equilibrium constants of the ligand-induced conformational transition of an HCN ion channel protein domain determined by DEER spectroscopy.

PubMed

Collauto, Alberto; DeBerg, Hannah A; Kaufmann, Royi; Zagotta, William N; Stoll, Stefan; Goldfarb, Daniella

2017-06-14

Ligand binding can induce significant conformational changes in proteins. The mechanism of this process couples equilibria associated with the ligand binding event and the conformational change. Here we show that by combining the application of W-band double electron-electron resonance (DEER) spectroscopy with microfluidic rapid freeze quench (μRFQ) it is possible to resolve these processes and obtain both equilibrium constants and reaction rates. We studied the conformational transition of the nitroxide labeled, isolated carboxy-terminal cyclic-nucleotide binding domain (CNBD) of the HCN2 ion channel upon binding of the ligand 3',5'-cyclic adenosine monophosphate (cAMP). Using model-based global analysis, the time-resolved data of the μRFQ DEER experiments directly provide fractional populations of the open and closed conformations as a function of time. We modeled the ligand-induced conformational change in the protein using a four-state model: apo/open (AO), apo/closed (AC), bound/open (BO), bound/closed (BC). These species interconvert according to AC + L ⇌ AO + L ⇌ BO ⇌ BC. By analyzing the concentration dependence of the relative contributions of the closed and open conformations at equilibrium, we estimated the equilibrium constants for the two conformational equilibria and the open-state ligand dissociation constant. Analysis of the time-resolved μRFQ DEER data gave estimates for the intrinsic rates of ligand binding and unbinding as well as the rates of the conformational change. This demonstrates that DEER can quantitatively resolve both the thermodynamics and the kinetics of ligand binding and the associated conformational change.

Laser ion source for multi-nucleon transfer reaction products

NASA Astrophysics Data System (ADS)

Hirayama, Y.; Watanabe, Y. X.; Imai, N.; Ishiyama, H.; Jeong, S. C.; Miyatake, H.; Oyaizu, M.; Kimura, S.; Mukai, M.; Kim, Y. H.; Sonoda, T.; Wada, M.; Huyse, M.; Kudryavtsev, Yu.; Van Duppen, P.

2015-06-01

We have developed a laser ion source for the target-like fragments (TLFs) produced in multi-nucleon transfer (MNT) reactions. The operation principle of the source is based on the in-gas laser ionization and spectroscopy (IGLIS) approach. In the source TLFs are thermalized and neutralized in high pressure and high purity argon gas, and are extracted after being selectively re-ionized in a multi-step laser resonance ionization process. The laser ion source has been implemented at the KEK Isotope Separation System (KISS) for β-decay spectroscopy of neutron-rich isotopes with N = 126 of nuclear astrophysical interest. The simulations of gas flow and ion-beam optics have been performed to optimize the gas cell for efficient thermalization and fast transporting the TLFs, and the mass-separator for efficient transport with high mass-resolving power, respectively. To confirm the performances expected at the design stage, off-line experiments have been performed by using 56Fe atoms evaporated from a filament in the gas cell. The gas-transport time of 230 ms in the argon cell and the measured KISS mass-resolving power of 900 are consistent with the designed values. The high purity of the gas-cell system, which is extremely important for efficient and highly-selective production of laser ions, was achieved and confirmed from the mass distribution of the extracted ions. After the off-line tests, on-line experiments were conducted by directly injecting energetic 56Fe beam into the gas cell. After thermalization of the injected 56Fe beam, laser-produced singly-charged 56Fe+ ions were extracted. The extraction efficiency and selectivity of the gas cell in the presence of plasma induced by 56Fe beam injection as well as the time profile of the extracted ions were investigated; extraction efficiency of 0.25%, a beam purity of >99% and an extraction time of 270 ms. It has been confirmed that the performance of the KISS laser ion source is satisfactory to start the measurements of lifetimes of the β-decayed nuclei with N = 126 .

Preliminary results on time-resolved ion beam induced luminescence applied to the provenance study of lapis lazuli

NASA Astrophysics Data System (ADS)

Czelusniak, C.; Palla, L.; Massi, M.; Carraresi, L.; Giuntini, L.; Re, A.; Lo Giudice, A.; Pratesi, G.; Mazzinghi, A.; Ruberto, C.; Castelli, L.; Fedi, M. E.; Liccioli, L.; Gueli, A.; Mandò, P. A.; Taccetti, F.

2016-03-01

This work will present preliminary results concerning the use of time-resolved ion beam induced luminescence applied to provenance studies of lapis lazuli. Measurements were performed at the pulsed beam facility at LABEC laboratory in Florence. Lapis lazuli is a semi-precious gemstone, used as ornament since the early civilizations that can be found in few places on Earth. The importance of this work lies in understanding the origin of various samples of lapis lazuli, from which it may be possible to gain insight into trade routes from ancient times. The samples studied in this work originated from Chile, Afghanistan, Tajikistan, Myanmar, and Siberia. The stones were irradiated with 3 MeV protons and the resulting luminescence was detected by a photomultiplier tube, whose output was acquired using a sampling digitizer VME module (CAEN/V1720). Wavelength discrimination was performed at 430 nm utilizing a range of beam currents. The results showed that, by changing the beam current intensity, one can study different features of lapis lazuli, and this may aid in distinguishing lapis lazuli from different provenances.

Indirect consequences of exciplex states on the phosphorescence lifetime of phenazine-based 1,2,3-triazole luminescent probes.

PubMed

Costa, Bárbara B A; Jardim, Guilherme A M; Santos, Paloma L; Calado, Hállen D R; Monkman, Andrew P; Dias, Fernando B; da Silva Júnior, Eufrânio N; Cury, Luiz A

2017-02-01

The optical properties of phenazine derivative probe solutions involving intersystem crossing from singlet to triplet states were investigated by time resolved spectroscopy. The room temperature phosphorescence emission presented different time responses when Cd 2+ ions were bound to the probe chemical structure. The complex exciplex formation observed to occur in this case was not directly responsible for the change in the phosphorescence lifetime. This was more influenced by the new molecular conformation and modified spin-orbit coupling imposed by the binding of the Cd 2+ ions to the phenazine molecules.

Time-Resolved Tandem Faraday Cup Development for High Energy TNSA Particles

NASA Astrophysics Data System (ADS)

Padalino, S.; Simone, A.; Turner, E.; Ginnane, M. K.; Glisic, M.; Kousar, B.; Smith, A.; Sangster, C.; Regan, S.

2015-11-01

MTW and OMEGA EP Lasers at LLE utilize ultra-intense laser light to produce high-energy ion pulses through Target Normal Sheath Acceleration (TNSA). A Time Resolved Tandem Faraday Cup (TRTF) was designed and built to collect and differentiate protons from heavy ions (HI) produced during TNSA. The TRTF includes a replaceable thickness absorber capable of stopping a range of user-selectable HI emitted from TNSA plasma. HI stop within the primary cup, while less massive particles continue through and deposit their remaining charge in the secondary cup, releasing secondary electrons in the process. The time-resolved beam current generated in each cup will be measured on a fast storage scope in multiple channels. A charge-exchange foil at the TRTF entrance modifies the charge state distribution of HI to a known distribution. Using this distribution and the time of flight of the HI, the total HI current can be determined. Initial tests of the TRTF have been made using a proton beam produced by SUNY Geneseo's 1.7 MV Pelletron accelerator. A substantial reduction in secondary electron production, from 70% of the proton beam current at 2MeV down to 0.7%, was achieved by installing a pair of dipole magnet deflectors which successfully returned the electrons to the cups in the TRTF. Ultimately the TRTF will be used to normalize a variety of nuclear physics cross sections and stopping power measurements. Based in part upon work supported by a DOE NNSA Award#DE-NA0001944.

Kinetics of ion and prompt electron emission from laser-produced plasma

DOE Office of Scientific and Technical Information (OSTI.GOV)

Farid, N.; Key Laboratory of Materials Modification by Laser, Ion and Electron Beams, School of Physics and Optical Engineering, Dalian University of Technology, Dalian; Harilal, S. S.

2013-07-15

We investigated ion emission dynamics of laser-produced plasma from several elements, comprised of metals and non-metals (C, Al, Si, Cu, Mo, Ta, W), under vacuum conditions using a Faraday cup. The estimated ion flux for various targets studied showed a decreasing tendency with increasing atomic mass. For metals, the ion flux is found to be a function of sublimation energy. A comparison of temporal ion profiles of various materials showed only high-Z elements exhibited multiple structures in the ion time of flight profile indicated by the observation of higher peak kinetic energies, which were absent for low-Z element targets. Themore » slower ions were seen regardless of the atomic number of target material propagated with a kinetic energy of 1–5 keV, while the fast ions observed in high-Z materials possessed significantly higher energies. A systematic study of plasma properties employing fast photography, time, and space resolved optical emission spectroscopy, and electron analysis showed that there existed different mechanisms for generating ions in laser ablation plumes. The origin of high kinetic energy ions is related to prompt electron emission from high-Z targets.« less

Effect of ion pairing on the fluorescence of berberine, a natural isoquinoline alkaloid

NASA Astrophysics Data System (ADS)

Megyesi, Mónika; Biczók, László

2007-10-01

Effect of association with chloride or perchlorate anions on the fluorescence properties of berberine, a cationic isoquinoline alkaloid, has been studied. Interaction with Cl - caused more efficient fluorescence quenching; it significantly accelerated the radiationless deactivation and slowed down the radiative transition. Combined analysis of spectrophotometric, steady-state and time-resolved fluorescence results provided 1.5 × 10 5 M -1 for the equilibrium constant of ion pairing with Cl - in CH 2Cl 2. Both ion pairing and enrichment of the microenvironment of berberine in ions led to excited state quenching in solvents of medium polarity, but only the latter effect was observed in the presence of perchlorates in butyronitrile.

Laser Induced Fluorescence Studies of Electrostatic Double Layers in an Expanding Helicon Plasma

NASA Astrophysics Data System (ADS)

Carr, Jerry, Jr.

We report the first evidence of a laboratory double layer (DL) collapsing in the presence of an instability studied by Chakraborty Thakur et al. 1 with the use of time resolved laser induced fluorescence (LIF) studies. Higher time resolution studies then provided the first statistically validated proof of the correlation between the ion acoustic instability and a DL. Time-frequency analysis in the form of time resolved cross power spectra and continuous wavelet transforms were used to provide insight into beam formation. The implications of this work is that in the creation of strong DLs in expanding plasmas for plasma propulsion or other applications may be self-limited through instability growth. Over the past decade, experimental and theoretical studies have demonstrated the formation of stable, electrostatic, current-free double layers (CFDLs) in plasmas with a strong density gradient; typically a result of a divergent magnetic field. In this work, we present evidence for the formation of multiple double layers within a single divergent magnetic field structure. Downstream of the divergent magnetic field, multiple accelerated ion populations are observed through laser induced fluorescence measurements of the ion velocity distribution function. The formation of the multiple double layer structure is a strong function of the neutral gas pressure in the experiment. The similarity of the accelerated ion populations observed in these laboratory experiments to ion populations observed in reconnection outflow regions in the magnetosphere and in numerical simulations is also described. If ion energization during magnetic reconnection also results solely from acceleration in electric fields, these observations imply a prediction that the ion heating, i.e., the broadening of ion velocity distribution functions, reported in magnetic reconnection experiments is more accurately described by a superposition of differently accelerated ion populations. Therefore, the ion gheatingh rate during reconnection should scale as the square root of the cube of the charge per unit mass (q3/m)1/2 for ions with varying charge-to-mass ratios. A new RFEA probe was benchmarked on the low pressure CFDL plasmas produced in WVU HELIX-LEIA. This work was the result of collaboration between the University of Tromso (UiT) and WVU. LIF was used to confirm the RFEAs ability to detect a beam when one was present. The RFEA was also able to detect the presence of a beam when LIF techniques were limited by metastable quenching. The probefs limitations in dealing with ion focusing are discussed as well.

Ultrafast measurements of chlorine dioxide photochemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ludowise, P.D.

Time-resolved mass spectrometry and time-resolved photoelectron spectroscopy are used to study the ultrafast photodissociation dynamics of chlorine dioxide, an important constituent in stratospheric ozone depletion. Chapter 1 introduces these pump/probe techniques, in which a femtosecond pump pulse excites a molecule to a dissociative state. At a later time, a second femtosecond probe pulse ionizes the molecule. The resulting mass and photoelectron spectra are acquired as a function of the delay between the pump and probe pulses, which follows the evolution of the molecule on the excited state. A comparison to other techniques used to study reaction dynamics is discussed. Chaptermore » 2 includes a detailed description of the design and construction of the experimental apparatus, which consists of a femtosecond laser system, a molecular beam time-of-flight spectrometer, and a data acquisition system. The time-of-flight spectrometer is specifically designed to have a short flight distance to maximize the photoelectron collection efficiency without degrading the resolution, which is limited by the bandwidth of the femtosecond laser system. Typical performance of the apparatus is demonstrated in a study of the time-resolved photoelectron spectroscopy of nitric oxide. The results of the time-resolved mass spectrometry experiments of chlorine dioxide are presented in Chapter 3. Upon excitation to the A {sup 2}A{sub 2} state near 3.2 eV, the molecule dissociates through an indirect two-step mechanism. The direct dissociation channel has been predicted to be open, but is not observed. A quantum beat is observed in the OClO{sup +} species, which is described as a vibrational coherence of the optically prepared A {sup 2}A{sub 2} state. Chapter 4 presents the results of the time-resolved photoelectron experiments of chlorine dioxide. At short delay time, the quantum beat of the OClO{sup +} species is observed in the X {sup 1}A{sub 1} state of the ion. At infinite delay, the signal is dominated by the ClO{sup +} ion, observed in a variety of electronic states. The photoelectron data is shown to support the indirect two-step dissociation mechanism derived from the mass results. Conclusions of the mass and photoelectron results are discussed in context of the stratospheric ozone depletion problem.« less

Time-dependent, x-ray spectral unfolds and brightness temperatures for intense Li{sup +} ion beam-driven hohlraums

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fehl, D.L.; Chandler, G.A.; Biggs, F.

X-ray-producing hohlraums are being studied as indirect drives for Inertial Confinement Fusion targets. In a 1994 target series on the PBFAII accelerator, cylindrical hohlraum targets were heated by an intense Li{sup +} ion beam and viewed by an array of 13 time-resolved, filtered x-ray detectors (XRDs). The UFO unfold code and its suite of auxiliary functions were used extensively in obtaining time- resolved x-ray spectra and radiation temperatures from this diagnostic. UFO was also used to obtain fitted response functions from calibration data, to simulate data from blackbody x-ray spectra of interest, to determine the suitability of various unfolding parametersmore » (e.g., energy domain, energy partition, smoothing conditions, and basis functions), to interpolate the XRD signal traces, and to unfold experimental data. The simulation capabilities of the code were useful in understanding an anomalous feature in the unfolded spectra at low photon energies ({le} 100 eV). Uncertainties in the differential and energy-integrated unfolded spectra were estimated from uncertainties in the data. The time-history of the radiation temperature agreed well with independent calculations of the wall temperature in the hohlraum.« less

Ion Dynamics of a BHT-600 Hall Thruster Measured with Time-Resolved Laser-Induced Fluorescence

DTIC Science & Technology

2016-01-14

LIF  Method V = 0 V V λ = λ0 λ > λ0 λ < λ0 Ion Velocity from  Doppler Shift: 0 5 10 15 20 25 30 0 0.1 0.2 0.3 0.4...0.5 0.6 0.7 0.8 0.9 1 Frequency (GHz) N o r m a l i z e d S i g n a l xneg28z6_AVG OG LIF OG Fit LIF Fit AFRL | BHT‐600 TRLIF | Jan 14, 2016 10...Distribution A: Approved for Public Release; Distribution Unlimited. PA# 16204 Time‐Resolved  LIF  Method Laser  Tapered Amp  D1  BS1  BS2  D2  O G C  

Transient alkylaminium radicals in n-hexane. Condensed-phase ion-molecule reactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Werst, D.W.; Trifunac, A.D.

Time-resolved fluorescence detected magnetic resonance (FDMR) is used to observe alkylaminium radicals formed in n-hexane solutions by electron pulse radiolysis. The ease of observation of aminium radical FDMR signals increases with increasing alkyl substitution of the amine solutes. The results are discussed in terms of the ion-molecule reactions, such as proton transfer, which compete with the electron-transfer processes, i.e, the electron transfer from solute molecules to n-hexane radical cations and geminate recombination.

Recent High-Intensity Experiments at the Trident Laser

NASA Astrophysics Data System (ADS)

Cobble, James; Palaniyappan, Sasikumar; Gautier, Cort; Kim, Yongho; Huang, Chengkun

2014-10-01

With near-diffraction-limited irradiance of 2 × 1020 W/cm2 on target and prelase contrast better than 10-8, we have accessed the regime of relativistic transparency (RT) at the Trident Laser. The goal was to assess electron debris emitted from the target rear surface with phase-contrast imaging (PCI) and current density measurements (hence, the total electron current). Companion diagnostics show whether the experiments are in the target-normal-sheath-acceleration mode or in the RT regime. The superb laser contrast allows us to shoot targets as thin as 50 nm. PCI at 527 nm is temporally resolved to 600 fs. It has shown the evolution of electron behavior over tens of ps, including thermal electrons accompanying the ion jet, accelerated to many tens of MeV earlier in time. Faraday-cup measurements indicate the transfer of many microC of charge during the laser drive. As a ride-along experiment using a gas Cherenkov detector (GCD), we have detected gamma rays of energy >5 MeV. This radiation has a prompt component and a lesser source, driven by accelerated ions, that is time resolved by the GCD. The ion time of flight is compared to Thomson parabola data. Electron energy spectra are also collected. This work is supported by US DOE/NNSA, performed at LANL, operated by LANS LLC under Contract DE-AC52-06NA25396.

Relativistic Transparency Experiments at the Trident Laser

NASA Astrophysics Data System (ADS)

Cobble, J. A.; Palaniyappan, S.; Gautier, D. C.; Kim, Y. H.; Clark, D. D.; Johnson, R. P.; Shimada, T.; Fernandez, J. C.; Herrmann, H. W.

2013-10-01

With near-diffraction-limited irradiance of 3 × 1020 W/cm2 on target and prelase contrast better than 10-9, we have accessed the regime of relativistic transparency (RT) at the Trident Laser. The goal was to assess electron debris emitted from the target rear surface with phase-contrast imaging (PCI) and current density measurements (hence, the total electron current). Companion diagnostics show whether the experiments are in the target-normal-sheath-acceleration mode or in the RT regime. The superb laser contrast allows us to shoot targets as thin as 50 nm. PCI at 527 nm is temporally resolved to 600 fs. It has shown the evolution of electron behavior over tens of ps, including thermal electrons accompanying the ion jet, accelerated to many tens of MeV earlier in time. Faraday-cup measurements indicate the transfer of many uC of charge during the laser drive. As a ride-along experiment using a gas Cherenkov detector (GCD), we have detected gamma rays of energy >5 MeV. This radiation has a prompt component and a lesser source, driven by accelerated ions, that is time resolved by the GCD. The ion time of flight is compared to Thomson parabola data. Electron energy spectra are also collected. This work has been performed under the auspices of the US DOE contract number DE-AC52-06NA25396.

Imaging and Rapid-Scanning Ion Mass Spectrometer (IRM) for the CASSIOPE e-POP Mission

NASA Astrophysics Data System (ADS)

Yau, Andrew W.; Howarth, Andrew; White, Andrew; Enno, Greg; Amerl, Peter

2015-06-01

The imaging and rapid-scanning ion mass spectrometer (IRM) is part of the Enhanced Polar Outflow Probe (e-POP) instrument suite on the Canadian CASSIOPE small satellite. Designed to measure the composition and detailed velocity distributions of ions in the ˜1-100 eV/q range on a non-spinning spacecraft, the IRM sensor consists of a planar entrance aperture, a pair of electrostatic deflectors, a time-of-flight (TOF) gate, a hemispherical electrostatic analyzer, and a micro-channel plate (MCP) detector. The TOF gate measures the transit time of each detected ion inside the sensor. The hemispherical analyzer disperses incident ions by their energy-per-charge and azimuth in the aperture plane onto the detector. The two electrostatic deflectors may be optionally programmed to step through a sequence of deflector voltages, to deflect ions of different incident elevation out of the aperture plane and energy-per-charge into the sensor aperture for sampling. The position and time of arrival of each detected ion at the detector are measured, to produce an image of 2-dimensional (2D), mass-resolved ion velocity distribution up to 100 times per second, or to construct a composite 3D velocity distribution by combining successive images in a deflector voltage sequence. The measured distributions are then used to investigate ion composition, density, drift velocity and temperature in polar ion outflows and related acceleration and transport processes in the topside ionosphere.

Vibrational stark effects to identify ion pairing and determine reduction potentials in electrolyte-free environments

DOE PAGES

Mani, Tomoyasu; Grills, David C.; Miller, John R.

2015-01-02

A recently-developed instrument for time-resolved infrared detection following pulse radiolysis has been used to measure the ν(C≡N) IR band of the radical anion of a CN-substituted fluorene in tetrahydrofuran. Specific vibrational frequencies can exhibit distinct frequency shifts due to ion-pairing, which can be explained in the framework of the vibrational Stark effect. Measurements of the ratio of free ions and ion-pairs in different electrolyte concentrations allowed us to obtain an association constant and free energy change for ion-pairing. As a result, this new method has the potential to probe the geometry of ion-pairing and allows the reduction potentials of moleculesmore » to be determined in the absence of electrolyte in an environment of low dielectric constant.« less

Hybrid model for simulation of plasma jet injection in tokamak

NASA Astrophysics Data System (ADS)

Galkin, Sergei A.; Bogatu, I. N.

2016-10-01

Hybrid kinetic model of plasma treats the ions as kinetic particles and the electrons as charge neutralizing massless fluid. The model is essentially applicable when most of the energy is concentrated in the ions rather than in the electrons, i.e. it is well suited for the high-density hyper-velocity C60 plasma jet. The hybrid model separates the slower ion time scale from the faster electron time scale, which becomes disregardable. That is why hybrid codes consistently outperform the traditional PIC codes in computational efficiency, still resolving kinetic ions effects. We discuss 2D hybrid model and code with exact energy conservation numerical algorithm and present some results of its application to simulation of C60 plasma jet penetration through tokamak-like magnetic barrier. We also examine the 3D model/code extension and its possible applications to tokamak and ionospheric plasmas. The work is supported in part by US DOE DE-SC0015776 Grant.

Photoionization and ion cyclotron resonance studies of the ion chemistry of ethylene oxide

NASA Technical Reports Server (NTRS)

Corderman, R. R.; Williamson, A. D.; Lebreton, P. R.; Buttrill, S. E., Jr.; Beauchamp, J. L.

1976-01-01

The formation of the ethylene oxide molecular ion and its subsequent ion-molecule reactions leading to the products C2H5O(+) and C3H5O(+) have been studied using time-resolved photoionization mass spectroscopy, ion cyclotron resonance spectroscopy, and photoelectron spectroscopy. An examination of the effects of internal energy on reactivity shows that the ratio of C3H5O(+) to C2H5O(+) increases by an order of magnitude with a single quantum of vibrational energy. The formation of (C2H4O/+/)-asterisk in a collision-induced isomerization is found which yields a ring-opened structure by C-C bond cleavage. The relaxed ring-opened C2H4O(+) ion reacts with neutral ethylene oxide by CH2(+) transfer to yield an intermediate product ion C3H6O(+) which gives C3H5O(+) by loss of H.

Wide-band, time-resolved photoacoustic study of electron-transfer reactions. Photoexcited magnesium porphyrin and quinones

DOE Office of Scientific and Technical Information (OSTI.GOV)

Feitelson, J.; Mauzerall, D.C.

1993-08-12

Wide-band, time-resolved, pulsed photoacoustics has been employed to study the electron-transfer reaction between a triplet magnesium porphyrin and various quinones in polar and nonpolar solvents. The reaction rate constants are near encounter limited. The yield of triplet state is 70% in both solvents. The yield of ions is 85% in the former and zero in the latter, in agreement with spin dephasing time and escape times from the Coulomb wells in the two solvents. In methanol the plot of measured heat output versus quinone redox potential is linear. This implies that the entropy of electron transfer is constant through themore » series, but it may not be negligible. 16 refs., 2 figs., 1 tab.« less

Ion mass spectrometry investigations of the discharge during reactive high power pulsed and direct current magnetron sputtering of carbon in Ar and Ar/N{sub 2}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schmidt, S.; Greczynski, G.; Jensen, J.

2012-07-01

Ion mass spectrometry was used to investigate discharges formed during high power impulse magnetron sputtering (HiPIMS) and direct current magnetron sputtering (DCMS) of a graphite target in Ar and Ar/N{sub 2} ambient. Ion energy distribution functions (IEDFs) were recorded in time-averaged and time-resolved mode for Ar{sup +}, C{sup +}, N{sub 2}{sup +}, N{sup +}, and C{sub x}N{sub y}{sup +} ions. An increase of N{sub 2} in the sputter gas (keeping the deposition pressure, pulse width, pulse frequency, and pulse energy constant) results for the HiPIMS discharge in a significant increase in C{sup +}, N{sup +}, and CN{sup +} ion energies.more » Ar{sup +}, N{sub 2}{sup +}, and C{sub 2}N{sup +} ion energies, in turn, did not considerably vary with the changes in working gas composition. The HiPIMS process showed higher ion energies and fluxes, particularly for C{sup +} ions, compared to DCMS. The time evolution of the plasma species was analyzed for HiPIMS and revealed the sequential arrival of working gas ions, ions ejected from the target, and later during the pulse-on time molecular ions, in particular CN{sup +} and C{sub 2}N{sup +}. The formation of fullerene-like structured CN{sub x} thin films for both modes of magnetron sputtering is explained by ion mass-spectrometry results and demonstrated by transmission electron microscopy as well as diffraction.« less

Electron spin dynamics and optical orientation of Mn2+ ions in GaAs

NASA Astrophysics Data System (ADS)

Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Sapega, V. F.; Yakovlev, D. R.; Bayer, M.

2013-04-01

We present an overview of spin-related phenomena in GaAs doped with low concentration of Mn-acceptors (below 1018 cm-3). We use the combination of different experimental techniques such as spin-flip Raman scattering and time-resolved photoluminescence. This allows to evaluate the time evolution of both electron and Mn spins. We show that optical orientation of Mn ions is possible under application of weak magnetic field, which is required to suppress the manganese spin relaxation. The optically oriented Mn2+ ions maintain the spin and return part of the polarization back to the electron spin system providing a long-lived electron spin memory. This leads to a bunch of spectacular effects such as non-exponential electron spin decay and spin precession in the effective exchange fields.

First spatial separation of a heavy ion isomeric beam with a multiple-reflection time-of-flight mass spectrometer

NASA Astrophysics Data System (ADS)

Dickel, T.; Plaß, W. R.; Ayet San Andres, S.; Ebert, J.; Geissel, H.; Haettner, E.; Hornung, C.; Miskun, I.; Pietri, S.; Purushothaman, S.; Reiter, M. P.; Rink, A.-K.; Scheidenberger, C.; Weick, H.; Dendooven, P.; Diwisch, M.; Greiner, F.; Heiße, F.; Knöbel, R.; Lippert, W.; Moore, I. D.; Pohjalainen, I.; Prochazka, A.; Ranjan, M.; Takechi, M.; Winfield, J. S.; Xu, X.

2015-05-01

211Po ions in the ground and isomeric states were produced via 238U projectile fragmentation at 1000 MeV/u. The 211Po ions were spatially separated in flight from the primary beam and other reaction products by the fragment separator FRS. The ions were energy-bunched, slowed-down and thermalized in a gas-filled cryogenic stopping cell (CSC). They were then extracted from the CSC and injected into a high-resolution multiple-reflection time-of-flight mass spectrometer (MR-TOF-MS). The excitation energy of the isomer and, for the first time, the isomeric-to-ground state ratio were determined from the measured mass spectrum. In the subsequent experimental step, the isomers were spatially separated from the ions in the ground state by an ion deflector and finally collected with a silicon detector for decay spectroscopy. This pioneering experimental result opens up unique perspectives for isomer-resolved studies. With this versatile experimental method new isomers with half-lives longer than a few milliseconds can be discovered and their decay properties can be measured with highest sensitivity and selectivity. These experiments can be extended to studies with isomeric beams in nuclear reactions.

Calibration of an advanced neutral particle analyzer for the Madison Symmetric Torus reversed-field pinch

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reusch, J. A.; Anderson, J. K.; Eilerman, S.

2012-10-15

A new E Parallel-To B neutral particle analyzer, which has recently been installed on Madison Symmetric Torus (MST) reversed-field pinch (RFP), has now been calibrated, allowing the measurement of the fast ion density and energy distribution. This diagnostic, dubbed the advanced neutral particle analyzer (ANPA), can simultaneously produce time resolved measurements of the efflux of both hydrogen and deuterium ions from the plasma over a 35 keV energy range with an energy resolution of 2-4 keV and a time resolution of 10 {mu}s. These capabilities are needed to measure both majority ion heating that occurs during magnetic reconnection events inmore » MST and the behavior of the fast ions from the 1 MW hydrogen neutral beam injector on MST. Calibration of the ANPA was performed using a custom ion source that resides in the flight tube between the MST and the ANPA. In this work, the ANPA will be described, the calibration procedure and results will be discussed, and initial measurements of the time evolution of 25 keV neutral beam injection-born fast ions will be presented.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Laskin, Julia

In this work, resonant ejection coupled with surface-induced dissociation (SID) in a Fourier transform ion cyclotron resonance mass spectrometer is used to examine fragmentation kinetics of two singly protonated hexapeptides, RYGGFL and KYGGFL, containing the basic arginine residue and less basic lysine residue at the N-terminus. The kinetics of individual reaction channels at different collision energies are probed by applying a short ejection pulse (1 ms) in resonance with the cyclotron frequency of a selected fragment ion and varying the delay time between ion-surface collision and resonant ejection while keeping total reaction delay time constant. Rice-Ramsperger-Kassel-Marcus (RRKM) modeling of themore » experimental data provides accurate threshold energies and activation entropies of individual reaction channels. Substitution of arginine with less basic lysine has a pronounced effect on the observed fragmentation kinetics of several pathways, including the b2 ion formation, but has little or no effect on formation of the b5+H2O fragment ion. The combination of resonant ejection SID, time- and collision energy-resolved SID, and RRKM modeling of both types of experimental data provides a detailed mechanistic understanding of the primary dissociation pathways of complex gaseous ions.« less

Mean carrier transport properties and charge collection dynamics of single-crystal, natural type IIa diamonds from ion-induced conductivity measurements

DOE Office of Scientific and Technical Information (OSTI.GOV)

Han, Sung Su

1993-09-01

Ion-induced conductivity has been used to investigate the detector characteristics of diamond detectors. Both integrated-charge, and time-resolved current measurements were performed to examine the mean carrier transport properties of diamond and the dynamics of charge collection under highly-localized and high-density excitation conditions. The integrated-charge measurements were conducted with a standard pulse-counting system with 241Am radioactivity as the excitation source for the detectors. The time-resolved current measurements were performed using a 70 GHz random sampling oscilloscope with the detectors incorporated into high-speed microstrip transmission lines and the excitation source for these measurements was an ion beam of either 5-MeV He +more » or 10-MeV Si 3+. The detectors used in both experiments can be described as metal-semiconductor-metal (MSM) devices where a volume of the detector material is sandwiched between two metal plates. A charge collection model was developed to interpret the integrated-charge measurements which enabled estimation of the energy required to produce an electron-hole pair (ϵ di) and the mean carrier transport properties in diamond, such as carrier mobility and lifetime, and the behavior of the electrical contacts to diamond.« less

Nanopipette exploring nanoworld.

PubMed

Takami, Tomohide; Park, Bae Ho; Kawai, Tomoji

2014-01-01

Nanopipettes, with tip orifices on the order of tens to hundreds of nanometers, have been utilized in the fields of analytical chemistry and nanophysiology. Nanopipettes make nanofabrication possible at liquid/solid interfaces. Moreover, they are utilized in time-resolved measurements and for imaging biological materials, e.g. , living cells, by using techniques such as scanning ion-conductance microscopy and scanning electrochemical microscopy. We have successfully fabricated ion-selective nanopipettes that can be used to identify targeted ions such as sodium and potassium in- and outside of living cells. In this review, we discuss the extent of utilization of nanopipettes in investigating the nanoworld. In addition, we discuss the potential applications of future nanopipettes.

Nanopipette exploring nanoworld

NASA Astrophysics Data System (ADS)

Takami, Tomohide; Park, Bae Ho; Kawai, Tomoji

2014-04-01

Nanopipettes, with tip orifices on the order of tens to hundreds of nanometers, have been utilized in the fields of analytical chemistry and nanophysiology. Nanopipettes make nanofabrication possible at liquid/solid interfaces. Moreover, they are utilized in time-resolved measurements and for imaging biological materials, e.g., living cells, by using techniques such as scanning ion-conductance microscopy and scanning electrochemical microscopy. We have successfully fabricated ion-selective nanopipettes that can be used to identify targeted ions such as sodium and potassium in- and outside of living cells. In this review, we discuss the extent of utilization of nanopipettes in investigating the nanoworld. In addition, we discuss the potential applications of future nanopipettes.

Experimental Observation of the Effects of Translational and Rotational Electrode Misalignment on a Planar Linear Ion Trap Mass Spectrometer

NASA Astrophysics Data System (ADS)

Tian, Yuan; Decker, Trevor K.; McClellan, Joshua S.; Wu, Qinghao; De la Cruz, Abraham; Hawkins, Aaron R.; Austin, Daniel E.

2018-04-01

The performance of miniaturized ion trap mass analyzers is limited, in part, by the accuracy with which electrodes can be fabricated and positioned relative to each other. Alignment of plates in a two-plate planar LIT is ideal to characterize misalignment effects, as it represents the simplest possible case, having only six degrees of freedom (DOF) (three translational and three rotational). High-precision motorized actuators were used to vary the alignment between the two ion trap plates in five DOFs—x, y, z, pitch, and yaw. A comparison between the experiment and previous simulations shows reasonable agreement. Pitch, or the degree to which the plates are parallel along the axial direction, has the largest and sharpest impact to resolving power, with resolving power dropping noticeably with pitch misalignment of a fraction of a degree. Lateral displacement (x) and yaw (rotation of one plate, but plates remain parallel) both have a strong impact on ion ejection efficiency, but little effect on resolving power. The effects of plate spacing (y-displacement) on both resolving power and ion ejection efficiency are attributable to higher-order terms in the trapping field. Varying the DC (axial) trapping potential can elucidate the effects where more misalignments in more than one DOF affect performance. Implications of these results for miniaturized ion traps are discussed. [Figure not available: see fulltext.

Characterization of high energy Xe ion irradiation effects in single crystal molybdenum with depth-resolved synchrotron microbeam diffraction

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yun, Di; Miao, Yinbin; Xu, Ruqing

2016-04-01

Microbeam X-ray diffraction experiments were conducted at beam line 34-ID of the Advanced Photon Source (APS) on fission fragment energy Xe heavy ion irradiated single crystal Molybdenum (Mo). Lattice strain measurements were obtained with a depth resolution of 0.7 mu m, which is critical in resolving the peculiar heterogeneity of irradiation damage associated with heavy ion irradiation. Q-space diffraction peak shift measurements were correlated with lattice strain induced by the ion irradiations. Transmission electron microscopy (TEM) characterizations were performed on the as-irradiated materials as well. Nanometer sized Xe bubble microstructures were observed via TEM. Molecular Dynamics (MD) simulations were performedmore » to help interpret the lattice strain measurement results from the experiment. This study showed that the irradiation effects by fission fragment energy Xe ion irradiations can be collaboratively understood with the depth resolved X-ray diffraction and TEM measurements under the assistance of MD simulations. (c) 2015 Elsevier B.V. All rights reserved.« less

Insight into the time-resolved extraction of aroma compounds during espresso coffee preparation: online monitoring by PTR-ToF-MS.

PubMed

Sánchez-López, José A; Zimmermann, Ralf; Yeretzian, Chahan

2014-12-02

Using proton-transfer-reaction time-of-flight mass-spectrometry (PTR-ToF-MS), we investigated the extraction dynamic of 95 ion traces in real time (time resolution = 1 s) during espresso coffee preparation. Fifty-two of these ions were tentatively identified. This was achieved by online sampling of the volatile organic compounds (VOCs) in close vicinity to the coffee flow, at the exit of the extraction hose of the espresso machine (single serve capsules). Ten replicates of six different single serve coffee types were extracted to a final weight between 20-120 g, according to the recommended cup size of the respective coffee capsule (Ristretto, Espresso, and Lungo), and analyzed. The results revealed considerable differences in the extraction kinetics between compounds, which led to a fast evolution of the volatile profiles in the extract flow and consequently to an evolution of the final aroma balance in the cup. Besides exploring the time-resolved extraction dynamics of VOCs, the dynamic data also allowed the coffees types (capsules) to be distinguished from one another. Both hierarchical cluster analysis (HCA) and principal component analysis (PCA) showed full separation between the coffees types. The methodology developed provides a fast and simple means of studying the extraction dynamics of VOCs and differentiating between different coffee types.

High Time-Resolved Kinetic Temperatures of Solar Wind Minor Ions Measured with SOHO/CELIAS/CTOF

NASA Astrophysics Data System (ADS)

Janitzek, N. P.; Berger, L.; Drews, C.; Wimmer-Schweingruber, R. F.

2017-12-01

Solar wind heavy ions with an atomic number Z > 2 are referred to as minor ions since they represent a fraction of less than one percent of all solar wind ions. They can be therefore regarded as test particles, only reacting to but not driving the dynamics of the solar wind plasma, which makes them a unique diagnostic tool for plasma wave phenomena both in the solar atmosphere and the extended heliosphere. In the past, several studies have investigated the kinetic temperatures of minor ions, but due to low counting statistics these studies are based on ion velocity distribution functions (VDFs) recorded over time periods of several hours. The Charge Time-Of-Flight (CTOF) mass spectrometer as part of the Charge, ELement and Isotope Analysis System (CELIAS) onboard the SOlar and Heliospheric Observatory (SOHO) provides solar wind heavy ion 1D radial VDFs with excellent charge state separation, an unprecedented cadence of 5 minutes and very high counting statistics, exceeding similar state-of-the-art instruments by a factor of ten. In our study, based on CTOF measurements at Langrangian point L1 between DOY 150 and DOY 220 in 1996, we investigate systematically the influence of the VDF time resolution on the derived kinetic temperatures for solar wind silicon and iron ions. The selected ion set spans a wide range of mass-per-charge from 3 amu/e < m/q < 8 amu/e. Therefore, it is suitable for the search of signatures of gyrofrequency-dependent heating processes resulting from the resonant interaction of heavy ions with ion-cyclotron waves.

Mass-resolved ion energy measurements at both electrodes of a 13.56 MHz plasma in CF4

NASA Astrophysics Data System (ADS)

Snijkers, R. J. M. M.; van Sambeek, M. J. M.; Hoppenbrouwers, M. B.; Kroesen, G. M. W.; de Hoog, F. J.

1996-06-01

The ion energy distributions (IEDs) at the electrodes in a capacitively coupled 13.56 MHz plasma in CF4 have been measured mass resolved with a Balzers quadrupole in combination with a home-built energy analyzer. Mass-resolved determination offers the possibility to compare the IED of different ions achieved in the same sheath. The IEDs have been determined at both the largest and the smallest electrode. Apart from the IEDs of the CF4 species, the IEDs of ionic species in plasmas in argon and nitrogen also were determined. Apart from the CF4 ionic species CF+3, CF+2, CF+, and F+, CHF+2 ions also are present in the CF4 plasma due to residual water in the reactor. Because the CHF+2 ions are not produced in the sheath and because we do not detect elastically scattered ions, the IEDs of these ions show the typical bimodal distribution for rf plasmas which corresponds to an IED of ions which have not collided in the sheath. From these IEDs we can obtain the sheath characteristics, such as the averaged sheath potential. From the IEDs of CF+n ions one can conclude that, in the sheath of the CF4 plasma, a large number of chemical reactions takes place between the CF+n ions and the neutrals.

The influence of surface contamination on the ion emission from nanosecond-pulsed laser ablation of Al and Cu

NASA Astrophysics Data System (ADS)

Ullah, S.; Dogar, A. H.; Qayyum, H.; Rehman, Z. U.; Qayyum, A.

2018-04-01

Ions emitted from planar Al and Cu targets irradiated with a 1064 nm pulsed laser were investigated with the help of a time-resolving Langmuir probe. It was found that the intensity of the ions emitted from a target area rapidly decreases with the increasing number of laser shots, and seems to reach saturation after about 10 laser shots. The saturated intensity of Al and Cu ions was approximately 0.1 and 0.3 times the intensity of the respective ions measured at the first laser shot, respectively. The higher target ion intensity for the first few shots is thought to be due to the enhanced ionization of target atoms by vacuum-ultraviolet radiations emitted from the thermally excited/ionized surface contaminants. The reduction of target ion intensity with an increasing number of laser shots thus indicates the removal of contaminants from the irradiated surface area. Laser-cleaned Al and Cu surfaces were then allowed to be recontaminated with residual vacuum gases and the ion intensity was measured at various time delays. The prolonged exposure of the cleaned target to vacuum residual gases completely restores the ion intensity. Regarding surface contaminants removal, laser shots of higher intensities were found to be more effective than a higher number of laser shots having lower intensities.

Applications of time-resolved laser fluorescence spectroscopy to the environmental biogeochemistry of actinides.

PubMed

Collins, Richard N; Saito, Takumi; Aoyagi, Noboru; Payne, Timothy E; Kimura, Takaumi; Waite, T David

2011-01-01

Time-resolved laser fluorescence spectroscopy (TRLFS) is a useful means of identifying certain actinide species resulting from various biogeochemical processes. In general, TRLFS differentiates chemical species of a fluorescent metal ion through analysis of different excitation and emission spectra and decay lifetimes. Although this spectroscopic technique has largely been applied to the analysis of actinide and lanthanide ions having fluorescence decay lifetimes on the order of microseconds, such as UO , Cm, and Eu, continuing development of ultra-fast and cryogenic TRLFS systems offers the possibility to obtain speciation information on metal ions having room-temperature fluorescence decay lifetimes on the order of nanoseconds to picoseconds. The main advantage of TRLFS over other advanced spectroscopic techniques is the ability to determine in situ metal speciation at environmentally relevant micromolar to picomolar concentrations. In the context of environmental biogeochemistry, TRLFS has principally been applied to studies of (i) metal speciation in aqueous and solid phases and (ii) the coordination environment of metal ions sorbed to mineral and bacterial surfaces. In this review, the principles of TRLFS are described, and the literature reporting the application of this methodology to the speciation of actinides in systems of biogeochemical interest is assessed. Significant developments in TRLFS methodology and advanced data analysis are highlighted, and we outline how these developments have the potential to further our mechanistic understanding of actinide biogeochemistry. American Society of Agronomy, Crop Science Society of America, and Soil Science Society of America.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bailey, J.E.; Adams, R.; Carlson, A.L.

Stark-shift measurements using emission spectroscopy are a powerful tool for advancing understanding in many plasma physics experiments. The authors use simultaneous 2-D-spatial and time-resolved spectra to study the electric field evolution in the 20 TW Particle Beam Fusion Accelerator II ion diode acceleration gap. Fiber optic arrays transport light from the gap to remote streaked spectrographs operated in a multiplexed mode that enables recording time-resolved spectra from eight spatial locations on a single instrument. Design optimization and characterization measurements of the multiplexed spectrograph properties include the astigmatism, resolution, dispersion variation, and sensitivity. A semi-automated line-fitting procedure determines the Stark shiftmore » and the related uncertainties. Fields up to 10 MV/cm are measured with an accuracy {+-}2--4%. Detailed tests of the fitting procedure confirm that the wavelength shift uncertainties are accurate to better than {+-}20%. Development of an active spectroscopy probe technique that uses laser-induced fluorescence from an injected atomic beam to obtain 3-D space- and time-resolved measurements of the electric and magnetic fields is in progress.« less

Ion manipulations in structures for lossless ion manipulations (SLIM): computational evaluation of a 90° turn and a switch

DOE PAGES

Garimella, Sandilya V. B.; Ibrahim, Yehia. M.; Webb, Ian K.; ...

2015-08-19

The process of redirecting ions through 90° turns and ‘tee’ switches utilizing Structures for Lossless Ion Manipulations (SLIM) was evaluated using theoretical and simulation methods at 4 Torr pressure. SIMION simulations were used to optimize and evaluate conditions for performing turns without loss of signal intensity or ion mobility resolving power. Fundamental considerations indicated that the “race track” effect during ion turns may incur only small losses to the ion mobility resolving power at 4 Torr pressure for the typical plume widths predicted in an optimized SLIM ‘tee’ switch design. The dynamic switching of ions into orthogonal channels was alsomore » evaluated using SIMION ion trajectory simulations, and achieved similar performance. Simulation results were in close agreement with experimental results and were used to refine SLIM designs and applied potentials for their use.« less

Laser-driven atomic-probe-beam diagnostics

NASA Astrophysics Data System (ADS)

Knyazev, B. A.; Greenly, J. B.; Hammer, D. A.

2000-12-01

A new laser-driven atomic-probe-beam diagnostic (LAD) is proposed for local, time-resolved measurements of electric field and ion dynamics in the accelerating gap of intense ion beam diodes. LAD adds new features to previous Stark-shift diagnostics which have been progressively developed in several laboratories, from passive observation of Stark effect on ion species or fast (charge-exchanged) neutrals present naturally in diodes, to active Stark atomic spectroscopy (ASAS) in which selected probe atoms were injected into the gap and excited to suitable states by resonant laser radiation. The LAD scheme is a further enhancement of ASAS in which the probe atoms are also used as a local (laser-ionized) ion source at an instant of time. Analysis of the ion energy and angular distribution after leaving the gap enables measurement, at the chosen ionization location in the gap, of both electrostatic potential and the development of ion divergence. Calculations show that all of these quantities can be measured with sub-mm and ns resolution. Using lithium or sodium probe atoms, fields from 0.1 to 10 MV/cm can be measured.

Extrinsic ion migration in perovskite solar cells

DOE PAGES

Li, Zhen; Xiao, Chuanxiao; Yang, Ye; ...

2017-04-10

In this study, the migration of intrinsic ions (e.g., MA +, Pb 2+, I –) in organic–inorganic hybrid perovskites has received significant attention with respect to the critical roles of these ions in the hysteresis and degradation in perovskite solar cells (PSCs). Here, we demonstrate that extrinsic ions (e.g., Li +, H +, Na +), when used in the contact layers in PSCs, can migrate across the perovskite layer and strongly impact PSC operation. In a TiO 2/perovskite/spiro-OMeTAD-based PSC, Li +-ion migration from spiro-OMeTAD to the perovskite and TiO 2 layer is illustrated by time-of-flight secondary-ion mass spectrometry. The movementmore » of Li + ions in PSCs plays an important role in modulating the solar cell performance, tuning TiO 2 carrier-extraction properties, and affecting hysteresis in PSCs. The influence of Li +-ion migration was investigated using time-resolved photoluminescence, Kelvin probe force microscopy, and external quantum efficiency spectra. Other extrinsic ions such as H + and Na + also show a clear impact on the performance and hysteresis in PSCs. Understanding the impacts of extrinsic ions in perovskite-based devices could lead to new material and device designs to further advance perovskite technology for various applications.« less

Characteristics of Ions Emission from Ultrashort Laser Produced Plasma

PubMed Central

Elsied, Ahmed M.; Termini, Nicholas C.; Diwakar, Prasoon K.; Hassanein, Ahmed

2016-01-01

The dynamic characteristics of the ions emitted from ultrashort laser interaction with materials were studied. A series of successive experiments were conducted for six different elements (C, Al, Cu, Mo, Gd, and W) using 40 fs, 800 nm Ti: Sapphire laser. Time-of-flight (TOF) ion profile was analyzed and charge emission dependencies were investigated. The effects of incident laser interaction with each element were studied over a wide range of laser fluences (0.8 J/cm2 to 24 J/cm2) corresponding to laser intensities (2.0 × 1013 W/cm2 to 6.0 × 1014 W/cm2). The dependencies of the angular resolved ion flux and energy were also investigated. The TOF ion profile exhibits two peaks corresponding to a fast and a slow ion regime. The slow ions emission was the result of thermal vaporization while fast ions emission was due to time dependent ambipolar electric field. A theoretical model is proposed to predict the total ion flux emitted during femtosecond laser interaction that depends on laser parameters, material properties, and plume hydrodynamics. Incident laser fluence directly impacts average charge state and in turn affects the ion flux. Slow ions velocity exhibited different behavior from fast ions velocity. The fast ions energy and flux were found to be more collimated. PMID:27905553

Influence of nitrogen admixture to argon on the ion energy distribution in reactive high power pulsed magnetron sputtering of chromium

NASA Astrophysics Data System (ADS)

Breilmann, W.; Maszl, C.; Hecimovic, A.; von Keudell, A.

2017-04-01

Reactive high power impulse magnetron sputtering (HiPIMS) of metals is of paramount importance for the deposition of various oxides, nitrides and carbides. The addition of a reactive gas such as nitrogen to an argon HiPIMS plasma with a metal target allows the formation of the corresponding metal nitride on the substrate. The addition of a reactive gas introduces new dynamics into the plasma process, such as hysteresis, target poisoning and the rarefaction of two different plasma gases. We investigate the dynamics for the deposition of chromium nitride by a reactive HiPIMS plasma using energy- and time-resolved ion mass spectrometry, fast camera measurements and temporal and spatially resolved optical emission spectroscopy. It is shown that the addition of nitrogen to the argon plasma gas significantly changes the appearance of the localized ionization zones, the so-called spokes, in HiPIMS plasmas. In addition, a very strong modulation of the metal ion flux within each HiPIMS pulse is observed, with the metal ion flux being strongly suppressed and the nitrogen molecular ion flux being strongly enhanced in the high current phase of the pulse. This behavior is explained by a stronger return effect of the sputtered metal ions in the dense plasma above the racetrack. This is best observed in a pure nitrogen plasma, because the ionization zones are mostly confined, implying a very high local plasma density and consequently also an efficient scattering process.

Heavy haze episodes in Beijing during January 2013: Inorganic ion chemistry and source analysis using highly time-resolved measurements from an urban site.

PubMed

Han, Bin; Zhang, Rui; Yang, Wen; Bai, Zhipeng; Ma, Zhiqiang; Zhang, Wenjie

2016-02-15

The heavy air pollution that occurred in Beijing in January of 2013 attracted intense attention around the world. During this period, we conducted highly time-resolved measurements of inorganic ions associated with PM2.5 at an urban site of Beijing, and investigated ion chemistry and potential sources. Hourly concentrations of Cl(-), NO3(-), SO4(2-), Na(+), NH4(+), K(+), Mg(2+), and Ca(2+) were measured. Peak concentrations of SO4(2-) and NO3(-) were observed on the 10th-15th, 21st-24th, and the 26th-30th during this monitoring campaign. The percentages of SO4(2-) and NH4(+) in total ion concentration increased with the enhancement of PM2.5 concentrations, indicating that high concentrations of SO4(2-) and NH4(+) may play important roles in the formation of haze episodes. The ratio of [NO3(-)]/[SO4(2-)] was calculated, revealing that the sources of SO4(2-) would contribute more to the formation of PM2.5 than mobile sources. Diurnal variations of SO4(2-), NO3(-), NH4(+) (SNA) exhibited a similar pattern, with high concentrations at night and low levels during the day, revealing that meteorological conditions, such as mixing layer height, relative humidity, were likely to be responsible for high levels of SNA at night. The roles of meteorological conditions were further discussed in the formation of secondary inorganic ions. Relative humidity and temperature played key roles and exhibited positive correlations with secondary inorganic ions. An aerosol inorganics simulation model showed that SNA existed mainly in the aqueous phase during the sampling period. Furthermore, potential sources were identified by applying positive matrix factorization model. Secondary nitrate, secondary sulfate, coal combustion and biomass burning, as well as fugitive dust, were considered to be major contributors to total ions. Copyright © 2015. Published by Elsevier B.V.

The time-resolved photoelectron spectrum of toluene using a perturbation theory approach

DOE Office of Scientific and Technical Information (OSTI.GOV)

Richings, Gareth W.; Worth, Graham A., E-mail: g.a.worth@bham.ac.uk

A theoretical study of the intra-molecular vibrational-energy redistribution of toluene using time-resolved photo-electron spectra calculated using nuclear quantum dynamics and a simple, two-mode model is presented. Calculations have been carried out using the multi-configuration time-dependent Hartree method, using three levels of approximation for the calculation of the spectra. The first is a full quantum dynamics simulation with a discretisation of the continuum wavefunction of the ejected electron, whilst the second uses first-order perturbation theory to calculate the wavefunction of the ion. Both methods rely on the explicit inclusion of both the pump and probe laser pulses. The third method includesmore » only the pump pulse and generates the photo-electron spectrum by projection of the pumped wavepacket onto the ion potential energy surface, followed by evaluation of the Fourier transform of the autocorrelation function of the subsequently propagated wavepacket. The calculations performed have been used to study the periodic population flow between the 6a and 10b16b modes in the S{sub 1} excited state, and compared to recent experimental data. We obtain results in excellent agreement with the experiment and note the efficiency of the perturbation method.« less

Collision Cross Sections and Ion Mobility Separation of Fragment Ions from Complex N-Glycans.

PubMed

Harvey, David J; Watanabe, Yasunori; Allen, Joel D; Rudd, Pauline; Pagel, Kevin; Crispin, Max; Struwe, Weston B

2018-06-01

Ion mobility mass spectrometry (IM-MS) holds great potential for structural glycobiology, in particular in its ability to resolve glycan isomers. Generally, IM-MS has largely been applied to intact glycoconjugate ions with reports focusing on the separation of different adduct types. Here, we explore IM separation and report the collision cross section (CCS) of complex type N-glycans and their fragments in negative ion mode following collision-induced dissociation (CID). CCSs of isomeric fragment ions were found, in some cases, to reveal structural details that were not present in CID spectra themselves. Many fragment ions were confirmed as possessing multiple structure, details of which could be obtained by comparing their drift time profiles to different glycans. By using fragmentation both before and after mobility separation, information was gathered on the fragmentation pathways producing some of the ions. These results help demonstrate the utility of IM and will contribute to the growing use of IM-MS for glycomics. Graphical Abstract ᅟ.

Collision Cross Sections and Ion Mobility Separation of Fragment Ions from Complex N-Glycans

NASA Astrophysics Data System (ADS)

Harvey, David J.; Watanabe, Yasunori; Allen, Joel D.; Rudd, Pauline; Pagel, Kevin; Crispin, Max; Struwe, Weston B.

2018-04-01

Ion mobility mass spectrometry (IM-MS) holds great potential for structural glycobiology, in particular in its ability to resolve glycan isomers. Generally, IM-MS has largely been applied to intact glycoconjugate ions with reports focusing on the separation of different adduct types. Here, we explore IM separation and report the collision cross section (CCS) of complex type N-glycans and their fragments in negative ion mode following collision-induced dissociation (CID). CCSs of isomeric fragment ions were found, in some cases, to reveal structural details that were not present in CID spectra themselves. Many fragment ions were confirmed as possessing multiple structure, details of which could be obtained by comparing their drift time profiles to different glycans. By using fragmentation both before and after mobility separation, information was gathered on the fragmentation pathways producing some of the ions. These results help demonstrate the utility of IM and will contribute to the growing use of IM-MS for glycomics. [Figure not available: see fulltext.

Time-resolved photoion imaging spectroscopy: Determining energy distribution in multiphoton absorption experiments

NASA Astrophysics Data System (ADS)

Qian, D. B.; Shi, F. D.; Chen, L.; Martin, S.; Bernard, J.; Yang, J.; Zhang, S. F.; Chen, Z. Q.; Zhu, X. L.; Ma, X.

2018-04-01

We propose an approach to determine the excitation energy distribution due to multiphoton absorption in the case of excited systems following decays to produce different ion species. This approach is based on the measurement of the time-resolved photoion position spectrum by using velocity map imaging spectrometry and an unfocused laser beam with a low fluence and homogeneous profile. Such a measurement allows us to identify the species and the origin of each ion detected and to depict the energy distribution using a pure Poisson's equation involving only one variable which is proportional to the absolute photon absorption cross section. A cascade decay model is used to build direct connections between the energy distribution and the probability to detect each ionic species. Comparison between experiments and simulations permits the energy distribution and accordingly the absolute photon absorption cross section to be determined. This approach is illustrated using C60 as an example. It may therefore be extended to a wide variety of molecules and clusters having decay mechanisms similar to those of fullerene molecules.

Hydride ions in oxide hosts hidden by hydroxide ions

PubMed Central

Hayashi, Katsuro; Sushko, Peter V.; Hashimoto, Yasuhiro; Shluger, Alexander L.; Hosono, Hideo

2014-01-01

The true oxidation state of formally ‘H−’ ions incorporated in an oxide host is frequently discussed in connection with chemical shifts of 1H nuclear magnetic resonance spectroscopy, as they can exhibit values typically attributed to H+. Here we systematically investigate the link between geometrical structure and chemical shift of H− ions in an oxide host, mayenite, with a combination of experimental and ab initio approaches, in an attempt to resolve this issue. We demonstrate that the electron density near the hydrogen nucleus in an OH− ion (formally H+ state) exceeds that in an H− ion. This behaviour is the opposite to that expected from formal valences. We deduce a relationship between the chemical shift of H− and the distance from the H− ion to the coordinating electropositive cation. This relationship is pivotal for resolving H− species that are masked by various states of H+ ions. PMID:24662678

Overtone Mobility Spectrometry (Part 2): Theoretical Considerations of Resolving Power

PubMed Central

Valentine, Stephen J.; Stokes, Sarah T.; Kurulugama, Ruwan T.; Nachtigall, Fabiane M.; Clemmer, David E.

2009-01-01

The transport of ions through multiple drift regions is modeled in order to develop an equation that is useful for an understanding of the resolving power of an overtone mobility spectrometry (OMS) technique. It is found that resolving power is influenced by a number of experimental variables, including those that define ion mobility spectrometry (IMS) resolving power: drift field (E), drift region length (L), and buffer gas temperature (T). However, unlike IMS, the resolving power of OMS is also influenced by the number of drift regions (n), harmonic frequency value (m), and the phase number (ϕ) of the applied drift field. The OMS resolving power dependence upon the new OMS variables (n, m, and ϕ) scales differently than the square root dependence of the E, L, and T variables in IMS. The results provide insight about optimal instrumental design and operation. PMID:19230705

Angle-resolved Auger electron spectra induced by neon ion impact on aluminum

NASA Technical Reports Server (NTRS)

Pepper, S. V.; Aron, P. R.

1986-01-01

Auger electron emission from aluminum bombarded with 1 to 5 keV neon ions was studied by angle-resolved electron spectroscopy. The position and shape of the spectral features depended on the incident ion energy, angle of ion incidence, and electron take-off angle with respect to the aluminum surface. These spectral dependencies were interpreted in terms of the Doppler shift given to the Auger electron velocity by the excited atom ejected into the vacuum. For oblique ion incidence it is concluded that a flux of high energy atoms are ejected in a direction close to the projection of the ion beam on the target surface. In addition, a new spectral feature was found and identified as due to Auger emission from excited neon in the aluminum matrix.

Bimodal Exciplex Formation in Bimolecular Photoinduced Electron Transfer Revealed by Ultrafast Time-Resolved Infrared Absorption.

PubMed

Koch, Marius; Licari, Giuseppe; Vauthey, Eric

2015-09-03

The dynamics of a moderately exergonic photoinduced charge separation has been investigated by ultrafast time-resolved infrared absorption with the dimethylanthracene/phthalonitrile donor/acceptor pair in solvents covering a broad range of polarity. A distinct spectral signature of an exciplex could be identified in the -C≡N stretching region. On the basis of quantum chemistry calculations, the 4-5 times larger width of this band compared to those of the ions and of the locally excited donor bands is explained by a dynamic distribution of exciplex geometry with different mutual orientations and distances of the constituents and, thus, with varying charge-transfer character. Although spectrally similar, two types of exciplexes could be distinguished by their dynamics: short-lived, "tight", exciplexes generated upon static quenching and longer-lived, "loose", exciplexes formed upon dynamic quenching in parallel with ion pairs. Tight exciplexes were observed in all solvents, except in the least polar diethyl ether where quenching is slower than diffusion. The product distribution of the dynamic quenching depends strongly on the solvent polarity: whereas no significant loose exciplex population could be detected in acetonitrile, both exciplex and ion pair are generated in less polar solvents, with the relative population of exciplex increasing with decreasing solvent polarity. These results are compared with those reported previously with donor/acceptor pairs in different driving force regimes to obtain a comprehensive picture of the role of the exciplexes in bimolecular photoinduced charge separation.

A hemispherical Langmuir probe array detector for angular resolved measurements on droplet-based laser-produced plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gambino, Nadia, E-mail: gambinon@ethz.ch; Brandstätter, Markus; Rollinger, Bob

2014-09-15

In this work, a new diagnostic tool for laser-produced plasmas (LPPs) is presented. The detector is based on a multiple array of six motorized Langmuir probes. It allows to measure the dynamics of a LPP in terms of charged particles detection with particular attention to droplet-based LPP sources for EUV lithography. The system design permits to temporally resolve the angular and radial plasma charge distribution and to obtain a hemispherical mapping of the ions and electrons around the droplet plasma. The understanding of these dynamics is fundamental to improve the debris mitigation techniques for droplet-based LPP sources. The device hasmore » been developed, built, and employed at the Laboratory for Energy Conversion, ETH Zürich. The experimental results have been obtained on the droplet-based LPP source ALPS II. For the first time, 2D mappings of the ion kinetic energy distribution around the droplet plasma have been obtained with an array of multiple Langmuir probes. These measurements show an anisotropic expansion of the ions in terms of kinetic energy and amount of ion charge around the droplet target. First estimations of the plasma density and electron temperature were also obtained from the analysis of the probe current signals.« less

Dusty Pair Plasma—Wave Propagation and Diffusive Transition of Oscillations

NASA Astrophysics Data System (ADS)

Atamaniuk, Barbara; Turski, Andrzej J.

2011-11-01

The crucial point of the paper is the relation between equilibrium distributions of plasma species and the type of propagation or diffusive transition of plasma response to a disturbance. The paper contains a unified treatment of disturbance propagation (transport) in the linearized Vlasov electron-positron and fullerene pair plasmas containing charged dust impurities, based on the space-time convolution integral equations. Electron-positron-dust/ion (e-p-d/i) plasmas are rather widespread in nature. Space-time responses of multi-component linearized Vlasov plasmas on the basis of multiple integral equations are invoked. An initial-value problem for Vlasov-Poisson/Ampère equations is reduced to the one multiple integral equation and the solution is expressed in terms of forcing function and its space-time convolution with the resolvent kernel. The forcing function is responsible for the initial disturbance and the resolvent is responsible for the equilibrium velocity distributions of plasma species. By use of resolvent equations, time-reversibility, space-reflexivity and the other symmetries are revealed. The symmetries carry on physical properties of Vlasov pair plasmas, e.g., conservation laws. Properly choosing equilibrium distributions for dusty pair plasmas, we can reduce the resolvent equation to: (i) the undamped dispersive wave equations, (ii) and diffusive transport equations of oscillations.

Time-dependent, x-ray spectral unfolds and brightness temperatures for intense Li{sup +} ion beam-driven hohlraums

DOE Office of Scientific and Technical Information (OSTI.GOV)

Fehl, D.L.; Chandler, G.A.; Biggs, F.

X-ray-producing hohlraums are being studied as indirect drives for inertial confinement fusion targets. In a 1994 target series on the PBFAII accelerator, cylindrical hohlraum targets were heated by an intense Li{sup +} ion beam and viewed by an array of 13 time-resolved, filtered x-ray detectors (XRDs). The unfold operator (UFO) code and its suite of auxiliary functions were used extensively in obtaining time-resolved x-ray spectra and radiation temperatures from this diagnostic. The UFO was also used to obtain fitted response functions from calibration data, to simulate data from blackbody x-ray spectra of interest, to determine the suitability of various unfoldingmore » parameters (e.g., energy domain, energy partition, smoothing conditions, and basis functions), to interpolate the XRD signal traces, and to unfold experimental data. The simulation capabilities of the code were useful in understanding an anomalous feature in the unfolded spectra at low photon energies ({le}100 eV). Uncertainties in the differential and energy-integrated unfolded spectra were estimated from uncertainties in the data. The time{endash}history of the radiation temperature agreed well with independent calculations of the wall temperature in the hohlraum. {copyright} {ital 1997 American Institute of Physics.}« less

VizieR Online Data Catalog: Parameterization of level-resolved RR data fro SPEX (Mao+, 2016)

NASA Astrophysics Data System (ADS)

Mao, J.; Kaastra, J.

2016-02-01

The fitting parameters for the level-resolved radiative recombination rate coefficients for H-like to Na-like ions from H (z=1) up to and including (z=30), in a wide temperature range. The electron temperature should be in units of eV. We refer to the recombined ion when we speak of the radiative recombination of a certain ion, e.g. for a bare oxygen ion capturing a free electron via radiative recombination to form H-like oxygen (O VIII, s=1, z=8). The fitting accuracies are better than 5% for ~99% of the levels considered here. (1 data file).

More evidence for azimuthal ion spin in HiPIMS discharges

NASA Astrophysics Data System (ADS)

Poolcharuansin, P.; Liebig, B.; Bradley, J. W.

2012-02-01

The velocity and energy distribution functions of ions escaping radially from the magnetic trap region of a HiPIMS discharge have been measured using a retarding field analyzer (RFA). Spatially and angularly resolved measurements recorded at a representative time show more energetic ions detected along a line-of-sight coincident with an oncoming rotating ion fluid, which circulates above the racetrack in the same direction as the electron E × B drift. The difference in the mean ion energies between measurements made into and against the direction of rotation is ~5 eV. Numerical solutions of the equation of motion for the ions accounting for azimuthal acceleration (modified two-stream instability model used by Lundin et al) have been found. The centripetal force caused by the radial electric field and a drag force term accounting for ion collisions revealed that only a small fraction (typically <5%) of the circulating ion flux can leave the discharge tangentially. Operating the discharge at different background pressures revealed an interplay between the azimuthal acceleration of ions, dominating under low pressure conditions and the scattering of ions into the RFA at higher pressure.

Characterization of high explosive particles using cluster secondary ion mass spectrometry.

PubMed

Gillen, Greg; Mahoney, Christine; Wight, Scott; Lareau, Richard

2006-01-01

The use of secondary ion mass spectrometry (SIMS) for the detection and spatially resolved analysis of individual high explosive particles is described. A C(8) (-) carbon cluster primary ion beam was used in a commercial SIMS instrument to analyze samples of high explosives dispersed as particles on silicon substrates. In comparison with monatomic primary ion bombardment, the carbon cluster primary ion beam was found to greatly enhance characteristic secondary ion signals from the explosive compounds while causing minimal beam-induced degradation. The resistance of these compounds to degradation under ion bombardment allows explosive particles to be analyzed under high primary ion dose bombardment (dynamic SIMS) conditions, facilitating the rapid acquisition of spatially resolved molecular information. The use of cluster SIMS combined with computer control of the sample stage position allows for the automated identification and counting of explosive particle distributions on silicon surfaces. This will be useful for characterizing the efficiency of transfer of particulates in trace explosive detection portal collectors and/or swipes utilized for ion mobility spectrometry applications.

Linearized spectrum correlation analysis for line emission measurements

NASA Astrophysics Data System (ADS)

Nishizawa, T.; Nornberg, M. D.; Den Hartog, D. J.; Sarff, J. S.

2017-08-01

A new spectral analysis method, Linearized Spectrum Correlation Analysis (LSCA), for charge exchange and passive ion Doppler spectroscopy is introduced to provide a means of measuring fast spectral line shape changes associated with ion-scale micro-instabilities. This analysis method is designed to resolve the fluctuations in the emission line shape from a stationary ion-scale wave. The method linearizes the fluctuations around a time-averaged line shape (e.g., Gaussian) and subdivides the spectral output channels into two sets to reduce contributions from uncorrelated fluctuations without averaging over the fast time dynamics. In principle, small fluctuations in the parameters used for a line shape model can be measured by evaluating the cross spectrum between different channel groupings to isolate a particular fluctuating quantity. High-frequency ion velocity measurements (100-200 kHz) were made by using this method. We also conducted simulations to compare LSCA with a moment analysis technique under a low photon count condition. Both experimental and synthetic measurements demonstrate the effectiveness of LSCA.

Adding high time resolution to charge-state-specific ion energy measurements for pulsed copper vacuum arc plasmas

NASA Astrophysics Data System (ADS)

Tanaka, Koichi; Han, Liang; Zhou, Xue; Anders, André

2015-08-01

Charge-state-resolved ion energy-time distributions of pulsed Cu arc plasma were obtained by using direct (time-dependent) acquisition of the ion detection signal from a commercial ion mass-per-charge and energy-per-charge analyzer. We find a shift of energies of Cu2+, Cu3+ and Cu4+ ions to lower values during the first few hundred microseconds after arc ignition, which is evidence for particle collisions in the plasma. The generation of Cu+ ions in the later part of the pulse, measured by the increase of Cu+ signal intensity and an associated slight reduction of the mean charge state, points to charge exchange reactions between ions and neutrals. At the very beginning of the pulse, when the plasma expands into vacuum and the plasma potential strongly fluctuates, ions with much higher energy (over 200 eV) are observed. Early in the pulse, the ion energies observed are approximately proportional to the ion charge state, and we conclude that the acceleration mechanism is primarily based on acceleration in an electric field. This field is directed away from the cathode, indicative of a potential hump. Measurements by a floating probe suggest that potential structures travel, and ions moving in the traveling field can gain high energies up to a few hundred electron-volts. Later in the pulse, the approximate proportionality is lost, which is related to increased smearing out of different energies due to collisions with neutrals, and/or to a change of the acceleration character from electrostatic to ‘gas-dynamic’, i.e. dominated by pressure gradient.

THOR Ion Mass Spectrometer (IMS)

NASA Astrophysics Data System (ADS)

Retinò, Alessandro

2017-04-01

Turbulence Heating ObserveR (THOR) is the first mission ever flown in space dedicated to plasma turbulence. The Ion Mass Spectrometer (IMS) onboard THOR will provide the first high-time resolution measurements of mass-resolved ions in near-Earth space, focusing on hot ions in the foreshock, shock and magnetosheath turbulent regions. These measurements are required to study how kinetic-scale turbulent fluctuations heat and accelerate different ion species. IMS will measure the full three-dimensional distribution functions of main ion species (H+, He++, O+) in the energy range 10 eV/q to 30 keV/q with energy resolution DE/E down to 10% and angular resolution down to 11.25˚ . The time resolution will be 150 ms for O+, 300 ms for He++ and ˜ 1s for O+, which correspond to ion scales in the the foreshock, shock and magnetosheath regions. Such high time resolution is achieved by mounting four identical IMS units phased by 90˚ in the spacecraft spin plane. Each IMS unit combines a top-hat electrostatic analyzer with deflectors at the entrance together with a time-of-flight section to perform mass selection. Adequate mass-per-charge resolution (M/q)/(ΔM/q) (≥ 8 for He++ and ≥ 3 for O+) is obtained through a 6 cm long Time-of-Flight (TOF) section. IMS electronics includes a fast sweeping high voltage board that is required to make measurements at high cadence. Ion detection includes Micro Channel Plates (MCPs) combined with Application-Specific Integrated Circuits (ASICs) for charge amplification and discrimination and a discrete Time-to-Amplitude Converter (TAC) to determine the ion time of flight. A processor board will be used to for ion events formatting and will interface with the Particle Processing Unit (PPU), which will perform data processing for THOR particle detectors. The IMS instrument is being designed and will be built and calibrated by an international consortium of scientific institutes from France, USA, Germany and Japan and Switzerland.

Complementary online aerosol mass spectrometry and offline FT-IR spectroscopy measurements: Prospects and challenges for the analysis of anthropogenic aerosol particle emissions

NASA Astrophysics Data System (ADS)

Faber, Peter; Drewnick, Frank; Bierl, Reinhard; Borrmann, Stephan

2017-10-01

The aerosol mass spectrometer (AMS) is well established in investigating highly time-resolved dynamics of submicron aerosol chemical composition including organic aerosol (OA). However, interpretation of mass spectra on molecular level is limited due to strong fragmentation of organic substances and potential reactions inside the AMS ion chamber. Results from complementary filter-based FT-IR absorption measurements were used to explain features in high-resolution AMS mass spectra of different types of OA (e.g. cooking OA, cigarette smoking OA, wood burning OA). Using this approach some AMS fragment ions were validated in this study as appropriate and rather specific markers for a certain class of organic compounds for all particle types under investigation. These markers can therefore be used to get deeper insights in the chemical composition of OA based on AMS mass spectra in upcoming studies. However, the specificity of other fragment ions such as C2H4O2+ (m/z 60.02114) remains ambiguous. In such cases, complementary FT-IR measurements allow the interpretation of highly time-resolved AMS mass spectra at the level of molecular functional groups. Furthermore, this study discusses the challenges in reducing inorganic interferences (e.g. from water and ammonium salts) in FT-IR spectra of atmospheric aerosols to decrease spectral uncertainties for better comparisons and, thus, to get more robust results.

Plasma characterization of the superconducting proton linear accelerator plasma generator using a 2 MHz compensated Langmuir probe.

PubMed

Schmitzer, C; Kronberger, M; Lettry, J; Sanchez-Arias, J; Störi, H

2012-02-01

The CERN study for a superconducting proton Linac (SPL) investigates the design of a pulsed 5 GeV Linac operating at 50 Hz. As a first step towards a future SPL H(-) volume ion source, a plasma generator capable of operating at Linac4 or nominal SPL settings has been developed and operated at a dedicated test stand. The hydrogen plasma is heated by an inductively coupled RF discharge e(-) and ions are confined by a magnetic multipole cusp field similar to the currently commissioned Linac4 H(-) ion source. Time-resolved measurements of the plasma potential, temperature, and electron energy distribution function obtained by means of a RF compensated Langmuir probe along the axis of the plasma generator are presented. The influence of the main tuning parameters, such as RF power and frequency and the timing scheme is discussed with the aim to correlate them to optimum H(-) ion beam parameters measured on an ion source test stand. The effects of hydrogen injection settings which allow operation at 50 Hz repetition rate are discussed.

Plasma characterization of the superconducting proton linear accelerator plasma generator using a 2 MHz compensated Langmuir probea)

NASA Astrophysics Data System (ADS)

Schmitzer, C.; Kronberger, M.; Lettry, J.; Sanchez-Arias, J.; Störi, H.

2012-02-01

The CERN study for a superconducting proton Linac (SPL) investigates the design of a pulsed 5 GeV Linac operating at 50 Hz. As a first step towards a future SPL H- volume ion source, a plasma generator capable of operating at Linac4 or nominal SPL settings has been developed and operated at a dedicated test stand. The hydrogen plasma is heated by an inductively coupled RF discharge e- and ions are confined by a magnetic multipole cusp field similar to the currently commissioned Linac4 H- ion source. Time-resolved measurements of the plasma potential, temperature, and electron energy distribution function obtained by means of a RF compensated Langmuir probe along the axis of the plasma generator are presented. The influence of the main tuning parameters, such as RF power and frequency and the timing scheme is discussed with the aim to correlate them to optimum H- ion beam parameters measured on an ion source test stand. The effects of hydrogen injection settings which allow operation at 50 Hz repetition rate are discussed.

Understanding ion association states and molecular dynamics using infrared spectroscopy

NASA Astrophysics Data System (ADS)

Masser, Hanqing

A molecular level understanding of the ion transport mechanism within polymer electrolytes is crucial to the further development for advanced energy storage applications. This can be achieved by the identification and quantitative measurement of different ion species in the system and further relating them to the ion conductivity. In the first part of this thesis, research is presented towards understanding the ion association states (free ions, ion pairs and ion aggregates) in ionomer systems, and the correlation of ion association states, ion conduction, polymer dynamics, and morphology. Ion conductivity in ionomers can be improved by lowering glass transition temperature, increasing polymer ion solvation ability, and adjusting ionomer structural variables such as ion content, cation type and side chain structure. These effects are studied in three ionomer systems respectively, using a combination of characterization methods. Fourier Transform Infrared Spectroscopy (FTIR) identifies and quantifies the ion association states. Dielectric Spectroscopy (DRS) characterizes ion conductivity and polymer and ion dynamics. X-ray scattering reveals changes in morphology. The influence of a cation solvating plasticizer on a polyester ionomer is systematically investigated with respect to ion association states, ion and polymer dynamics and morphology. A decrease in the number ratio of ion aggregates with increased plasticizer content and a slight increase at elevated temperature are observed in FTIR. Similar results are also detected by X-ray scattering. As determined from dielectric spectroscopy, ion conductivity increases with plasticizer content, in accordance with the decrease in glass transition temperature. Research on copolymer of poly(ethylene oxide) (PEO) and poly(tetramethylene oxide) (PTMO) based ionomers further develops an understanding of the trade-off between ion solvation and segmental dynamics. Upon the incorporation of PTMO, the majority of the PTMO microphase separates from the PEO-rich microphase, and ionic groups are preferentially solvated by PEO chains and reside in the PEO-rich microphase. As the ratio of PTMO increases, the fraction of aggregates increases, resulting in more highly coordinated aggregation states. Results on ion association states are in good agreement with previous results on ion conductivity, polymer dynamics and morphology. The effects of ion content, cation type and ionic side chain structure on ion association states are systemically studied in a series of ionomers with short ethylene oxide and ionic sulfonated styrene side chains, and then correlated to the ion and polymer dynamic characterization. It is found that ionomers with modest ion content, large cation and styrene ionic side chain have the most "free ions" and ion pairs, and highest ion conductivity. Ion conduction in ionomers is optimized by systematically changing their chemical structures. In addition to knowledge of ion association states, a IR band shape also contains information on molecular dynamics. In companion investigation, the vibrational relaxation and dynamic transitions of conformationally insensitive normal modes in two different polymer systems (atactic polystyrene and deuterated poly(methyl methacrylate)) are studied. The information on vibrational relaxations is resolved by conducting precisely controlled FTIR experiments, applying specialized curve resolving data analysis, and calculating time correlation functions through numerical Fourier transformation. The vibrational relaxations of these modes can be described by a two process model: a fast process on the time scale of 0.01 ps, which is inhomogeneously broadened by a slow process on the time scale of picoseconds.

X-ray scattering measurements of strong ion-ion correlations in shock-compressed aluminum.

PubMed

Ma, T; Döppner, T; Falcone, R W; Fletcher, L; Fortmann, C; Gericke, D O; Landen, O L; Lee, H J; Pak, A; Vorberger, J; Wünsch, K; Glenzer, S H

2013-02-08

The strong ion-ion correlation peak characteristic of warm dense matter (WDM) is observed for the first time using simultaneous angularly, temporally, and spectrally resolved x-ray scattering measurements in laser-driven shock-compressed aluminum. Laser-produced molybdenum x-ray line emission at an energy of 17.9 keV is employed to probe aluminum compressed to a density of ρ>8 g/cm(3). We observe a well pronounced peak in the static structure factor at a wave number of k=4.0 Å(-1). The measurements of the magnitude and position of this correlation peak are precise enough to test different theoretical models for the ion structure and show that only models taking the complex interaction in WDM into account agree with the data. This also demonstrates a new highly accurate diagnostic to directly measure the state of compression of warm dense matter.

An experiment on the dynamics of ion implantation and sputtering of surfaces

NASA Astrophysics Data System (ADS)

Wright, G. M.; Barnard, H. A.; Kesler, L. A.; Peterson, E. E.; Stahle, P. W.; Sullivan, R. M.; Whyte, D. G.; Woller, K. B.

2014-02-01

A major impediment towards a better understanding of the complex plasma-surface interaction is the limited diagnostic access to the material surface while it is undergoing plasma exposure. The Dynamics of ION Implantation and Sputtering Of Surfaces (DIONISOS) experiment overcomes this limitation by uniquely combining powerful, non-perturbing ion beam analysis techniques with a steady-state helicon plasma exposure chamber, allowing for real-time, depth-resolved in situ measurements of material compositions during plasma exposure. Design solutions are described that provide compatibility between the ion beam analysis requirements in the presence of a high-intensity helicon plasma. The three primary ion beam analysis techniques, Rutherford backscattering spectroscopy, elastic recoil detection, and nuclear reaction analysis, are successfully implemented on targets during plasma exposure in DIONISOS. These techniques measure parameters of interest for plasma-material interactions such as erosion/deposition rates of materials and the concentration of plasma fuel species in the material surface.

An experiment on the dynamics of ion implantation and sputtering of surfaces.

PubMed

Wright, G M; Barnard, H A; Kesler, L A; Peterson, E E; Stahle, P W; Sullivan, R M; Whyte, D G; Woller, K B

2014-02-01

A major impediment towards a better understanding of the complex plasma-surface interaction is the limited diagnostic access to the material surface while it is undergoing plasma exposure. The Dynamics of ION Implantation and Sputtering Of Surfaces (DIONISOS) experiment overcomes this limitation by uniquely combining powerful, non-perturbing ion beam analysis techniques with a steady-state helicon plasma exposure chamber, allowing for real-time, depth-resolved in situ measurements of material compositions during plasma exposure. Design solutions are described that provide compatibility between the ion beam analysis requirements in the presence of a high-intensity helicon plasma. The three primary ion beam analysis techniques, Rutherford backscattering spectroscopy, elastic recoil detection, and nuclear reaction analysis, are successfully implemented on targets during plasma exposure in DIONISOS. These techniques measure parameters of interest for plasma-material interactions such as erosion/deposition rates of materials and the concentration of plasma fuel species in the material surface.

Real-time observation of intramolecular proton transfer in the electronic ground state of chloromalonaldehyde: an ab initio study of time-resolved photoelectron spectra.

PubMed

do N Varella, Márcio T; Arasaki, Yasuki; Ushiyama, Hiroshi; Takatsuka, Kazuo; Wang, Kwanghsi; McKoy, Vincent

2007-02-07

The authors report on studies of time-resolved photoelectron spectra of intramolecular proton transfer in the ground state of chloromalonaldehyde, employing ab initio photoionization matrix elements and effective potential surfaces of reduced dimensionality, wherein the couplings of proton motion to the other molecular vibrational modes are embedded by averaging over classical trajectories. In the simulations, population is transferred from the vibrational ground state to vibrationally hot wave packets by pumping to an excited electronic state and dumping with a time-delayed pulse. These pump-dump-probe simulations demonstrate that the time-resolved photoelectron spectra track proton transfer in the electronic ground state well and, furthermore, that the geometry dependence of the matrix elements enhances the tracking compared with signals obtained with the Condon approximation. Photoelectron kinetic energy distributions arising from wave packets localized in different basins are also distinguishable and could be understood, as expected, on the basis of the strength of the optical couplings in different regions of the ground state potential surface and the Franck-Condon overlaps of the ground state wave packets with the vibrational eigenstates of the ion potential surface.

A mini-photofragment translational spectrometer with ion velocity map imaging using low voltage acceleration

NASA Astrophysics Data System (ADS)

Qi, Wenke; Jiang, Pan; Lin, Dan; Chi, Xiaoping; Cheng, Min; Du, Yikui; Zhu, Qihe

2018-01-01

A mini time-sliced ion velocity map imaging photofragment translational spectrometer using low voltage acceleration has been constructed. The innovation of this apparatus adopts a relative low voltage (30-150 V) to substitute the traditional high voltage (650-4000 V) to accelerate and focus the fragment ions. The overall length of the flight path is merely 12 cm. There are many advantages for this instrument, such as compact structure, less interference, and easy to operate and control. Low voltage acceleration gives a longer turn-around time to the photofragment ions forming a thicker Newton sphere, which provides sufficient time for slicing. Ion trajectory simulation has been performed for determining the structure dimensions and the operating voltages. The photodissociation and multiphoton ionization of O2 at 224.999 nm is used to calibrate the ion images and examine the overall performance of the new spectrometer. The velocity resolution (Δν/ν) of this spectrometer from O2 photodissociation is about 0.8%, which is better than most previous results using high acceleration voltage. For the case of CF3I dissociation at 277.38 nm, many CF3 vibrational states have been resolved, and the anisotropy parameter has been measured. The application of low voltage acceleration has shown its advantages on the ion velocity map imaging (VMI) apparatus. The miniaturization of the VMI instruments can be realized on the premise of high resolution.

PM10 source apportionment in Milan (Italy) using time-resolved data.

PubMed

Bernardoni, Vera; Vecchi, Roberta; Valli, Gianluigi; Piazzalunga, Andrea; Fermo, Paola

2011-10-15

In this work Positive Matrix Factorization (PMF) was applied to 4-hour resolved PM10 data collected in Milan (Italy) during summer and winter 2006. PM10 characterisation included elements (Mg-Pb), main inorganic ions (NH(4)(+), NO(3)(-), SO(4)(2-)), levoglucosan and its isomers (mannosan and galactosan), and organic and elemental carbon (OC and EC). PMF resolved seven factors that were assigned to construction works, re-suspended dust, secondary sulphate, traffic, industry, secondary nitrate, and wood burning. Multi Linear Regression was applied to obtain the PM10 source apportionment. The 4-hour temporal resolution allowed the estimation of the factor contributions during peculiar episodes, which would have not been detected with the traditional 24-hour sampling strategy. Copyright © 2011 Elsevier B.V. All rights reserved.

Real-time visualization of the vibrational wavepacket dynamics in electronically excited pyrimidine via femtosecond time-resolved photoelectron imaging

NASA Astrophysics Data System (ADS)

Li, Shuai; Long, Jinyou; Ling, Fengzi; Wang, Yanmei; Song, Xinli; Zhang, Song; Zhang, Bing

2017-07-01

The vibrational wavepacket dynamics at the very early stages of the S1-T1 intersystem crossing in photoexcited pyrimidine is visualized in real time by femtosecond time-resolved photoelectron imaging and time-resolved mass spectroscopy. A coherent superposition of the vibrational states is prepared by the femtosecond pump pulse at 315.3 nm, resulting in a vibrational wavepacket. The composition of the prepared wavepacket is directly identified by a sustained quantum beat superimposed on the parent-ion transient, possessing a frequency in accord with the energy separation between the 6a1 and 6b2 states. The dephasing time of the vibrational wavepacket is determined to be 82 ps. More importantly, the variable Franck-Condon factors between the wavepacket components and the dispersed cation vibrational levels are experimentally illustrated to identify the dark state and follow the energy-flow dynamics on the femtosecond time scale. The time-dependent intensities of the photoelectron peaks originated from the 6a1 vibrational state exhibit a clear quantum beating pattern with similar periodicity but a phase shift of π rad with respect to those from the 6b2 state, offering an unambiguous picture of the restricted intramolecular vibrational energy redistribution dynamics in the 6a1/6b2 Fermi resonance.

[Quenched fluorescein: a reference dye for instrument response function of TCSPC].

PubMed

Pan, Hai-feng; Ding, Jing-xin; Liang, Rong-rong; Tao, Zhan-dong; Liu, Meng-wei; Zhang, San-jun; Xu, Jian-hua

2014-08-01

Measuring the instrument response function (IRF) and fitting by reconvolution algorithms are routines to improve time resolution in fluorescence lifetime measurements. Iodide ions were successfully used to quench the fluorescence of fluorescein in this study. By systematically adding saturated NaI water solution in basic fluorescein solution, the lifetimes of fluorescein were reduced from 4 ns to 24 ps. The quenched lifetime of fluorescein obtained from the analysis of Time-Correlated Single Photon Counting (TCSPC) measurement agrees well with that from femtosecond frequency up-conversion measurement. In time resolved excitation spectra measurements, the IRF should be measured at various detection wavelengths providing scattring materials are used. This study could not only reduce the complexity of IRF measurement, but also avoid the existing color effect in system. This study should have wide applications in time resolved fluorescence spectroscopy and fluorescence lifetime imaging.

Spectral modeling of laser-produced underdense titanium plasmas

NASA Astrophysics Data System (ADS)

Chung, Hyun-Kyung; Back, Christina A.; Scott, Howard A.; Constantin, Carmen; Lee, Richard W.

2004-11-01

Experiments were performed at the NIKE laser to create underdense low-Z plasmas with a small amount of high-Z dopant in order to study non-LTE population kinetics. An absolutely calibrated spectra in 470-3000 eV was measured in time-resolved and time-averaged fashion from SiO2 aerogel target with 3% Ti dopant. K-shell Ti emission was observed as well as L-shell Ti emission. Time-resolved emission show that lower energy photons peak later than higher energy photons due to plasma cooling. In this work, we compare the measured spectra with non-LTE spectral calculations of titanium emission at relatively low temperatures < 1 keV and electron densities from 1e19 to 1e21 cm-3. A temperature diagnostics using the charge state distributions dominated by L-shell ions will be discussed.

Laser characterization of the unsteady 2-D ion flow field in a Hall thruster with breathing mode oscillations

NASA Astrophysics Data System (ADS)

Lucca Fabris, Andrea; Young, Christopher; MacDonald-Tenenbaum, Natalia; Hargus, William, Jr.; Cappelli, Mark

2016-10-01

Hall thrusters are a mature form of electric propulsion for spacecraft. One commonly observed low frequency (10-50 kHz) discharge current oscillation in these E × B devices is the breathing mode, linked to a propagating ionization front traversing the channel. The complex time histories of ion production and acceleration in the discharge channel and near-field plume lead to interesting dynamics and interactions in the central plasma jet and downstream plume regions. A time-resolved laser-induced fluorescence (LIF) diagnostic non-intrusively measures 2-D ion velocity and relative ion density throughout the plume of a commercial BHT-600 Hall thruster manufactured by Busek Co. Low velocity classes of ions observed in addition to the main accelerated population are linked to propellant ionization outside of the device. Effects of breathing mode dynamics are shown to persist far downstream where modulations in ion velocity and LIF intensity are correlated with discharge current oscillations. This work is sponsored by the U.S. Air Force Office of Scientific Research with Dr. M. Birkan as program manager. C.Y. acknowledges support from the DOE NSSA Stewardship Science Graduate Fellowship under contract DE-FC52-08NA28752.

Breaking through the false coincidence barrier in electron–ion coincidence experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Osborn, David L.; Hayden, Carl C.; Hemberger, Patrick

Photoelectron Photoion Coincidence (PEPICO) spectroscopy holds the promise of a universal, isomer-selective, and sensitive analytical technique for time-resolved quantitative analysis of bimolecular chemical reactions. Unfortunately, its low dynamic range of ~10 3 has largely precluded its use for this purpose, where a dynamic range of at least 10 5 is generally required. This limitation is due to the false coincidence background common to all coincidence experiments, especially at high count rates. Electron/ion pairs emanating from separate ionization events but arriving within the ion time of flight (TOF) range of interest constitute the false coincidence background. Although this background has uniformmore » intensity at every m/z value, the Poisson scatter in the false coincidence background obscures small signals. In this paper, temporal ion deflection coupled with a position-sensitive ion detector enables suppression of the false coincidence background, increasing the dynamic range in the PEPICO TOF mass spectrum by 2–3 orders of magnitude. The ions experience a time-dependent electric deflection field at a well-defined fraction of their time of flight. This deflection defines an m/z- and ionization-time dependent ion impact position for true coincidences, whereas false coincidences appear randomly outside this region and can be efficiently suppressed. When cold argon clusters are ionized, false coincidence suppression allows us to observe species up to Ar 9 +, whereas Ar 4 + is the largest observable cluster under traditional operation. As a result, this advance provides mass-selected photoelectron spectra for fast, high sensitivity quantitative analysis of reacting systems.« less

Breaking through the false coincidence barrier in electron–ion coincidence experiments

DOE PAGES

Osborn, David L.; Hayden, Carl C.; Hemberger, Patrick; ...

2016-10-31

Photoelectron Photoion Coincidence (PEPICO) spectroscopy holds the promise of a universal, isomer-selective, and sensitive analytical technique for time-resolved quantitative analysis of bimolecular chemical reactions. Unfortunately, its low dynamic range of ~10 3 has largely precluded its use for this purpose, where a dynamic range of at least 10 5 is generally required. This limitation is due to the false coincidence background common to all coincidence experiments, especially at high count rates. Electron/ion pairs emanating from separate ionization events but arriving within the ion time of flight (TOF) range of interest constitute the false coincidence background. Although this background has uniformmore » intensity at every m/z value, the Poisson scatter in the false coincidence background obscures small signals. In this paper, temporal ion deflection coupled with a position-sensitive ion detector enables suppression of the false coincidence background, increasing the dynamic range in the PEPICO TOF mass spectrum by 2–3 orders of magnitude. The ions experience a time-dependent electric deflection field at a well-defined fraction of their time of flight. This deflection defines an m/z- and ionization-time dependent ion impact position for true coincidences, whereas false coincidences appear randomly outside this region and can be efficiently suppressed. When cold argon clusters are ionized, false coincidence suppression allows us to observe species up to Ar 9 +, whereas Ar 4 + is the largest observable cluster under traditional operation. As a result, this advance provides mass-selected photoelectron spectra for fast, high sensitivity quantitative analysis of reacting systems.« less

Importance of counteranions on the hydration structure of the curium ion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Atta Fynn, Raymond; Bylaska, Eric J.; De Jong, Wibe A.

2013-07-04

Using density functional theory based ab initio molecular dynamics and metadynamics we show that counter ions can trigger noticeable changes in the hydration shell structure of the curium ion. The free energies of curium-water coordination and the solvent hydrogen bond (HB) lifetimes in the absence and presence the counter anions predict that chloride and bromide counter anions strengthen the first shell and consequently the 8-fold coordination state is dominant by at least 98%. In contrast, the perchlorate counter anions are found to weaken the coordination shell and the HB network, with the 9-fold and 8-fold states existing in an 8:1more » ratio, which is in good agreement with reported 9:1 ratio seen in time resolved fluorescence spectroscopy experiments. To our knowledge this is the first time molecular simulations have shown that counter anions can directly affect the first hydration shell structure of a cation.« less

Capturing the radical ion-pair intermediate in DNA guanine oxidation

PubMed Central

Jie, Jialong; Liu, Kunhui; Wu, Lidan; Zhao, Hongmei; Song, Di; Su, Hongmei

2017-01-01

Although the radical ion pair has been frequently invoked as a key intermediate in DNA oxidative damage reactions and photoinduced electron transfer processes, the unambiguous detection and characterization of this species remain formidable and unresolved due to its extremely unstable nature and low concentration. We use the strategy that, at cryogenic temperatures, the transient species could be sufficiently stabilized to be detectable spectroscopically. By coupling the two techniques (the cryogenic stabilization and the time-resolved laser flash photolysis spectroscopy) together, we are able to capture the ion-pair transient G+•⋯Cl− in the chlorine radical–initiated DNA guanine (G) oxidation reaction, and provide direct evidence to ascertain the intricate type of addition/charge separation mechanism underlying guanine oxidation. The unique spectral signature of the radical ion-pair G+•⋯Cl− is identified, revealing a markedly intense absorption feature peaking at 570 nm that is distinctive from G+• alone. Moreover, the ion-pair spectrum is found to be highly sensitive to the protonation equilibria within guanine-cytosine base pair (G:C), which splits into two resolved bands at 480 and 610 nm as the acidic proton transfers along the central hydrogen bond from G+• to C. We thus use this exquisite sensitivity to track the intrabase-pair proton transfer dynamics in the double-stranded DNA oligonucleotides, which is of critical importance for the description of the proton-coupled charge transfer mechanisms in DNA. PMID:28630924

Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization

PubMed Central

Amini, Kasra; Savelyev, Evgeny; Brauße, Felix; Berrah, Nora; Bomme, Cédric; Brouard, Mark; Burt, Michael; Christensen, Lauge; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Kierspel, Thomas; Krecinic, Faruk; Lauer, Alexandra; Lee, Jason W. L.; Müller, Maria; Müller, Erland; Mullins, Terence; Redlin, Harald; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Vallance, Claire; Wiese, Joss; Johnsson, Per; Küpper, Jochen; Rudenko, Artem; Rouzée, Arnaud; Stapelfeldt, Henrik; Rolles, Daniel; Boll, Rebecca

2018-01-01

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon–iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules. PMID:29430482

Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization.

PubMed

Amini, Kasra; Savelyev, Evgeny; Brauße, Felix; Berrah, Nora; Bomme, Cédric; Brouard, Mark; Burt, Michael; Christensen, Lauge; Düsterer, Stefan; Erk, Benjamin; Höppner, Hauke; Kierspel, Thomas; Krecinic, Faruk; Lauer, Alexandra; Lee, Jason W L; Müller, Maria; Müller, Erland; Mullins, Terence; Redlin, Harald; Schirmel, Nora; Thøgersen, Jan; Techert, Simone; Toleikis, Sven; Treusch, Rolf; Trippel, Sebastian; Ulmer, Anatoli; Vallance, Claire; Wiese, Joss; Johnsson, Per; Küpper, Jochen; Rudenko, Artem; Rouzée, Arnaud; Stapelfeldt, Henrik; Rolles, Daniel; Boll, Rebecca

2018-01-01

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon-iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. The results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

Biological tissue imaging with a position and time sensitive pixelated detector.

PubMed

Jungmann, Julia H; Smith, Donald F; MacAleese, Luke; Klinkert, Ivo; Visser, Jan; Heeren, Ron M A

2012-10-01

We demonstrate the capabilities of a highly parallel, active pixel detector for large-area, mass spectrometric imaging of biological tissue sections. A bare Timepix assembly (512 × 512 pixels) is combined with chevron microchannel plates on an ion microscope matrix-assisted laser desorption time-of-flight mass spectrometer (MALDI TOF-MS). The detector assembly registers position- and time-resolved images of multiple m/z species in every measurement frame. We prove the applicability of the detection system to biomolecular mass spectrometry imaging on biologically relevant samples by mass-resolved images from Timepix measurements of a peptide-grid benchmark sample and mouse testis tissue slices. Mass-spectral and localization information of analytes at physiologic concentrations are measured in MALDI-TOF-MS imaging experiments. We show a high spatial resolution (pixel size down to 740 × 740 nm(2) on the sample surface) and a spatial resolving power of 6 μm with a microscope mode laser field of view of 100-335 μm. Automated, large-area imaging is demonstrated and the Timepix' potential for fast, large-area image acquisition is highlighted.

Negative ion kinetics in RF glow discharges

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gottscho, R.A.; Gacbe, C.E.

1986-04-01

Using temporally and spatially resolved laser spectroscopy, the authors have determined the identities, approximate concentrations, effects on the local field, and kinetics of formation and loss of negative ions in RF discharges. CI/sup -/ and BCI/sub 3//sup -/ are the dominant negative ions found in low-frequency discharges through CI/sub 2/ and BCI/sub 3/, respectively. The electron affinity for CI is measured to be 3.6118 +- 0.0005 eV. Negative ion kinetics are strongly affected by application of the RF field. Formation of negative ions by attachment of slow electrons in RF discharges is governed by the extent and duration of electronmore » energy relaxation. Similarly, destruction of negative ions by collisional detachment and field extraction is dependent upon ion energy modulation. Thus, at low frequency, the anion density peaks at the beginning of the anodic and cathodic half-cycles after electrons have attached but before detachment and extraction have had time to occur. At higher frequencies, electrons have insufficient time to attach before they are reheated and the instantaneous anion density in the sheath is greatly reduced. When the negative ion density is comparable to the positive ion density, the plasma potential is observed to lie below the anode potential, double layers form between sheath and plasma, and anions and electrons are accelerated by large sheath fields to electrode surfaces.« less

The use of dopants in high field asymmetric waveform spectrometry.

PubMed

Ross, Stuart K; McDonald, Gwenda; Marchant, Sarah

2008-05-01

Ion mobility spectrometry (IMS) is proven core technology for the gas-phase detection of chemical warfare (CW) agents. One disadvantage of IMS technology is that ions of similar mobility cannot readily be resolved, resulting in false alarm responses and a loss of user confidence. High field asymmetric waveform spectrometry (HiFAWS) is an emerging technology for the gas-phase detection of CW agents. Of particular interest is the potential of a HiFAWS-based platform to reduce the number of false alarms by resolving ions that cannot be discriminated using IMS. It has been demonstrated that a water clustering/declustering mechanism can be a dominant process in HiFAWS. Ions that cannot be discriminated in IMS because they possess the same low field mobility value can be resolved using HiFAWS due to differences in the extent of low field ion solvation and high field ion desolvation. When operating in complex environments such as those potentially experienced in military and security arenas, IMS systems commonly employ internal dopants to reduce the number of background responses. It is possible that HiFAWS systems may also require the use of internal dopants for the same reason. It has been demonstrated that dopants employed for use in IMS may not be suitable for use in HiFAWS.

Signal processing for ION mobility spectrometers

NASA Technical Reports Server (NTRS)

Taylor, S.; Hinton, M.; Turner, R.

1995-01-01

Signal processing techniques for systems based upon Ion Mobility Spectrometry will be discussed in the light of 10 years of experience in the design of real-time IMS. Among the topics to be covered are compensation techniques for variations in the number density of the gas - the use of an internal standard (a reference peak) or pressure and temperature sensors. Sources of noise and methods for noise reduction will be discussed together with resolution limitations and the ability of deconvolution techniques to improve resolving power. The use of neural networks (either by themselves or as a component part of a processing system) will be reviewed.

Depth-resolved photo- and ionoluminescence of LiF and Al2O3

NASA Astrophysics Data System (ADS)

Skuratov, V. A.; Kirilkin, N. S.; Kovalev, Yu. S.; Strukova, T. S.; Havanscak, K.

2012-09-01

Microluminescence and laser confocal scanning microscopy techniques have been used to study spatial distribution of F-type color centers in LiF and mechanical stress profiles in Al2O3:Cr single crystals irradiated with 1.2 MeV/amu Ar, Kr, Xe and 3 MeV/amu Kr and Bi ions. It was found that F2 and F3+-center profiles at low ion fluences correlate with ionizing energy loss profiles. With increasing ion fluence, after ion track halo overlapping, the luminescence yield is defined by radiation defects formed in elastic collisions in the end-of-range area. Stress profiles and stress tensor components in ruby crystals across swift heavy ion irradiated layers have been deduced from depth-resolved photo-stimulated spectra using piezospectroscopic effect. Experimental data show that that stresses are compressive in basal plane and tensile in perpendicular direction in all samples irradiated with high energy ions.

Visualization of lithium-ion transport and phase evolution within and between manganese oxide nanorods.

PubMed

Xu, Feng; Wu, Lijun; Meng, Qingping; Kaltak, Merzuk; Huang, Jianping; Durham, Jessica L; Fernandez-Serra, Marivi; Sun, Litao; Marschilok, Amy C; Takeuchi, Esther S; Takeuchi, Kenneth J; Hybertsen, Mark S; Zhu, Yimei

2017-05-24

Multiple lithium-ion transport pathways and local phase changes upon lithiation in silver hollandite are revealed via in situ microscopy including electron diffraction, imaging and spectroscopy, coupled with density functional theory and phase field calculations. We report unexpected inter-nanorod lithium-ion transport, where the reaction fronts and kinetics are maintained within the neighbouring nanorod. Notably, this is the first time-resolved visualization of lithium-ion transport within and between individual nanorods, where the impact of oxygen deficiencies is delineated. Initially, fast lithium-ion transport is observed along the long axis with small net volume change, resulting in two lithiated silver hollandite phases distinguishable by orthorhombic distortion. Subsequently, a slower reaction front is observed, with formation of polyphase lithiated silver hollandite and face-centred-cubic silver metal with substantial volume expansion. These results indicate lithium-ion transport is not confined within a single nanorod and may provide a paradigm shift for one-dimensional tunnelled materials, particularly towards achieving high-rate capability.

Visualization of lithium-ion transport and phase evolution within and between manganese oxide nanorods

DOE PAGES

Xu, Feng; Wu, Lijun; Meng, Qingping; ...

2017-05-24

Multiple lithium-ion transport pathways and local phase changes upon lithiation in silver hollandite are revealed via in situ microscopy including electron diffraction, imaging and spectroscopy, coupled with density functional theory and phase field calculations. Here, we report unexpected inter-nanorod lithium-ion transport, where the reaction fronts and kinetics are maintained within the neighbouring nanorod. Notably, this is the first time-resolved visualization of lithium-ion transport within and between individual nanorods, where the impact of oxygen deficiencies is delineated. Initially, fast lithium-ion transport is observed along the long axis with small net volume change, resulting in two lithiated silver hollandite phases distinguishable bymore » orthorhombic distortion. As a result, a slower reaction front is observed, with formation of polyphase lithiated silver hollandite and face-centred-cubic silver metal with substantial volume expansion. Our results indicate lithium-ion transport is not confined within a single nanorod and may provide a paradigm shift for one-dimensional tunnelled materials, particularly towards achieving high-rate capability.« less

Visualization of lithium-ion transport and phase evolution within and between manganese oxide nanorods

DOE Office of Scientific and Technical Information (OSTI.GOV)

Xu, Feng; Wu, Lijun; Meng, Qingping

Multiple lithium-ion transport pathways and local phase changes upon lithiation in silver hollandite are revealed via in situ microscopy including electron diffraction, imaging and spectroscopy, coupled with density functional theory and phase field calculations. Here, we report unexpected inter-nanorod lithium-ion transport, where the reaction fronts and kinetics are maintained within the neighbouring nanorod. Notably, this is the first time-resolved visualization of lithium-ion transport within and between individual nanorods, where the impact of oxygen deficiencies is delineated. Initially, fast lithium-ion transport is observed along the long axis with small net volume change, resulting in two lithiated silver hollandite phases distinguishable bymore » orthorhombic distortion. As a result, a slower reaction front is observed, with formation of polyphase lithiated silver hollandite and face-centred-cubic silver metal with substantial volume expansion. Our results indicate lithium-ion transport is not confined within a single nanorod and may provide a paradigm shift for one-dimensional tunnelled materials, particularly towards achieving high-rate capability.« less

Observations of a field-aligned ion/ion-beam instability in a magnetized laboratory plasma

NASA Astrophysics Data System (ADS)

Heuer, P. V.; Weidl, M. S.; Dorst, R. S.; Schaeffer, D. B.; Bondarenko, A. S.; Tripathi, S. K. P.; Van Compernolle, B.; Vincena, S.; Constantin, C. G.; Niemann, C.; Winske, D.

2018-03-01

Collisionless coupling between super Alfvénic ions and an ambient plasma parallel to a background magnetic field is mediated by a set of electromagnetic ion/ion-beam instabilities including the resonant right hand instability (RHI). To study this coupling and its role in parallel shock formation, a new experimental configuration at the University of California, Los Angeles utilizes high-energy and high-repetition-rate lasers to create a super-Alfvénic field-aligned debris plasma within an ambient plasma in the Large Plasma Device. We used a time-resolved fluorescence monochromator and an array of Langmuir probes to characterize the laser plasma velocity distribution and density. The debris ions were observed to be sufficiently super-Alfvénic and dense to excite the RHI. Measurements with magnetic flux probes exhibited a right-hand circularly polarized frequency chirp consistent with the excitation of the RHI near the laser target. We compared measurements to 2D hybrid simulations of the experiment.

Observations of a field-aligned ion/ion-beam instability in a magnetized laboratory plasma

DOE PAGES

Heuer, P. V.; Weidl, M. S.; Dorst, R. S.; ...

2018-03-01

Collisionless coupling between super Alfvénic ions and an ambient plasma parallel to a background magnetic field is mediated by a set of electromagnetic ion/ion-beam instabilities including the resonant right hand instability (RHI). To study this coupling and its role in parallel shock formation, a new experimental configuration at the University of California, Los Angeles utilizes high-energy and high-repetition-rate lasers to create a super-Alfvénic field-aligned debris plasma within an ambient plasma in the Large Plasma Device. We used a time-resolved fluorescence monochromator and an array of Langmuir probes to characterize the laser plasma velocity distribution and density. The debris ions weremore » observed to be sufficiently super-Alfvénic and dense to excite the RHI. Measurements with magnetic flux probes exhibited a right-hand circularly polarized frequency chirp consistent with the excitation of the RHI near the laser target. To conclude, we compared measurements to 2D hybrid simulations of the experiment.« less

Observations of a field-aligned ion/ion-beam instability in a magnetized laboratory plasma

DOE Office of Scientific and Technical Information (OSTI.GOV)

Heuer, P. V.; Weidl, M. S.; Dorst, R. S.

Collisionless coupling between super Alfvénic ions and an ambient plasma parallel to a background magnetic field is mediated by a set of electromagnetic ion/ion-beam instabilities including the resonant right hand instability (RHI). To study this coupling and its role in parallel shock formation, a new experimental configuration at the University of California, Los Angeles utilizes high-energy and high-repetition-rate lasers to create a super-Alfvénic field-aligned debris plasma within an ambient plasma in the Large Plasma Device. We used a time-resolved fluorescence monochromator and an array of Langmuir probes to characterize the laser plasma velocity distribution and density. The debris ions weremore » observed to be sufficiently super-Alfvénic and dense to excite the RHI. Measurements with magnetic flux probes exhibited a right-hand circularly polarized frequency chirp consistent with the excitation of the RHI near the laser target. To conclude, we compared measurements to 2D hybrid simulations of the experiment.« less

Ion Mobility Separation of Isomeric Carbohydrate Precursor Ions and Acquisition of their Independent Tandem Mass Spectra

PubMed Central

Zhu, Maolei; Bendiak, Brad; Clowers, Brian; Hill, Herbert H.

2010-01-01

The rapid separation of isomeric precursor ions of oligosaccharides prior to their analysis by MSn was demonstrated using an ambient pressure ion mobility spectrometer (IMS) interfaced with a quadrupole ion trap. Separations were not limited to specific types of isomers; representative isomers differing solely in the stereochemistry of sugars, in their anomeric configurations, and in their overall branching patterns and linkage positions could be resolved in the millisecond time frame. Physical separation of precursor ions permitted independent mass spectra of individual oligosaccharide isomers to be acquired to at least MS3, the number of stages of dissociation limited only practically by the abundance of specific product ions. IMS-MSn analysis was particularly valuable in the evaluation of isomeric oligosaccharides that yielded identical sets of product ions in MS/MS experiments, revealing pairs of isomers that would otherwise not be known to be present in a mixture if evaluated solely by MS dissociation methods alone. A practical example of IMS-MSn analysis of a set of isomers included within a single HPLC fraction of oligosaccharides released from bovine submaxillary mucin is described. PMID:19562326

Energy Transfer Efficiency from ZnO-Nanocrystals to Eu3+ Ions Embedded in SiO₂ Film for Emission at 614 nm.

PubMed

Mangalam, Vivek; Pita, Kantisara

2017-08-10

In this work, we study the energy transfer mechanism from ZnO nanocrystals (ZnO-nc) to Eu 3+ ions by fabricating thin-film samples of ZnO-nc and Eu 3+ ions embedded in a SiO₂ matrix using the low-cost sol-gel technique. The time-resolved photoluminescence (TRPL) measurements from the samples were analyzed to understand the contribution of energy transfer from the various ZnO-nc emission centers to Eu 3+ ions. The decay time obtained from the TRPL measurements was used to calculate the energy transfer efficiencies from the ZnO-nc emission centers, and these results were compared with the energy transfer efficiencies calculated from steady-state photoluminescence emission results. The results in this work show that high transfer efficiencies from the excitonic and Zn defect emission centers is mostly due to the energy transfer from ZnO-nc to Eu 3+ ions which results in the radiative emission from the Eu 3+ ions at 614 nm, while the energy transfer from the oxygen defect emissions is most probably due to the energy transfer from ZnO-nc to the new defects created due to the incorporation of the Eu 3+ ions.

Detection of Reaction Intermediates in Mg2+-Dependent DNA Synthesis and RNA Degradation by Time-Resolved X-Ray Crystallography.

PubMed

Samara, Nadine L; Gao, Yang; Wu, Jinjun; Yang, Wei

2017-01-01

Structures of enzyme-substrate/product complexes have been studied for over four decades but have been limited to either before or after a chemical reaction. Recently using in crystallo catalysis combined with X-ray diffraction, we have discovered that many enzymatic reactions in nucleic acid metabolism require additional metal ion cofactors that are not present in the substrate or product state. By controlling metal ions essential for catalysis, the in crystallo approach has revealed unprecedented details of reaction intermediates. Here we present protocols used for successful studies of Mg 2+ -dependent DNA polymerases and ribonucleases that are applicable to analyses of a variety of metal ion-dependent reactions. © 2017 Elsevier Inc. All rights reserved.

Exciplex formation in bimolecular photoinduced electron-transfer investigated by ultrafast time-resolved infrared spectroscopy.

PubMed

Koch, Marius; Letrun, Romain; Vauthey, Eric

2014-03-12

The dynamics of bimolecular photoinduced electron-transfer reactions has been investigated with three donor/acceptor (D/A) pairs in tetrahydrofuran (THF) and acetonitrile (ACN) using a combination of ultrafast spectroscopic techniques, including time-resolved infrared absorption. For the D/A pairs with the highest driving force of electron transfer, all transient spectroscopic features can be unambiguously assigned to the excited reactant and the ionic products. For the pair with the lowest driving force, three additional transient infrared bands, more intense in THF than in ACN, with a time dependence that differs from those of the other bands are observed. From their frequency and solvent dependence, these bands can be assigned to an exciplex. Moreover, polarization-resolved measurements point to a relatively well-defined mutual orientation of the constituents and to a slower reorientational time compared to those of the individual reactants. Thanks to the minimal overlap of the infrared signature of all transient species in THF, a detailed reaction scheme including the relevant kinetic and thermodynamic parameters could be deduced for this pair. This analysis reveals that the formation and recombination of the ion pair occur almost exclusively via the exciplex.

Determination of nonlinear optical properties by time resolved Z-scan in Nd-doped phosphate glass

NASA Astrophysics Data System (ADS)

de Souza, J. M.; de Lima, W. J.; Pilla, V.; Andrade, A. A.; Dantas, N. O.; Messias, D. N.

2017-02-01

In this work, we have used a Ti3+:Safira laser tuned at 803nm to performed time-resolved measurements using the Z-scan technique to characterize the nonlinear optical properties of phosphate glasses. The glass matrices, labeled PAN (P2O5-Al2O3-Na2CO3) and PANK (P2O5-Al2O3- Na2O-K2O), were doped with increasing Nd3+ concentration, ranging from 0.5 to 5 wt%. For both systems, we have seen that the optical nonlinearity has a linear dependence with the doping ion concentration. Therefore, we propose a new approach to obtain the parameters Δα and Δσ. All results obtained are in good agreement with others found in the literature.

How to resolve microsecond current fluctuations in single ion channels: The power of beta distributions

PubMed Central

Schroeder, Indra

2015-01-01

Abstract A main ingredient for the understanding of structure/function correlates of ion channels is the quantitative description of single-channel gating and conductance. However, a wealth of information provided from fast current fluctuations beyond the temporal resolution of the recording system is often ignored, even though it is close to the time window accessible to molecular dynamics simulations. This kind of current fluctuations provide a special technical challenge, because individual opening/closing or blocking/unblocking events cannot be resolved, and the resulting averaging over undetected events decreases the single-channel current. Here, I briefly summarize the history of fast-current fluctuation analysis and focus on the so-called “beta distributions.” This tool exploits characteristics of current fluctuation-induced excess noise on the current amplitude histograms to reconstruct the true single-channel current and kinetic parameters. A guideline for the analysis and recent applications demonstrate that a construction of theoretical beta distributions by Markov Model simulations offers maximum flexibility as compared to analytical solutions. PMID:26368656

Time-resolved spectroscopy of solid poly/1-vinyl naphthalene/ following electron beam pulse radiolysis - Pulse radiolytic studies on polymers

NASA Technical Reports Server (NTRS)

Coulter, D. R.; Liang, R. H.; Di Stefano, S.; Moacanin, J.; Gupta, A.

1982-01-01

Transient emission studies following pulse radiolysis of solid poly(1-vinyl naphthalene) show existence of excited monomers and two excimers. Quenching experiments indicate that excimers are not formed directly by recombination of ions but probably by trapping of migrating monomeric excitation in preformed traps whose density is approximately one in 1000.

Time resolved impedance spectroscopy analysis of lithium phosphorous oxynitride - LiPON layers under mechanical stress

NASA Astrophysics Data System (ADS)

Glenneberg, Jens; Bardenhagen, Ingo; Langer, Frederieke; Busse, Matthias; Kun, Robert

2017-08-01

In this paper we present investigations on the morphological and electrochemical changes of lithium phosphorous oxynitride (LiPON) under mechanically bent conditions. Therefore, two types of electrochemical cells with LiPON thin films were prepared by physical vapor deposition. First, symmetrical cells with two blocking electrodes (Cu/LiPON/Cu) were fabricated. Second, to simulate a more application-related scenario cells with one blocking and one non-blocking electrode (Cu/LiPON/Li/Cu) were analyzed. In order to investigate mechanical distortion induced transport property changes in LiPON layers the cells were deposited on a flexible polyimide substrate. Morphology of the as-prepared samples and deviations from the initial state after applying external stress by bending the cells over different radii were investigated by Focused Ion Beam- Scanning Electron Microscopy (FIB-SEM) cross-section and surface images. Mechanical stress induced changes in the impedance were evaluated by time-resolved electrochemical impedance spectroscopy (EIS). Due to the formation of a stable, ion-conducting solid electrolyte interphase (SEI), cells with lithium show decreased impedance values. Furthermore, applying mechanical stress to the cells results in a further reduction of the electrolyte resistance. These results are supported by finite element analysis (FEA) simulations.

Microplasma array patterning of reactive oxygen and nitrogen species onto polystyrene

NASA Astrophysics Data System (ADS)

Szili, Endre J.; Dedrick, James; Oh, Jun-Seok; Bradley, James W.; Boswell, Roderick W.; Charles, Christine; Short, Robert D.; Al-Bataineh, Sameer A.

2017-02-01

We investigate an approach for the patterning of reactive oxygen and nitrogen species (RONS) onto polystyrene using atmospheric-pressure microplasma arrays. The spectrally integrated and time-resolved optical emission from the array is characterised with respect to the applied voltage, applied-voltage frequency and pressure; and the array is used to achieve spatially resolved modification of polystyrene at three pressures: 500 Torr, 760 Torr and 1000 Torr. As determined by time-of-flight secondary ion mass spectrometry (ToF-SIMS), regions over which surface modification occurs are clearly restricted to areas that are exposed to individual microplasma cavities. Analysis of the negative-ion ToF-SIMS mass spectra from the centre of the modified microspots shows that the level of oxidation is dependent on the operating pressure, and closely correlated with the spatial distribution of the optical emission. The functional groups that are generated by the microplasma array on the polystyrene surface are shown to readily participate in an oxidative reaction in phosphate buffered saline solution (pH 7.4). Patterns of oxidised and chemically reactive functionalities could potentially be applied to the future development of biomaterial surfaces, where spatial control over biomolecule or cell function is needed.

Terahertz-Radiation-Enhanced Emission of Fluorescence from Gas Plasma

NASA Astrophysics Data System (ADS)

Liu, Jingle; Zhang, X.-C.

2009-12-01

We report the study of femtosecond laser-induced air plasma fluorescence under the illumination of terahertz (THz) pulses. Semiclassical modeling and experimental verification indicate that time-resolved THz radiation-enhanced emission of fluorescence is dominated by the electron kinetics and the electron-impact excitation of gas molecules or ions. We demonstrate that the temporal waveform of the THz field could be retrieved from the transient enhanced fluorescence, making omnidirectional, coherent detection available for THz time-domain spectroscopy.

Fast Orthogonal Separation by Superposition of Time of Flight and Field Asymmetric Ion Mobility Spectrometry.

PubMed

Bohnhorst, Alexander; Kirk, Ansgar T; Berger, Marc; Zimmermann, Stefan

2018-01-16

Ion mobility spectrometry is a powerful and low-cost technique for the identification of chemical warfare agents, toxic chemicals, or explosives in air. Drift tube ion mobility spectrometers (DT-IMS) separate ions by the absolute value of their low field ion mobility, while field asymmetric ion mobility spectrometers (FAIMS) separate them by the change of their ion mobility at high fields. However, using one of these devices alone, some common and harmless substances show the same response as the hazardous target substances. In order to increase the selectivity, orthogonal data are required. Thus, in this work, we present for the first time an ambient pressure ion mobility spectrometer which is able to separate ions both by their differential and low field mobility, providing additional information for selectivity enhancement. This novel field asymmetric time of flight ion mobility spectrometer (FAT-IMS) allows high repetition rates and reaches limits of detection in the low ppb range common for DT-IMS. The device consists of a compact 44 mm drift tube with a tritium ionization source and a resolving power of 70. An increased separation of four substances with similar low field ion mobility is shown: phosgene (K 0 = 2.33 cm 2 /(V s)), 1,1,2-trichlorethane (K 0 = 2.31 cm 2 /(V s)), chlorine (K 0 = 2.24 cm 2 /(V s)), and nitrogen dioxide (K 0 = 2.25 cm 2 /(V s)). Furthermore, the behavior and limits of detection for acetonitrile, dimethyl methylphosphonate, diisopropyl methyl phosphonate in positive polarity and carbon dioxide, sulfur dioxide, hydrochloric acid, cyanogen chloride, and hydrogen cyanide in negative polarity are investigated.

Observations of strong ion-ion correlations in dense plasmas

DOE PAGES

Ma, T.; Fletcher, L.; Pak, A.; ...

2014-04-24

Using simultaneous spectrally, angularly, and temporally resolved x-ray scattering, we measure the pronounced ion-ion correlation peak in a strongly coupled plasma. Laser-driven shock-compressed aluminum at ~3× solid density is probed with high-energy photons at 17.9 keV created by molybdenum He-α emission in a laser-driven plasma source. The measured elastic scattering feature shows a well-pronounced correlation peak at a wave vector of k=4Å –1. The magnitude of this correlation peak cannot be described by standard plasma theories employing a linear screened Coulomb potential. Advanced models, including a strong short-range repulsion due to the inner structure of the aluminum ions are howevermore » in good agreement with the scattering data. These studies have demonstrated a new highly accurate diagnostic technique to directly measure the state of compression and the ion-ion correlations. Furthermore, we have since applied this new method in single-shot wave-number resolved S(k) measurements to characterize the physical properties of dense plasmas.« less

Origin of Blue-Green Emission in α-Zn2P2O7 and Local Structure of Ln3+ Ion in α-Zn2P2O7:Ln3+ (Ln = Sm, Eu): Time-Resolved Photoluminescence, EXAFS, and DFT Measurements.

PubMed

Gupta, Santosh Kumar; Ghosh, Partha Sarathi; Yadav, Ashok Kumar; Jha, Shambhu Nath; Bhattacharyya, Dibyendu; Kadam, Ramakant Mahadeo

2017-01-03

Considering the fact that pyrophosphate-based hosts are in high demand for making highly efficient luminescence materials, we doped two visible lanthanide ions, viz. Sm 3+ and Eu 3+ , in Zn 2 P 2 O 7 . Interestingly, it was oberved that pure Zn 2 P 2 O 7 displayed blue-green dual emission on irradiation with ultraviolet light. Emission and lifetime spectroscopy shows the presence of defects in pyrophosphate samples which are responsible for such emission. DFT calculations clearly pinpointed that the electronic transitions between defect states located at just below the conduction band minimum (arises due to V O 1+ and V O 2+ defects) and valence band maximum, as well as impurity states situated in the band gap, can lead to dual emission in the blue-green region, as is also indicated by emission and lifetime spectra. X-ray absorption near edge spectroscopy (XANES) shows the stabilization of europium as well as samarium ion in the +3 oxidation state in α-Zn 2 P 2 O 7 . The fact that α-Zn 2 P 2 O 7 has two different coordination numbers for zinc ions, i.e. five- and six-coordinate, the study of dopant ion distribution in this particular matrix will be an important step in realizing a highly efficient europium- and samarium-based red-emitting phosphor. Time resolved photoluminescence (TRPL) shows that both of these ions are heterogeneously distributed between five- and six-coordinated Zn 2+ sites and it is the six-coordinated Zn 2+ site which is the most favorable for lanthanide ion doping. Extended X-ray absorption fine structure (EXAFS) measurements also suggested that a six-coordinated zinc ion is the preferred site occupied by trivalent lanthanide ions, which is in complete agreement with TRPL results. It was observed that there is almost complete transfer of photon energy from Zn 2 P 2 O 7 to Eu 3+ , whereas this transfer is inefficient and almost incomplete in case of Sm 3+ , which is indeed important information for the realization of pyrophosphate-based tunable phosphors.

A compact high resolution ion mobility spectrometer for fast trace gas analysis.

PubMed

Kirk, Ansgar T; Allers, Maria; Cochems, Philipp; Langejuergen, Jens; Zimmermann, Stefan

2013-09-21

Drift tube ion mobility spectrometers (IMS) are widely used for fast trace gas detection in air, but portable compact systems are typically very limited in their resolving power. Decreasing the initial ion packet width improves the resolution, but is generally associated with a reduced signal-to-noise-ratio (SNR) due to the lower number of ions injected into the drift region. In this paper, we present a refined theory of IMS operation which employs a combined approach for the analysis of the ion drift and the subsequent amplification to predict both the resolution and the SNR of the measured ion current peak. This theoretical analysis shows that the SNR is not a function of the initial ion packet width, meaning that compact drift tube IMS with both very high resolution and extremely low limits of detection can be designed. Based on these implications, an optimized combination of a compact drift tube with a length of just 10 cm and a transimpedance amplifier has been constructed with a resolution of 183 measured for the positive reactant ion peak (RIP(+)), which is sufficient to e.g. separate the RIP(+) from the protonated acetone monomer, even though their drift times only differ by a factor of 1.007. Furthermore, the limits of detection (LODs) for acetone are 180 pptv within 1 s of averaging time and 580 pptv within only 100 ms.

Ion beam enhancement in magnetically insulated ion diodes for high-intensity pulsed ion beam generation in non-relativistic mode

NASA Astrophysics Data System (ADS)

Zhu, X. P.; Zhang, Z. C.; Pushkarev, A. I.; Lei, M. K.

2016-01-01

High-intensity pulsed ion beam (HIPIB) with ion current density above Child-Langmuir limit is achieved by extracting ion beam from anode plasma of ion diodes with suppressing electron flow under magnetic field insulation. It was theoretically estimated that with increasing the magnetic field, a maximal value of ion current density may reach nearly 3 times that of Child-Langmuir limit in a non-relativistic mode and close to 6 times in a highly relativistic mode. In this study, the behavior of ion beam enhancement by magnetic insulation is systematically investigated in three types of magnetically insulated ion diodes (MIDs) with passive anode, taking into account the anode plasma generation process on the anode surface. A maximal enhancement factor higher than 6 over the Child-Langmuir limit can be obtained in the non-relativistic mode with accelerating voltage of 200-300 kV. The MIDs differ in two anode plasma formation mechanisms, i.e., surface flashover of a dielectric coating on the anode and explosive emission of electrons from the anode, as well as in two insulation modes of external-magnetic field and self-magnetic field with either non-closed or closed drift of electrons in the anode-cathode (A-K) gap, respectively. Combined with ion current density measurement, energy density characterization is employed to resolve the spatial distribution of energy density before focusing for exploring the ion beam generation process. Consistent results are obtained on three types of MIDs concerning control of neutralizing electron flows for the space charge of ions where the high ion beam enhancement is determined by effective electron neutralization in the A-K gap, while the HIPIB composition of different ion species downstream from the diode may be considerably affected by the ion beam neutralization during propagation.

The magnetic recoil spectrometer (MRSt) for time-resolved measurements of the neutron spectrum at the National Ignition Facility (NIF)

DOE PAGES

Frenje, J. A.; Hilsabeck, T. J.; Wink, C. W.; ...

2016-08-02

The next-generation magnetic recoil spectrometer for time-resolved measurements of the neutron spectrum has been conceptually designed for the National Ignition Facility. This spectrometer, called MRSt, represents a paradigm shift in our thinking about neutron spectrometry for inertial confinement fusion applications, as it will provide simultaneously information about the burn history and time evolution of areal density (ρR), apparent ion temperature (T i), yield (Y n), and macroscopic flows during burn. From this type of data, an assessment of the evolution of the fuel assembly, hotspot, and alpha heating can be made. According to simulations, the MRSt will provide accurate datamore » with a time resolution of ~20 ps and energy resolution of ~100 keV for total neutron yields above ~10 16. Lastly, at lower yields, the diagnostic will be operated at a higher-efficiency, lower-energy-resolution mode to provide a time resolution of ~20 ps.« less

The magnetic recoil spectrometer (MRSt) for time-resolved measurements of the neutron spectrum at the National Ignition Facility (NIF).

PubMed

Frenje, J A; Hilsabeck, T J; Wink, C W; Bell, P; Bionta, R; Cerjan, C; Gatu Johnson, M; Kilkenny, J D; Li, C K; Séguin, F H; Petrasso, R D

2016-11-01

The next-generation magnetic recoil spectrometer for time-resolved measurements of the neutron spectrum has been conceptually designed for the National Ignition Facility. This spectrometer, called MRSt, represents a paradigm shift in our thinking about neutron spectrometry for inertial confinement fusion applications, as it will provide simultaneously information about the burn history and time evolution of areal density (ρR), apparent ion temperature (T i ), yield (Y n ), and macroscopic flows during burn. From this type of data, an assessment of the evolution of the fuel assembly, hotspot, and alpha heating can be made. According to simulations, the MRSt will provide accurate data with a time resolution of ∼20 ps and energy resolution of ∼100 keV for total neutron yields above ∼10 16 . At lower yields, the diagnostic will be operated at a higher-efficiency, lower-energy-resolution mode to provide a time resolution of ∼20 ps.

The magnetic recoil spectrometer (MRSt) for time-resolved measurements of the neutron spectrum at the National Ignition Facility (NIF)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Frenje, J. A., E-mail: jfrenje@psfc.mit.edu; Wink, C. W.; Gatu Johnson, M.

The next-generation magnetic recoil spectrometer for time-resolved measurements of the neutron spectrum has been conceptually designed for the National Ignition Facility. This spectrometer, called MRSt, represents a paradigm shift in our thinking about neutron spectrometry for inertial confinement fusion applications, as it will provide simultaneously information about the burn history and time evolution of areal density (ρR), apparent ion temperature (T{sub i}), yield (Y{sub n}), and macroscopic flows during burn. From this type of data, an assessment of the evolution of the fuel assembly, hotspot, and alpha heating can be made. According to simulations, the MRSt will provide accurate datamore » with a time resolution of ∼20 ps and energy resolution of ∼100 keV for total neutron yields above ∼10{sup 16}. At lower yields, the diagnostic will be operated at a higher-efficiency, lower-energy-resolution mode to provide a time resolution of ∼20 ps.« less

Investigation of temporal-resolved emission spectra of highly charged Al ions from laser-produced plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Su, M. G., E-mail: sumg@nwnu.edu.cn; Sun, D. X.; Dong, C. Z.

2016-03-15

Temporal evolution of extreme ultraviolet emission from laser-produced aluminum (Al) plasma has been experimentally and theoretically investigated. Al plasmas have been measured by using the temporal-spatially resolved laser-produced plasma technique. The emission lines can be identified from 2p-3s, 3d, 4s, 4d, 5d transition lines from Al{sup 3+} to Al{sup 6+} ions. In order to quickly diagnose the plasma, the assumptions of a normalized Boltzmann distribution among the excited states and a steady-state collisional-radiative model are used to estimate the values of electron temperature and electron density in plasma. We succeeded in reproducing the simulated spectra related to the different timemore » delays, which are in good agreement with experiments. Temporal evolution behavior of highly charged Al ions in plasma has been analyzed, and the exponential decay about electron temperature and electron density has been obtained. The results indicate that the temporal-spatially resolved measurement is essential for accurate understanding of evolution behavior of highly charged ions in laser-produced plasmas.« less

Time- and Space-Resolved SAXS Experiments Inform on Phase Transition Kinetics in Hydrated, Liquid-Crystalline Films of Polyion-Surfactant Ion "Complex Salts".

PubMed

Li, Joaquim; Gustavsson, Charlotte; Piculell, Lennart

2016-05-24

Detailed time- and space-resolved SAXS experiments show the variation with hydration of liquid crystalline structures in ethanol-cast 5-80 μm thick films of polyion-surfactant ion "complex salts" (CS). The CS were dodecyl- (C12) or hexadecyl- (C16) trimethylammonium surfactants with polyacrylate (DP 25 or 6000) counter-polyions. The experiments were carried out on vertical films in humid air above a movable water bath, so that gradients of hydration were generated, which could rapidly be altered. Scans over different positions along a film, kept fixed relative to the bath, showed that the surfactant aggregates of the various liquid-crystalline CS structures grow in cross-sectional area with decreasing hydration. This behavior is attributed to the low water content. Studies of films undergoing rapid dehydration, made possible by the original experimental setup, gave strong evidence that some of the investigated systems remain kinetically trapped for minutes in a nonequilibrium Pm3n micellar cubic phase before switching to the equilibrium P6mm 2D hexagonal phase. Both the length of the polyion and the length of the surfactant hydrocarbon "tail" affect the kinetics of the phase transition. The slowness of the cubic-to-hexagonal structural transition is attributed to the fact that it requires major rearrangements of the polyions and surfactant ions relative to each other. By contrast, other structure changes, such as between the hexagonal and rectangular phases, were observed to occur much more rapidly.

Radiobiological study by using laser-driven proton beams

NASA Astrophysics Data System (ADS)

Yogo, A.; Sato, K.; Nishikino, M.; Mori, M.; Teshima, T.; Numasaki, H.; Murakami, M.; Demizu, Y.; Akagi, S.; Nagayama, S.; Ogura, K.; Sagisaka, A.; Orimo, S.; Nishiuchi, M.; Pirozhkov, A. S.; Ikegami, M.; Tampo, M.; Sakaki, H.; Suzuki, M.; Daito, I.; Oishi, Y.; Sugiyama, H.; Kiriyama, H.; Okada, H.; Kanazawa, S.; Kondo, S.; Shimomura, T.; Nakai, Y.; Tanoue, M.; Sugiyama, H.; Sasao, H.; Wakai, D.; Kawachi, T.; Nishimura, H.; Bolton, P. R.; Daido, H.

2009-07-01

Particle acceleration driven by high-intensity laser systems is widely attracting interest as a potential alternative to conventional ion acceleration, including ion accelerator applications to tumor therapy. Recent works have shown that a high intensity laser pulse can produce single proton bunches of a high current and a short pulse duration. This unique feature of laser-ion acceleration can lead to progress in the development of novel ion sources. However, there has been no experimental study of the biological effects of laser-driven ion beams. We describe in this report the first demonstrated irradiation effect of laser-accelerated protons on human lung cancer cells. In-vitro A549 cells are irradiated with a proton dose of 20 Gy, resulting in a distinct formation of γ-H2AX foci as an indicator of DNA double-strand breaks. This is a pioneering result that points to future investigations of the radiobiological effects of laser-driven ion beams. The laser-driven ion beam is apotential excitation source for time-resolved determination of hydroxyl (OH) radical yield, which will explore relationship between the fundamental chemical reactions of radiation effects and consequent biological processes.

Determination of ion mobility collision cross sections for unresolved isomeric mixtures using tandem mass spectrometry and chemometric deconvolution.

PubMed

Harper, Brett; Neumann, Elizabeth K; Stow, Sarah M; May, Jody C; McLean, John A; Solouki, Touradj

2016-10-05

Ion mobility (IM) is an important analytical technique for determining ion collision cross section (CCS) values in the gas-phase and gaining insight into molecular structures and conformations. However, limited instrument resolving powers for IM may restrict adequate characterization of conformationally similar ions, such as structural isomers, and reduce the accuracy of IM-based CCS calculations. Recently, we introduced an automated technique for extracting "pure" IM and collision-induced dissociation (CID) mass spectra of IM overlapping species using chemometric deconvolution of post-IM/CID mass spectrometry (MS) data [J. Am. Soc. Mass Spectrom., 2014, 25, 1810-1819]. Here we extend those capabilities to demonstrate how extracted IM profiles can be used to calculate accurate CCS values of peptide isomer ions which are not fully resolved by IM. We show that CCS values obtained from deconvoluted IM spectra match with CCS values measured from the individually analyzed corresponding peptides on uniform field IM instrumentation. We introduce an approach that utilizes experimentally determined IM arrival time (AT) "shift factors" to compensate for ion acceleration variations during post-IM/CID and significantly improve the accuracy of the calculated CCS values. Also, we discuss details of this IM deconvolution approach and compare empirical CCS values from traveling wave (TW)IM-MS and drift tube (DT)IM-MS with theoretically calculated CCS values using the projected superposition approximation (PSA). For example, experimentally measured deconvoluted TWIM-MS mean CCS values for doubly-protonated RYGGFM, RMFGYG, MFRYGG, and FRMYGG peptide isomers were 288.8 Å(2), 295.1 Å(2), 296.8 Å(2), and 300.1 Å(2); all four of these CCS values were within 1.5% of independently measured DTIM-MS values. Copyright © 2016 Elsevier B.V. All rights reserved.

Highly Charged Rydberg Ions from the Coulomb Explosion of Clusters

NASA Astrophysics Data System (ADS)

Komar, D.; Kazak, L.; Almassarani, M.; Meiwes-Broer, K.-H.; Tiggesbäumker, J.

2018-03-01

Ion emission from a nanoplasma produced in the interaction of intense optical laser pulses with argon clusters is studied resolving simultaneously charge states and recoil energies. By applying appropriate static electric fields we observe that a significant fraction of the ions Arq + (q =1 - 7 ) has electrons with binding energies lower than 150 meV; i.e., nRyd≥15 levels are populated. Charge state changes observed on a μ s time scale can be attributed to electron emission due to autoionizing Rydberg states, indicating that high-ℓ Rydberg levels are populated as well. The experiments support theoretical predictions that a significant fraction of delocalized electrons, which are bound with hundreds of eV to the nanoplasma after the laser exposure, fill up meV bound ion states in the adiabatic expansion. We expect the process to be relevant for the long-term evolution of expanding laser-induced dense plasmas in general.

Numerical simulation of filling a magnetic flux tube with a cold plasma: Anomalous plasma effects

NASA Technical Reports Server (NTRS)

Singh, Nagendra; Leung, W. C.

1995-01-01

Large-scale models of plasmaspheric refilling have revealed that during the early stage of the refilling counterstreaming ion beams are a common feature. However, the instability of such ion beams and its effect on refilling remain unexplored. In order to learn the basic effects of ion beam instabilities on refilling, we have performed numerical simulations of the refilling of an artificial magnetic flux tube. (The shape and size of the tube are assumed so that the essential features of the refilling problem are kept in the simulation and at the same time the small scale processes driven by the ion beams are sufficiently resolved.) We have also studied the effect of commonly found equatorially trapped warm and/or hot plasma on the filling of a flux tube with a cold plasma. Three types of simulation runs have been performed.

The role of Nb in intensity increase of Er ion upconversion luminescence in zirconia

DOE Office of Scientific and Technical Information (OSTI.GOV)

Smits, K., E-mail: smits@cfi.lu.lv; Sarakovskis, A.; Grigorjeva, L.

2014-06-07

It is found that Nb co-doping increases the luminescence and upconversion luminescence intensity in rare earth doped zirconia. Er and Yb-doped nanocrystalline samples with or without Nb co-doping were prepared by sol-gel method and thermally annealed to check for the impact of phase transition on luminescence properties. Phase composition and grain sizes were examined by X-ray diffraction; the morphology was checked by scanning- and high-resolution transmission electron microscopes. Both steady-state and time-resolved luminescence were studied. Comparison of samples with different oxygen vacancy concentrations and different Nb concentrations confirmed the known assumption that oxygen vacancies are the main agents for tetragonalmore » or cubic phase stabilization. The oxygen vacancies quench the upconversion luminescence; however, they also prevent agglomeration of rare-earth ions and/or displacement of rare-earth ions to grain surfaces. It is found that co-doping with Nb ions significantly (>20 times) increases upconversion luminescence intensity. Hence, ZrO{sub 2}:Er:Yb:Nb nanocrystals may show promise for upconversion applications.« less

Statistical precision of the intensities retrieved from constrained fitting of overlapping peaks in high-resolution mass spectra

DOE PAGES

Cubison, M. J.; Jimenez, J. L.

2015-06-05

Least-squares fitting of overlapping peaks is often needed to separately quantify ions in high-resolution mass spectrometer data. A statistical simulation approach is used to assess the statistical precision of the retrieved peak intensities. The sensitivity of the fitted peak intensities to statistical noise due to ion counting is probed for synthetic data systems consisting of two overlapping ion peaks whose positions are pre-defined and fixed in the fitting procedure. The fitted intensities are sensitive to imperfections in the m/Q calibration. These propagate as a limiting precision in the fitted intensities that may greatly exceed the precision arising from counting statistics.more » The precision on the fitted peak intensity falls into one of three regimes. In the "counting-limited regime" (regime I), above a peak separation χ ~ 2 to 3 half-widths at half-maximum (HWHM), the intensity precision is similar to that due to counting error for an isolated ion. For smaller χ and higher ion counts (~ 1000 and higher), the intensity precision rapidly degrades as the peak separation is reduced ("calibration-limited regime", regime II). Alternatively for χ < 1.6 but lower ion counts (e.g. 10–100) the intensity precision is dominated by the additional ion count noise from the overlapping ion and is not affected by the imprecision in the m/Q calibration ("overlapping-limited regime", regime III). The transition between the counting and m/Q calibration-limited regimes is shown to be weakly dependent on resolving power and data spacing and can thus be approximated by a simple parameterisation based only on peak intensity ratios and separation. A simple equation can be used to find potentially problematic ion pairs when evaluating results from fitted spectra containing many ions. Longer integration times can improve the precision in regimes I and III, but a given ion pair can only be moved out of regime II through increased spectrometer resolving power. As a result, studies presenting data obtained from least-squares fitting procedures applied to mass spectral peaks should explicitly consider these limits on statistical precision.« less

Quantifying Fusion Born Ion Populations in Magnetically Confined Plasmas using Ion Cyclotron Emission

DOE PAGES

Carbajal, L.; Warwick Univ., Coventry; Dendy, R. O.; ...

2017-03-07

Ion cyclotron emission (ICE) offers unique promise as a diagnostic of the fusion born alpha-particle population in magnetically confined plasmas. Pioneering observations from JET and TFTR found that ICE intensity P ICE scales approximately linearly with the measured neutron flux from fusion reactions, and with the inferred concentration, n /n i , of fusion-born alpha-particles confined within the plasma. We present fully nonlinear self-consistent kinetic simulations that reproduce this scaling for the first time. This resolves a longstanding question in the physics of fusion alpha particle confinement and stability in MCF plasmas. It confirms the MCI as the likely emissionmore » mechanism and greatly strengthens the basis for diagnostic exploitation of ICE in future burning plasmas.« less

Quantifying Fusion Born Ion Populations in Magnetically Confined Plasmas using Ion Cyclotron Emission

NASA Astrophysics Data System (ADS)

Carbajal, L.; Dendy, R. O.; Chapman, S. C.; Cook, J. W. S.

2017-03-01

Ion cyclotron emission (ICE) offers a unique promise as a diagnostic of the fusion born alpha-particle population in magnetically confined plasmas. Pioneering observations from JET and TFTR found that ICE intensity PICE scales approximately linearly with the measured neutron flux from fusion reactions, and with the inferred concentration, nα/ni, of fusion born alpha particles confined within the plasma. We present fully nonlinear self-consistent kinetic simulations that reproduce this scaling for the first time. This resolves a long-standing question in the physics of fusion alpha-particle confinement and stability in magnetic confinement fusion plasmas. It confirms the magnetoacoustic cyclotron instability as the likely emission mechanism and greatly strengthens the basis for diagnostic exploitation of ICE in future burning plasmas.

Quantifying Fusion Born Ion Populations in Magnetically Confined Plasmas using Ion Cyclotron Emission.

PubMed

Carbajal, L; Dendy, R O; Chapman, S C; Cook, J W S

2017-03-10

Ion cyclotron emission (ICE) offers a unique promise as a diagnostic of the fusion born alpha-particle population in magnetically confined plasmas. Pioneering observations from JET and TFTR found that ICE intensity P_{ICE} scales approximately linearly with the measured neutron flux from fusion reactions, and with the inferred concentration, n_{α}/n_{i}, of fusion born alpha particles confined within the plasma. We present fully nonlinear self-consistent kinetic simulations that reproduce this scaling for the first time. This resolves a long-standing question in the physics of fusion alpha-particle confinement and stability in magnetic confinement fusion plasmas. It confirms the magnetoacoustic cyclotron instability as the likely emission mechanism and greatly strengthens the basis for diagnostic exploitation of ICE in future burning plasmas.

Short intense ion pulses for materials and warm dense matter research

NASA Astrophysics Data System (ADS)

Seidl, Peter A.; Persaud, Arun; Waldron, William L.; Barnard, John J.; Davidson, Ronald C.; Friedman, Alex; Gilson, Erik P.; Greenway, Wayne G.; Grote, David P.; Kaganovich, Igor D.; Lidia, Steven M.; Stettler, Matthew; Takakuwa, Jeffrey H.; Schenkel, Thomas

2015-11-01

We have commenced experiments with intense short pulses of ion beams on the Neutralized Drift Compression Experiment-II at Lawrence Berkeley National Laboratory, by generating beam spots size with radius r<1 mm within 2 ns FWHM and approximately 1010 ions/pulse. To enable the short pulse durations and mm-scale focal spot radii, the 1.2 MeV Li+ ion beam is neutralized in a 1.6-meter drift compression section located after the last accelerator magnet. An 8-Tesla short focal length solenoid compresses the beam in the presence of the large volume plasma near the end of this section before the target. The scientific topics to be explored are warm dense matter, the dynamics of radiation damage in materials, and intense beam and beam-plasma physics including selected topics of relevance to the development of heavy-ion drivers for inertial fusion energy. Here we describe the accelerator commissioning and time-resolved ionoluminescence measurements of yttrium aluminum perovskite using the fully integrated accelerator and neutralized drift compression components.

Spatio-temporally resolved spectral measurements of laser-produced plasma and semiautomated spectral measurement-control and analysis software

NASA Astrophysics Data System (ADS)

Cao, S. Q.; Su, M. G.; Min, Q.; Sun, D. X.; O'Sullivan, G.; Dong, C. Z.

2018-02-01

A spatio-temporally resolved spectral measurement system of highly charged ions from laser-produced plasmas is presented. Corresponding semiautomated computer software for measurement control and spectral analysis has been written to achieve the best synchronicity possible among the instruments. This avoids the tedious comparative processes between experimental and theoretical results. To demonstrate the capabilities of this system, a series of spatio-temporally resolved experiments of laser-produced Al plasmas have been performed and applied to benchmark the software. The system is a useful tool for studying the spectral structures of highly charged ions and for evaluating the spatio-temporal evolution of laser-produced plasmas.

Reprint Of: Enhanced spatially-resolved trace analysis using combined SIMS-single-stage AMS

NASA Astrophysics Data System (ADS)

Grabowski, K. S.; Groopman, E. E.; Fahey, A. J.

2018-01-01

Secondary ion mass spectrometry (SIMS) provides spatially resolved trace analysis of solid materials, but can be complicated by unresolved abundant molecular isobars. By adding a 300-kV single-stage accelerator mass spectrometer (SSAMS) as a detector for a Cameca ims 4f SIMS, one can measure more abundant positive ions from the SIMS while removing molecular isobars, thus improving very low abundance trace element and isotope analysis. This paper describes important features and capabilities of such an integrated system at the Naval Research Laboratory using charge state +1 ions. Transmission loss is compared to molecule destruction as gas flow to the molecule-destruction cell increases. As most measurements tolerate more modest abundance sensitivities than for 14C analysis, a lower gas flow is acceptable, so good transmission of 20-50% for ions of interest can be maintained for a broad range of ion masses. This new instrument has measured isotope ratios for uranium, lead, rare earths, and other elements from particulates and localized regions, with molecule destruction enabling the measurement at low SIMS mass resolving power and thus high transmission, as examples will show. This new and world-unique instrument provides improved capabilities for applications in nuclear and other forensics, geochemistry, cosmochemistry, and the development of optical, electronic, multifunctional, and structural materials.

Enhanced spatially-resolved trace analysis using combined SIMS-single-stage AMS

NASA Astrophysics Data System (ADS)

Grabowski, K. S.; Groopman, E. E.; Fahey, A. J.

2017-11-01

Secondary ion mass spectrometry (SIMS) provides spatially resolved trace analysis of solid materials, but can be complicated by unresolved abundant molecular isobars. By adding a 300-kV single-stage accelerator mass spectrometer (SSAMS) as a detector for a Cameca ims 4f SIMS, one can measure more abundant positive ions from the SIMS while removing molecular isobars, thus improving very low abundance trace element and isotope analysis. This paper describes important features and capabilities of such an integrated system at the Naval Research Laboratory using charge state +1 ions. Transmission loss is compared to molecule destruction as gas flow to the molecule-destruction cell increases. As most measurements tolerate more modest abundance sensitivities than for 14C analysis, a lower gas flow is acceptable, so good transmission of 20-50% for ions of interest can be maintained for a broad range of ion masses. This new instrument has measured isotope ratios for uranium, lead, rare earths, and other elements from particulates and localized regions, with molecule destruction enabling the measurement at low SIMS mass resolving power and thus high transmission, as examples will show. This new and world-unique instrument provides improved capabilities for applications in nuclear and other forensics, geochemistry, cosmochemistry, and the development of optical, electronic, multifunctional, and structural materials.

Alignment and Imaging of the CS2 Dimer Inside Helium Nanodroplets

NASA Astrophysics Data System (ADS)

Pickering, James D.; Shepperson, Benjamin; Hübschmann, Bjarke A. K.; Thorning, Frederik; Stapelfeldt, Henrik

2018-03-01

The carbon disulphide (CS2) dimer is formed inside He nanodroplets and identified using fs laser-induced Coulomb explosion, by observing the CS2+ ion recoil velocity. It is then shown that a 160 ps moderately intense laser pulse can align the dimer in advantageous spatial orientations which allow us to determine the cross-shaped structure of the dimer by analysis of the correlations between the emission angles of the nascent CS2+ and S+ ions, following the explosion process. Our method will enable fs time-resolved structural imaging of weakly bound molecular complexes during conformational isomerization, including formation of exciplexes.

Ion Composition in Titan's Exosphere from the Cassini Plasma Spectrometer

NASA Astrophysics Data System (ADS)

Woodson, A.; Smith, H. T.; Johnson, R. E.

2013-12-01

A primary goal of the Cassini mission has been to characterize the complex interaction between Saturn's magnetosphere and Titan's ionosphere. To this end, the Cassini spacecraft carries two instruments-the Ion and Neutral Mass Spectrometer (INMS) and the Cassini Plasma Spectrometer (CAPS)-capable of energy- and mass-analysis. The Ion Mass Spectrometer (IMS), one of three instruments composing CAPS, is designed to characterize diffuse plasmas throughout the magnetosphere while the INMS is optimized for measurements within Titan's upper atmosphere. As such, mass-resolved ion compositions confirming a variety of hydrocarbons and nitriles have been extracted from INMS data for numerous Titan encounters. Similar analysis of IMS data, however, has largely been resolution-limited to the identification of 'light' and 'heavy' ion groups in the wake. Herein we present a technique for extracting Dalton-resolved ion compositions from IMS spectra acquired below ~5 Titan radii. The method is then applied to data from the T40 encounter and the resulting relative abundances compared with those derived from the INMS data for the same encounter.

Impact of metal ions in porphyrin-based applied materials for visible-light photocatalysis: key information from ultrafast electronic spectroscopy.

PubMed

Kar, Prasenjit; Sardar, Samim; Alarousu, Erkki; Sun, Jingya; Seddigi, Zaki S; Ahmed, Saleh A; Danish, Ekram Y; Mohammed, Omar F; Pal, Samir Kumar

2014-08-11

Protoporphyrin IX-zinc oxide (PP-ZnO) nanohybrids have been synthesized for applications in photocatalytic devices. High-resolution transmission electron microscopy (HRTEM), X-ray diffraction (XRD), and steady-state infrared, absorption, and emission spectroscopies have been used to analyze the structural details and optical properties of these nanohybrids. Time-resolved fluorescence and transient absorption techniques have been applied to study the ultrafast dynamic events that are key to photocatalytic activities. The photocatalytic efficiency under visible-light irradiation in the presence of naturally abundant iron(III) and copper(II) ions has been found to be significantly retarded in the former case, but enhanced in the latter case. More importantly, femtosecond (fs) transient absorption data have clearly demonstrated that the residence of photoexcited electrons from the sensitizer PP in the centrally located iron moiety hinders ground-state bleach recovery of the sensitizer, affecting the overall photocatalytic rate of the nanohybrid. The presence of copper(II) ions, on the other hand, offers additional stability against photobleaching and eventually enhances the efficiency of photocatalysis. In addition, we have also explored the role of UV light in the efficiency of photocatalysis and have rationalized our observations from femtosecond- to picosecond-resolved studies. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

A tandem time–of–flight spectrometer for negative–ion/positive–ion coincidence measurements with soft x-ray excitation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stråhlman, Christian, E-mail: Christian.Strahlman@maxlab.lu.se; Sankari, Rami; Nyholm, Ralf

2016-01-15

We present a newly constructed spectrometer for negative–ion/positive–ion coincidence spectroscopy of gaseous samples. The instrument consists of two time–of–flight ion spectrometers and a magnetic momentum filter for deflection of electrons. The instrument can measure double and triple coincidences between mass–resolved negative and positive ions with high detection efficiency. First results include identification of several negative–ion/positive–ion coincidence channels following inner-shell photoexcitation of sulfur hexafluoride (SF{sub 6})

Chemical imaging of molecular changes in a hydrated single cell by dynamic secondary ion mass spectrometry and super-resolution microscopy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hua, Xin; Szymanski, Craig; Wang, Zhaoying

2016-01-01

Chemical imaging of single cells is important in capturing biological dynamics. Single cell correlative imaging is realized between structured illumination microscopy (SIM) and time-of-flight secondary ion mass spectrometry (ToF-SIMS) using System for Analysis at the Liquid Vacuum Interface (SALVI), a multimodal microreactor. SIM characterized cells and guided subsequent ToF-SIMS analysis. Dynamic ToF-SIMS provided time- and space-resolved cell molecular mapping. Lipid fragments were identified in the hydrated cell membrane. Principal component analysis was used to elucidate chemical component differences among mouse lung cells that uptake zinc oxide nanoparticles. Our results provided submicron chemical spatial mapping for investigations of cell dynamics atmore » the molecular level.« less

The negative ions of strontium and barium

NASA Astrophysics Data System (ADS)

Garwan, M. A.; Kilius, L. R.; Litherland, A. E.; Nadeau, M.-J.; Zhao, X.-L.

1990-12-01

Recent theoretical calculations have predicted a tendency toward higher electron affinities for heavier alkaline elements. Experimental evidence has been obtained for the existence of strontium and barium negative ions created from pure elements in a caesium sputter ion source. Accelerator mass spectrometric techniques were employed to resolve the above elemental negative ions from the interfering molecular species.

[Clinical experience of carbon ion radiotherapy for malignant tumors].

PubMed

Ishikawa, Hitoshi; Tsuji, Hiroshi; Tsujii, Hirohiko

2006-04-01

The carbon ion (C-ion) beams provide unique advantageous biological and physical properties in radiotherapy (RT) for malignant tumors. C-ion beams have a high relative biological effectiveness (RBE) resulting from the high linear energy transfer (LET). In terms of their physical characteristics, C-ion beams exhibit a spread-out Bragg peak (SOBP) and make for a better dose distribution of the target volume by specified beam modulations. Between June 1994 and August 2005, a total of 2,371 patients with malignant tumors were registered in phase I/II dose-escalation studies and clinical phase II trials using C-ion beams generated at Heavy Ion Medical Accelerator in Chiba (HIMAC). In the initial dose-escalation studies, grade 3 or more late rectal complications had developed in some patients. However, the adverse effects were resolved because of the use of appropriate dose levels and modification of the radiation technique. C-ion beams can carry out hypofractionated radiotherapy with a large fraction dose and reduce the overall treatment times compared with conventional radiotherapy. They can also achieve better local tumor control even for radio-resistant tumors such as malignant melanoma, hepatocellular carcinoma and bone and soft tissue sarcomas with minimal morbidity to the normal surrounding tissues.

Velocity space resolved absolute measurement of fast ion losses induced by a tearing mode in the ASDEX Upgrade tokamak

NASA Astrophysics Data System (ADS)

Galdon-Quiroga, J.; Garcia-Munoz, M.; Sanchis-Sanchez, L.; Mantsinen, M.; Fietz, S.; Igochine, V.; Maraschek, M.; Rodriguez-Ramos, M.; Sieglin, B.; Snicker, A.; Tardini, G.; Vezinet, D.; Weiland, M.; Eriksson, L. G.; The ASDEX Upgrade Team; The EUROfusion MST1 Team

2018-03-01

Absolute flux of fast ion losses induced by tearing modes have been measured by means of fast ion loss detectors (FILD) for the first time in RF heated plasmas in the ASDEX Upgrade tokamak. Up to 30 MW m-2 of fast ion losses are measured by FILD at 5 cm from the separatrix, consistent with infra-red camera measurements, with energies in the range of 250-500 keV and pitch angles corresponding to large trapped orbits. A resonant interaction between the fast ions in the high energy tail of the ICRF distribution and a m/n  =  5/4 tearing mode leads to enhanced fast ion losses. Around 9.3 +/- 0.7 % of the fast ion losses are found to be coherent with the mode and scale linearly with its amplitude, indicating the convective nature of the transport mechanism. Simulations have been carried out to estimate the contribution of the prompt losses. A good agreement is found between the simulated and the measured velocity space of the losses. The velocity space resonances that may be responsible for the enhanced fast ion losses are identified.

Stimulated Motion Suppression (STMS): a New Approach to Break the Resolution Barrier for Ion Trap Mass Spectrometry

NASA Astrophysics Data System (ADS)

Zhou, Xiaoyu; Liu, Xinwei; Chiang, Spencer; Cao, Wenbo; Li, Ming; Ouyang, Zheng

2018-05-01

Ion trap is an excellent platform to perform tandem mass spectrometry (MS/MS), but has an intrinsic drawback in resolving power. Using ion resonant ejection as an example, the resolution degradation can be largely attributed to the broadening of the resonant frequency band (RFB) between ion motion and driving alternative-current (AC). To solve this problem, stimulated motion suppression (STMS) was developed. The key idea of STMS is the use of two suppression alternative-current (SAC) signals, which both have reversed initial phases to the main AC. The SACs can block the unexpected sideband ion resonances (or ejections), therefore playing a key role in sharpening the RFB. The proof-of-concept has been demonstrated through ion trajectory simulations and validated experimentally. STMS provides a new and versatile means for the improvement of the ion trap resolution, which for a long time has reached the bottleneck through conventional methods, e.g., increasing the radio-frequency (RF) voltage and decreasing the mass scan rate. At the end, it is worth noting that the idea of STMS is very general and principally can be applied in any RF device for the purposes of high-resolution mass analysis and ion isolation.

Time-resolved magnetic spectrometer measurements of the SABRE positive polarity magnetically insulated transmission line voltage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Menge, P.R.; Cuneo, M.E.; Hanson, D.L.

A magnetic spectrometer has been fielded on the coaxial magnetically insulated transmission line (MITL) of the SABRE ten-cavity inductive voltage adder operated in positive polarity (6 MV, 300 kA, 50 ns). Located 1 m upstream from an extraction ion diode, this diagnostic is capable of measuring the SABRE voltage pulse with a 2 ns resolution. Ions (protons and carbon) from either a flashover or plasma gun source are accelerated from the inner anode across the gap to the outer cathode and into a drift tube terminated by the magnetic spectrometer. The magnetically deflected ions are recorded on up to sixteenmore » PIN diodes (diameter = 1 mm, thickness = 35 {mu}). The voltage waveform is produced from the time-of-flight information. Results confirm previous observations of a vacuum wave precursor separated from the magnetically insulated wave. Verification of upstream precursor erosion techniques are possible with this instrument. Measurements of peak voltage show good agreement with other time-integrated voltage diagnostics. Comparisons with theoretical voltage predictions derived from a flow impedance model of MITL behavior will be presented.« less

Resolving the Kinetic Reconnection Length Scale in Global Magnetospheric Simulations with MHD-EPIC

NASA Astrophysics Data System (ADS)

Toth, G.; Chen, Y.; Cassak, P.; Jordanova, V.; Peng, B.; Markidis, S.; Gombosi, T. I.

2016-12-01

We have recently developed a new modeling capability: the Magnetohydrodynamics with Embedded Particle-in-Cell (MHD-EPIC) algorithm with support from Los Alamos SHIELDS and NSF INSPIRE grants. We have implemented MHD-EPIC into the Space Weather Modeling Framework (SWMF) using the implicit Particle-in-Cell (iPIC3D) and the BATS-R-US extended magnetohydrodynamic codes. The MHD-EPIC model allows two-way coupled simulations in two and three dimensions with multiple embedded PIC regions. Both BATS-R-US and iPIC3D are massively parallel codes. The MHD-EPIC approach allows global magnetosphere simulations with embedded kinetic simulations. For small magnetospheres, like Ganymede or Mercury, we can easily resolve the ion scales around the reconnection sites. Modeling the Earth magnetosphere is very challenging even with our efficient MHD-EPIC model due to the large separation between the global and ion scales. On the other hand the large separation of scales may be exploited: the solution may not be sensitive to the ion inertial length as long as it is small relative to the global scales. The ion inertial length can be varied by changing the ion mass while keeping the MHD mass density, the velocity, and pressure the same for the initial and boundary conditions. Our two-dimensional MHD-EPIC simulations for the dayside reconnection region show in fact, that the overall solution is not sensitive to ion inertial length. The shape, size and frequency of flux transfer events are very similar for a wide range of ion masses. Our results mean that 3D MHD-EPIC simulations for the Earth and other large magnetospheres can be made computationally affordable by artificially increasing the ion mass: the required grid resolution and time step in the PIC model are proportional to the ion inertial length. Changing the ion mass by a factor of 4, for example, speeds up the PIC code by a factor of 256. In fact, this approach allowed us to perform an hour-long 3D MHD-EPIC simulations for the Earth magnetosphere.

Ion Mobility Separation of Variant Histone Tails Extending to the “Middle-down” Range

PubMed Central

Shvartsburg, Alexandre A.; Zheng, Yupeng; Smith, Richard D.; Kelleher, Neil L.

2012-01-01

Differential ion mobility spectrometry (FAIMS) can baseline-resolve multiple variants of post-translationally modified peptides extending to the 3 - 4 kDa range, which differ in the localization of a PTM as small as acetylation. Essentially orthogonal separations for different charge states expand the total peak capacity in proportion to the number of observed states that increases for longer polypeptides. This might enable resolving localization variants for yet larger peptides and even intact proteins. PMID:22559289

First measurements of the temporal evolution of the plasma density in HiPIMS discharges using THz time domain spectroscopy

NASA Astrophysics Data System (ADS)

Meier, Steffen M.; Hecimovic, Ante; Tsankov, Tsanko V.; Luggenhölscher, Dirk; Czarnetzki, Uwe

2018-03-01

In this paper, the novel technique of THz time domain spectroscopy has been applied to obtain time-resolved measurements of the plasma density in the active zone of a HiPIMS discharge with a titanium target. The obtained peak values are in the range of 1012-1013 cm-3 for discharge current densities of 1-4 A cm-2 at 0.5 and 2 Pa argon pressure. The measured densities show good correlation with the discharge current and voltage and the intensity of various atomic and ionic lines. The well known phases of the discharge have been identified and related to the variation of the electron density. The measurement results show that the plasma density remains nearly constant during the runaway/self-sputtering phase. Based on that, it is conjectured that singly charged titanium ions are the dominant ion species during this phase.

Silver chlorobromide nanocubes with significantly improved uniformity: synthesis and assembly into photonic crystals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Li, Zheng; Okasinski, John S.; Gosztola, David J.

2015-01-01

Silver chlorobromide (AgClxBr1-x, 0 < x < 1) nanocubes with a highly uniform size, morphology, and crystallinity have been successfully synthesized through a co-precipitation of Ag+ ions with both Cl- and Br- ions in ethylene glycol containing polyvinyl pyrrolidone at mild temperatures. Compositions of the synthesized nanocubes can be easily tuned by controlling the molar ratio of Cl- to Br- ions in the reaction solutions. The size of the nanocubes is determined by varying a number of parameters including the molar ratio of Cl- to Br- ions, injection rate of Ag+ ions, and reaction temperature. The real-time formation of colloidalmore » AgClxBr1-x nanocubes has been monitored, for the first time, by in situ highenergy synchrotron X-ray diffraction. The time-resolved results reveal that a fast injection rate of Ag+ ions is critical for the formation of AgClxBr1-x nanocubes with a highly pure face-centered cubic crystalline phase. The improved uniformity of the AgClxBr1-x nanocubes is beneficial for assembling them into order superlattices (e.g., photonic crystals) even by simply applying centrifugation forces. The stop band of the resulting photonic crystals can be easily tuned from the ultraviolet to the infrared region by using AgClxBr1-x nanocubes with different sizes. The variation of the dielectric constant of AgClxBr1-x associated with the change of the relative concentration of halide ions provides an additional knob to tune the optical properties of photonic crystals.« less

All-optical atom trap as a target for MOTRIMS-like collision experiments

NASA Astrophysics Data System (ADS)

Sharma, S.; Acharya, B. P.; De Silva, A. H. N. C.; Parris, N. W.; Ramsey, B. J.; Romans, K. L.; Dorn, A.; de Jesus, V. L. B.; Fischer, D.

2018-04-01

Momentum-resolved scattering experiments with laser-cooled atomic targets have been performed since almost two decades with magneto-optical trap recoil ion momentum spectroscopy (MOTRIMS) setups. Compared to experiments with gas-jet targets, MOTRIMS features significantly lower target temperatures allowing for an excellent recoil ion momentum resolution. However, the coincident and momentum-resolved detection of electrons was long rendered impossible due to incompatible magnetic field requirements. Here we report on an experimental approach which is based on an all-optical 6Li atom trap that—in contrast to magneto-optical traps—does not require magnetic field gradients in the trapping region. Atom temperatures of about 2 mK and number densities up to 109 cm-3 make this trap ideally suited for momentum-resolved electron-ion coincidence experiments. The overall configuration of the trap is very similar to conventional magneto-optical traps. It mainly requires small modifications of laser beam geometries and polarization which makes it easily implementable in other existing MOTRIMS experiments.

A Photoluminescence Study of the Changes Induced in the Zinc White Pigment by Formation of Zinc Complexes

PubMed Central

Artesani, Alessia; Gherardi, Francesca; Nevin, Austin; Valentini, Gianluca; Comelli, Daniela

2017-01-01

It is known that oil paintings containing zinc white are subject to rapid degradation. This is caused by the interaction between the active groups of binder and the metal ions of the pigment, which gives rise to the formation of new zinc complexes (metal soaps). Ongoing studies on zinc white paints have been limited to the chemical mechanisms that lead to the formation of zinc complexes. On the contrary, little is known of the photo-physical changes induced in the zinc oxide crystal structure following this interaction. Time-resolved photoluminescence spectroscopy has been applied to follow modifications in the luminescent zinc white pigment when mixed with binder. Significant changes in trap state photoluminescence emissions have been detected: the enhancement of a blue emission combined with a change of the decay kinetic of the well-known green emission. Complementary data from molecular analysis of paints using Fourier transform infrared spectroscopy confirms the formation of zinc carboxylates and corroborates the mechanism for zinc complexes formation. We support the hypothesis that zinc ions migrate into binder creating novel vacancies, affecting the photoluminescence intensity and lifetime properties of zinc oxide. Here, we further demonstrate the advantages of a time-resolved photoluminescence approach for studying defects in semiconductor pigments. PMID:28772700

An integrated approach using high time-resolved tools to study the origin of aerosols.

PubMed

Di Gilio, A; de Gennaro, G; Dambruoso, P; Ventrella, G

2015-10-15

Long-range transport of natural and/or anthropogenic particles can contribute significantly to PM10 and PM2.5 concentrations and some European cities often fail to comply with PM daily limit values due to the additional impact of particles from remote sources. For this reason, reliable methodologies to identify long-range transport (LRT) events would be useful to better understand air pollution phenomena and support proper decision-making. This study explores the potential of an integrated and high time-resolved monitoring approach for the identification and characterization of local, regional and long-range transport events of high PM. In particular, the goal of this work was also the identification of time-limited event. For this purpose, a high time-resolved monitoring campaign was carried out at an urban background site in Bari (southern Italy) for about 20 days (1st-20th October 2011). The integration of collected data as the hourly measurements of inorganic ions in PM2.5 and their gas precursors and of the natural radioactivity, in addition to the analyses of aerosol maps and hourly back trajectories (BT), provided useful information for the identification and chemical characterization of local sources and trans-boundary intrusions. Non-sea salt (nss) sulfate levels were found to increase when air masses came from northeastern Europe and higher dispersive conditions of the atmosphere were detected. Instead, higher nitrate and lower nss-sulfate concentrations were registered in correspondence with air mass stagnation and attributed to local traffic source. In some cases, combinations of local and trans-boundary sources were observed. Finally, statistical investigations such as the principal component analysis (PCA) applied on hourly ion concentrations and the cluster analyses, the Potential Source Contribution Function (PSCF) and the Concentration Weighted Trajectory (CWT) models computed on hourly back-trajectories enabled to complete a cognitive framework and confirm the influence of aerosol transported from heavily polluted areas on the receptor site. Copyright © 2015 Elsevier B.V. All rights reserved.

Influence of argon and oxygen on charge-state-resolved ion energy distributions of filtered aluminum arcs

NASA Astrophysics Data System (ADS)

Rosén, Johanna; Anders, André; Mráz, Stanislav; Atiser, Adil; Schneider, Jochen M.

2006-06-01

The charge-state-resolved ion energy distributions (IEDs) in filtered aluminum vacuum arc plasmas were measured and analyzed at different oxygen and argon pressures in the range of 0.5-8.0 mTorr. A significant reduction of the ion energy was detected as the pressure was increased, most pronounced in an argon environment and for the higher charge states. The corresponding average charge state decreased from 1.87 to 1.0 with increasing pressure. The IEDs of all metal ions in oxygen were fitted with shifted Maxwellian distributions. The results show that it is possible to obtain a plasma composition with a narrow charge-state distribution as well as a narrow IED. These data may enable tailoring thin film properties through selecting growth conditions that are characterized by predefined charge state and energy distributions.

Intact mass detection, interpretation, and visualization to automate Top-Down proteomics on a large scale

PubMed Central

Durbin, Kenneth R.; Tran, John C.; Zamdborg, Leonid; Sweet, Steve M. M.; Catherman, Adam D.; Lee, Ji Eun; Li, Mingxi; Kellie, John F.; Kelleher, Neil L.

2011-01-01

Applying high-throughput Top-Down MS to an entire proteome requires a yet-to-be-established model for data processing. Since Top-Down is becoming possible on a large scale, we report our latest software pipeline dedicated to capturing the full value of intact protein data in automated fashion. For intact mass detection, we combine algorithms for processing MS1 data from both isotopically resolved (FT) and charge-state resolved (ion trap) LC-MS data, which are then linked to their fragment ions for database searching using ProSight. Automated determination of human keratin and tubulin isoforms is one result. Optimized for the intricacies of whole proteins, new software modules visualize proteome-scale data based on the LC retention time and intensity of intact masses and enable selective detection of PTMs to automatically screen for acetylation, phosphorylation, and methylation. Software functionality was demonstrated using comparative LC-MS data from yeast strains in addition to human cells undergoing chemical stress. We further these advances as a key aspect of realizing Top-Down MS on a proteomic scale. PMID:20848673

Studies of Ion Beam Charge Neutralization by Ferroelectric Plasma Sources

NASA Astrophysics Data System (ADS)

Stepanov, A.; Gilson, E. P.; Grisham, L.; Davidson, R. C.

2013-10-01

Space-charge forces limit the possible transverse compression of high perveance ion beams that are used in ion-beam-driven high energy density physics applications; the minimum radius to which a beam can be focused is an increasing function of perveance. The limit can be overcome if a plasma is introduced in the beam path between the focusing element and the target in order to neutralize the space charge of the beam. This concept has been implemented on the Neutralized Drift Compression eXperiment (NDCX) at LBNL using Ferroelectric Plasma Sources (FEPS). In our experiment at PPPL, we propagate a perveance-dominated ion beam through a FEPS to study the effect of the neutralizing plasma on the beam envelope and its evolution in time. A 30-60 keV space-charge-dominated Argon beam is focused with an Einzel lens into a FEPS located at the beam waist. The beam is intercepted downstream from the FEPS by a movable Faraday cup that provides time-resolved 2D current density profiles of the beam spot on target. We report results on: (a) dependence of charge neutralization on FEPS plasma density; (b) effects on beam emittance, and (c) time evolution of the beam envelope after the FEPS pulse. Research supported by the U.S. Department of Energy.

Effect of fatigue/ageing on the lithium distribution in cylinder-type Li-ion batteries

NASA Astrophysics Data System (ADS)

Mühlbauer, M. J.; Dolotko, O.; Hofmann, M.; Ehrenberg, H.; Senyshyn, A.

2017-04-01

The lithium concentration in the graphite anode of fatigued (cycled 1000 times at 25 °C) Li-ion cell of 18650-type has been probed non-destructively by spatially resolved neutron diffraction. The amount x of Li in LixC6 has been determined in a central plane of a cylinder-type Li-ion cell. A radial mesh with a gauge volume of 2 × 2 × 20 mm3 was used. Besides the evidently lower lithiation grade, caused by a lack of free movable lithium and a loss of electrolyte, a development of fatigue-driven spatial lithium inhomogeneities has been observed in radial direction. Observed changes have been discussed in light of their correlations to an increase of the internal cell resistance and to a change of the electrolyte concentration.

Alternative modeling methods for plasma-based Rf ion sources

DOE Office of Scientific and Technical Information (OSTI.GOV)

Veitzer, Seth A., E-mail: veitzer@txcorp.com; Kundrapu, Madhusudhan, E-mail: madhusnk@txcorp.com; Stoltz, Peter H., E-mail: phstoltz@txcorp.com

Rf-driven ion sources for accelerators and many industrial applications benefit from detailed numerical modeling and simulation of plasma characteristics. For instance, modeling of the Spallation Neutron Source (SNS) internal antenna H{sup −} source has indicated that a large plasma velocity is induced near bends in the antenna where structural failures are often observed. This could lead to improved designs and ion source performance based on simulation and modeling. However, there are significant separations of time and spatial scales inherent to Rf-driven plasma ion sources, which makes it difficult to model ion sources with explicit, kinetic Particle-In-Cell (PIC) simulation codes. Inmore » particular, if both electron and ion motions are to be explicitly modeled, then the simulation time step must be very small, and total simulation times must be large enough to capture the evolution of the plasma ions, as well as extending over many Rf periods. Additional physics processes such as plasma chemistry and surface effects such as secondary electron emission increase the computational requirements in such a way that even fully parallel explicit PIC models cannot be used. One alternative method is to develop fluid-based codes coupled with electromagnetics in order to model ion sources. Time-domain fluid models can simulate plasma evolution, plasma chemistry, and surface physics models with reasonable computational resources by not explicitly resolving electron motions, which thereby leads to an increase in the time step. This is achieved by solving fluid motions coupled with electromagnetics using reduced-physics models, such as single-temperature magnetohydrodynamics (MHD), extended, gas dynamic, and Hall MHD, and two-fluid MHD models. We show recent results on modeling the internal antenna H{sup −} ion source for the SNS at Oak Ridge National Laboratory using the fluid plasma modeling code USim. We compare demonstrate plasma temperature equilibration in two-temperature MHD models for the SNS source and present simulation results demonstrating plasma evolution over many Rf periods for different plasma temperatures. We perform the calculations in parallel, on unstructured meshes, using finite-volume solvers in order to obtain results in reasonable time.« less

Alternative modeling methods for plasma-based Rf ion sources.

PubMed

Veitzer, Seth A; Kundrapu, Madhusudhan; Stoltz, Peter H; Beckwith, Kristian R C

2016-02-01

Rf-driven ion sources for accelerators and many industrial applications benefit from detailed numerical modeling and simulation of plasma characteristics. For instance, modeling of the Spallation Neutron Source (SNS) internal antenna H(-) source has indicated that a large plasma velocity is induced near bends in the antenna where structural failures are often observed. This could lead to improved designs and ion source performance based on simulation and modeling. However, there are significant separations of time and spatial scales inherent to Rf-driven plasma ion sources, which makes it difficult to model ion sources with explicit, kinetic Particle-In-Cell (PIC) simulation codes. In particular, if both electron and ion motions are to be explicitly modeled, then the simulation time step must be very small, and total simulation times must be large enough to capture the evolution of the plasma ions, as well as extending over many Rf periods. Additional physics processes such as plasma chemistry and surface effects such as secondary electron emission increase the computational requirements in such a way that even fully parallel explicit PIC models cannot be used. One alternative method is to develop fluid-based codes coupled with electromagnetics in order to model ion sources. Time-domain fluid models can simulate plasma evolution, plasma chemistry, and surface physics models with reasonable computational resources by not explicitly resolving electron motions, which thereby leads to an increase in the time step. This is achieved by solving fluid motions coupled with electromagnetics using reduced-physics models, such as single-temperature magnetohydrodynamics (MHD), extended, gas dynamic, and Hall MHD, and two-fluid MHD models. We show recent results on modeling the internal antenna H(-) ion source for the SNS at Oak Ridge National Laboratory using the fluid plasma modeling code USim. We compare demonstrate plasma temperature equilibration in two-temperature MHD models for the SNS source and present simulation results demonstrating plasma evolution over many Rf periods for different plasma temperatures. We perform the calculations in parallel, on unstructured meshes, using finite-volume solvers in order to obtain results in reasonable time.

On the design of the NIF Continuum Spectrometer

NASA Astrophysics Data System (ADS)

Thorn, D. B.; MacPhee, A.; Ayers, J.; Galbraith, J.; Hardy, C. M.; Izumi, N.; Bradley, D. K.; Pickworth, L. A.; Bachmann, B.; Kozioziemski, B.; Landen, O.; Clark, D.; Schneider, M. B.; Hill, K. W.; Bitter, M.; Nagel, S.; Bell, P. M.; Person, S.; Khater, H. Y.; Smith, C.; Kilkenny, J.

2017-08-01

In inertial confinement fusion (ICF) experiments on the National Ignition Facility (NIF), measurements of average ion temperature using DT neutron time of flight broadening and of DD neutrons do not show the same apparent temperature. Some of this may be due to time and space dependent temperature profiles in the imploding capsule which are not taken into account in the analysis. As such, we are attempting to measure the electron temperature by recording the free-free electron-ion scattering-spectrum from the tail of the Maxwellian temperature distribution. This will be accomplished with the new NIF Continuum Spectrometer (ConSpec) which spans the x-ray range of 20 keV to 30 keV (where any opacity corrections from the remaining mass of the ablator shell are negligible) and will be sensitive to temperatures between ˜ 3 keV and 6 keV. The optical design of the ConSpec is designed to be adaptable to an x-ray streak camera to record time resolved free-free electron continuum spectra for direct measurement of the dT/dt evolution across the burn width of a DT plasma. The spectrometer is a conically bent Bragg crystal in a focusing geometry that allows for the dispersion plane to be perpendicular to the spectrometer axis. Additionally, to address the spatial temperature dependence, both time integrated and time resolved pinhole and penumbral imaging will be provided along the same polar angle. The optical and mechanical design of the instrument is presented along with estimates for the dispersion, solid angle, photometric sensitivity, and performance.

Time-resolved fluorescence study of exciplex formation in diastereomeric naproxen-pyrrolidine dyads.

PubMed

Khramtsova, Ekaterina A; Plyusnin, Viktor F; Magin, Ilya M; Kruppa, Alexander I; Polyakov, Nikolay E; Leshina, Tatyana V; Nuin, Edurne; Marin, M Luisa; Miranda, Miguel A

2013-12-19

The influence of chirality on the elementary processes triggered by excitation of the (S,S)- and (R,S)- diastereoisomers of naproxen-pyrrolidine (NPX-Pyr) dyads has been studied by time-resolved fluorescence in acetonitrile-benzene mixtures. In these systems, the quenching of the (1)NPX*-Pyr singlet excited state occurs through electron transfer and exciplex formation. Fluorescence lifetimes and quantum yields revealed a significant difference (around 20%) between the (S,S)- and (R,S)- diastereomers. In addition, the quantum yields of exciplexes differed by a factor of 2 regardless of solvent polarity. This allows us to suggest a similar influence of the chiral centers on the local charge transfer resulting in exciplex and full charge separation that leads to ion-biradicals. A simplified scheme is proposed to estimate a set of rate constant values (k1-k5) for the elementary stages in each solvent system.

Amine-functionalized lanthanide-doped zirconia nanoparticles: optical spectroscopy, time-resolved fluorescence resonance energy transfer biodetection, and targeted imaging.

PubMed

Liu, Yongsheng; Zhou, Shanyong; Tu, Datao; Chen, Zhuo; Huang, Mingdong; Zhu, Haomiao; Ma, En; Chen, Xueyuan

2012-09-12

Ultrasmall inorganic oxide nanoparticles doped with trivalent lanthanide ions (Ln(3+)), a new and huge family of luminescent bioprobes, remain nearly untouched. Currently it is a challenge to synthesize biocompatible ultrasmall oxide bioprobes. Herein, we report a new inorganic oxide bioprobe based on sub-5 nm amine-functionalized tetragonal ZrO(2)-Ln(3+) nanoparticles synthesized via a facile solvothermal method and ligand exchange. By utilizing the long-lived luminescence of Ln(3+), we demonstrate its application as a sensitive time-resolved fluorescence resonance energy transfer (FRET) bioprobe to detect avidin with a record-low detection limit of 3.0 nM. The oxide nanoparticles also exhibit specific recognition of cancer cells overexpressed with urokinase plasminogen activator receptor (uPAR, an important marker of tumor biology and metastasis) and thus may have great potentials in targeted bioimaging.

High throughput on-chip analysis of high-energy charged particle tracks using lensfree imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Luo, Wei; Shabbir, Faizan; Gong, Chao

2015-04-13

We demonstrate a high-throughput charged particle analysis platform, which is based on lensfree on-chip microscopy for rapid ion track analysis using allyl diglycol carbonate, i.e., CR-39 plastic polymer as the sensing medium. By adopting a wide-area opto-electronic image sensor together with a source-shifting based pixel super-resolution technique, a large CR-39 sample volume (i.e., 4 cm × 4 cm × 0.1 cm) can be imaged in less than 1 min using a compact lensfree on-chip microscope, which detects partially coherent in-line holograms of the ion tracks recorded within the CR-39 detector. After the image capture, using highly parallelized reconstruction and ion track analysis algorithms running on graphics processingmore » units, we reconstruct and analyze the entire volume of a CR-39 detector within ∼1.5 min. This significant reduction in the entire imaging and ion track analysis time not only increases our throughput but also allows us to perform time-resolved analysis of the etching process to monitor and optimize the growth of ion tracks during etching. This computational lensfree imaging platform can provide a much higher throughput and more cost-effective alternative to traditional lens-based scanning optical microscopes for ion track analysis using CR-39 and other passive high energy particle detectors.« less

Spatially resolved nuclear spin relaxation, electron spin relaxation and light absorption in swift heavy ion irradiated LiF crystals.

PubMed

Stork, H; Dinse, K-P; Ditter, M; Fujara, F; Masierak, W; Neumann, R; Schuster, B; Schwartz, K; Trautmann, C

2010-05-12

Spatially resolved (19)F and (7)Li spin-lattice relaxation rates are measured for LiF single crystals after irradiation with two kinds of swift heavy ions ((12)C of 133 MeV and (208)Pb of 1.78 GeV incident energy). Like in earlier studies on (130)Xe and (238)U irradiated LiF crystals, we found a strong enhancement of the nuclear spin-lattice relaxation rate within the ion penetration depth and a slight--but still significant--enhancement beyond. By evaluating the nuclear relaxation rate enhancement within the ion range after irradiation with different projectiles, a universal relationship between the spin-lattice relaxation rate and the dose is deduced. The results of accompanying X-band electron paramagnetic resonance relaxation measurements and optical absorption spectroscopy are included in a physical interpretation of this relationship. Also the reason for the enhanced relaxation rate beyond the ion range is further discussed.

Fourier Transfrom Ion Cyclotron Resonance Mass Spectrometry at High Magnetic Field

NASA Astrophysics Data System (ADS)

Marshall, Alan G.

1998-03-01

At high magnetic field (9.4 tesla at NHMFL), Fourier transform ion cyclotron resonance mass spectrometry performance improves dramatically: mass resolving power, axialization efficiency, and scan speed (each proportional to B), maximum ion mass, dynamic range, ion trapping period, kinetic energy, and electron self-cooling rate for sympathetic cooling (each proportional to B^2), and ion coalescence tendency (proportional 1/B^2). These advantages may apply singly (e.g., unit mass resolution for proteins of >100,000 Da), or compound (e.g., 10-fold improvement in S/N ratio for 9.4 T vs. 6 T at the same resolving power). Examples range from direct determination of molecular formulas of diesel fuel components by accurate mass measurement (=B10.1 ppm) to protein structure and dynamics probed by H/D exchange. This work was supported by N.S.F. (CHE-93-22824; CHE-94-13008), N.I.H. (GM-31683), Florida State University, and the National High Magnetic Field Laboratory in Tallahassee, FL.

Communication: Electron ionization of DNA bases.

PubMed

Rahman, M A; Krishnakumar, E

2016-04-28

No reliable experimental data exist for the partial and total electron ionization cross sections for DNA bases, which are very crucial for modeling radiation damage in genetic material of living cell. We have measured a complete set of absolute partial electron ionization cross sections up to 500 eV for DNA bases for the first time by using the relative flow technique. These partial cross sections are summed to obtain total ion cross sections for all the four bases and are compared with the existing theoretical calculations and the only set of measured absolute cross sections. Our measurements clearly resolve the existing discrepancy between the theoretical and experimental results, thereby providing for the first time reliable numbers for partial and total ion cross sections for these molecules. The results on fragmentation analysis of adenine supports the theory of its formation in space.

Nonradiative transition dynamics in alexandrite

NASA Technical Reports Server (NTRS)

Gayen, S. K.; Wang, W. B.; Petricevic, V.; Alfano, R. R.

1986-01-01

The first direct picosecond time-resolved measurement of the nonradiative transition dynamics between the excited 4T2 pump band and the metastable 2E storage level of the trivalent chromium ion in alexandrite is reported. The nonradiative relaxation times of 17 ps for intra-4T2 vibrational transitions, and 27 ps for 4T2-2E electronic transition are obtained. The thermal repopulation rate of the 4T2 state from the metastable 2E level is of the order 3.5 x 10 to the 9th per s.

Protein displacements under external forces: An atomistic Langevin dynamics approach.

PubMed

Gnandt, David; Utz, Nadine; Blumen, Alexander; Koslowski, Thorsten

2009-02-28

We present a fully atomistic Langevin dynamics approach as a method to simulate biopolymers under external forces. In the harmonic regime, this approach permits the computation of the long-term dynamics using only the eigenvalues and eigenvectors of the Hessian matrix of second derivatives. We apply this scheme to identify polymorphs of model proteins by their mechanical response fingerprint, and we relate the averaged dynamics of proteins to their biological functionality, with the ion channel gramicidin A, a phosphorylase, and neuropeptide Y as examples. In an environment akin to dilute solutions, even small proteins show relaxation times up to 50 ns. Atomically resolved Langevin dynamics computations have been performed for the stretched gramicidin A ion channel.

Fluorescence of acridinic dyes in anionic surfactant solution

NASA Astrophysics Data System (ADS)

Pereira, Robson Valentim; Gehlen, Marcelo Henrique

2005-10-01

The interaction of the cationic dyes acridine, 9-aminoacridine (9AA), and proflavine, with sodium dodecyl sulfate (SDS) was studied by electronic absorption, steady-state and time-resolved fluorescence spectroscopies. The dyes interact with SDS in the pre-micellar region leading in two cases to dimerization in dye-surfactant aggregates, but with distinct molecular arrangements. For proflavine, the observed red shift of the electronic absorption band indicates the presence of J-aggregate, which are nonfluorescent. In the case of 9AA, the aggregates were characterized as nonspecific (neither J- nor H-type is spectroscopically observed). The time-resolved emission spectra gives evidences of the presence of weakly bound dimers by the recovery of three defined decay times by global analysis: dye monomer ( τ1 = 16.4 ns), dimer ( τ2 = 7.1 ns), and a faster component ( τ3 = 2.1 ns) ascribed to intracluster energy migration between monomer and dimer. Acridine has a weak interaction with SDS forming only an ion pair without further self-aggregation of the dye.

Fluorescence of acridinic dyes in anionic surfactant solution.

PubMed

Pereira, Robson Valentim; Gehlen, Marcelo Henrique

2005-10-01

The interaction of the cationic dyes acridine, 9-aminoacridine (9AA), and proflavine, with sodium dodecyl sulfate (SDS) was studied by electronic absorption, steady-state and time-resolved fluorescence spectroscopies. The dyes interact with SDS in the pre-micellar region leading in two cases to dimerization in dye-surfactant aggregates, but with distinct molecular arrangements. For proflavine, the observed red shift of the electronic absorption band indicates the presence of J-aggregate, which are nonfluorescent. In the case of 9AA, the aggregates were characterized as nonspecific (neither J- nor H-type is spectroscopically observed). The time-resolved emission spectra gives evidences of the presence of weakly bound dimers by the recovery of three defined decay times by global analysis: dye monomer (tau1 = 16.4 ns), dimer (tau2 = 7.1 ns), and a faster component (tau3 = 2.1 ns) ascribed to intracluster energy migration between monomer and dimer. Acridine has a weak interaction with SDS forming only an ion pair without further self-aggregation of the dye.

Time-resolved second-harmonic generation from gold nanoparticle arrays

NASA Astrophysics Data System (ADS)

Ferrara, D. W.; Tetz, K. A.; McMahon, M. D.; Haglund, R. F., Jr.

2007-09-01

We have studied the effects of planar inversion symmetry and particle-coupling of gold nanoparticle (NP) arrays by angle dependent second-harmonic generation (SHG). Time- and angle- resolved measurements were made using a mode-locked Ti:sapphire 800 nm laser onto gold NP arrays with plasmon resonance tuned to match the laser wavelength in order to produce maximum SHG signal. Finite-difference time domain simulations are used to model the near-field distributions for the various geometries and compared to experiment. The arrays were fabricated by focused ion-beam lithography and metal vapor deposition followed by standard lift-off protocols, producing NPs approximately 20nm high with various in-plane dimensions and interparticle gaps. Above a threshold fluence of ~ 7.3 × 10 -5 mJ/cm2 we find that the SHG scales with the third power of intensity, rather than the second, and atomic-force microscopy shows that the NPs have undergone a reshaping process leading to more nearly spherical shapes.

Atmospheric Pressure Ionization Permanent Magnet Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

PubMed Central

Vilkov, Andrey N.; Gamage, Chaminda M.; Misharin, Alexander S.; Doroshenko, Vladimir M.; Tolmachev, Dmitry A.; Tarasova, Irina A.; Kharybin, Oleg N.; Novoselov, Konstantin P.; Gorshkov, Michael V.

2007-01-01

A new Fourier Transform Ion Cyclotron Resonance mass spectrometer based on a permanent magnet with an atmospheric pressure ionization source was designed and constructed. A mass resolving power (full-width-at-half-maximum) of up to 80,000 in the electron ionization mode and 25,000 in the electrospray mode was obtained. Also, a mass measurement accuracy at low-ppm level has been demonstrated for peptide mixtures in a mass range of up to 1,200 m/z in the isotopically resolved mass spectra. PMID:17587594

Sounding of the Ion Energization Region: Resolving Ambiguities

NASA Technical Reports Server (NTRS)

LaBelle, James

2003-01-01

Dartmouth College provided a single-channel high-frequency wave receiver to the Sounding of the Ion Energization Region: Resolving Ambiguities (SIERRA) rocket experiment launched from Poker Flat, Alaska, in January 2002. The receiver used signals from booms, probes, preamplifiers, and differential amplifiers provided by Cornell University coinvestigators. Output was to a dedicated 5 MHz telemetry link provided by WFF, with a small amount of additional Pulse Code Modulation (PCM) telemetry required for the receiver gain information. We also performed preliminary analysis of the data. The work completed is outlined below, in chronological order.

Combining Structural Probes in the Gas Phase - Ion Mobility- Resolved Action-FRET

NASA Astrophysics Data System (ADS)

Daly, Steven; MacAleese, Luke; Dugourd, Philippe; Chirot, Fabien

2018-01-01

In the context of native mass spectrometry, the development of gas-phase structural probes sensitive to the different levels of structuration of biomolecular assemblies is necessary to push forward conformational studies. In this paper, we provide the first example of the combination of ion mobility (IM) and Förster resonance energy transfer (FRET) measurements within the same experimental setup. The possibility to obtain mass- and mobility-resolved FRET measurements is demonstrated on a model peptide and applied to monitor the collision-induced unfolding of ubiquitin. [Figure not available: see fulltext.

Ion beam enhancement in magnetically insulated ion diodes for high-intensity pulsed ion beam generation in non-relativistic mode

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhu, X. P.; Surface Engineering Laboratory, School of Materials Science and Engineering, Dalian University of Technology, Dalian 116024; Zhang, Z. C.

High-intensity pulsed ion beam (HIPIB) with ion current density above Child-Langmuir limit is achieved by extracting ion beam from anode plasma of ion diodes with suppressing electron flow under magnetic field insulation. It was theoretically estimated that with increasing the magnetic field, a maximal value of ion current density may reach nearly 3 times that of Child-Langmuir limit in a non-relativistic mode and close to 6 times in a highly relativistic mode. In this study, the behavior of ion beam enhancement by magnetic insulation is systematically investigated in three types of magnetically insulated ion diodes (MIDs) with passive anode, takingmore » into account the anode plasma generation process on the anode surface. A maximal enhancement factor higher than 6 over the Child-Langmuir limit can be obtained in the non-relativistic mode with accelerating voltage of 200–300 kV. The MIDs differ in two anode plasma formation mechanisms, i.e., surface flashover of a dielectric coating on the anode and explosive emission of electrons from the anode, as well as in two insulation modes of external-magnetic field and self-magnetic field with either non-closed or closed drift of electrons in the anode-cathode (A-K) gap, respectively. Combined with ion current density measurement, energy density characterization is employed to resolve the spatial distribution of energy density before focusing for exploring the ion beam generation process. Consistent results are obtained on three types of MIDs concerning control of neutralizing electron flows for the space charge of ions where the high ion beam enhancement is determined by effective electron neutralization in the A-K gap, while the HIPIB composition of different ion species downstream from the diode may be considerably affected by the ion beam neutralization during propagation.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koh, S.K.; Song, S.K.; Choi, W.K.

A Kaufman-type 5 cm convex gridded ion-beam source is characterized in terms of angle-resolved ion-beam current density and beam uniformity at various discharge currents, electromagnet currents, and acceleration potentials. {copyright} {ital 1995} {ital American} {ital Institute} {ital of} {ital Physics}.

Influence of argon and oxygen on charge-state-resolved ion energydistributions of filtered aluminum arcs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rosen, Johanna; Anders, Andre; Mraz, Stanislav

2006-03-23

The charge-state-resolved ion energy distributions (IEDs) in filtered aluminum vacuum arc plasmas were measured and analyzed at different oxygen and argon pressures in the range 0.5 8.0 mTorr. A significant reduction of the ion energy was detected as the pressure was increased, most pronounced in an argon environment and for the higher charge states. The corresponding average charge state decreased from 1.87 to 1.0 with increasing pressure. The IEDs of all metal ions in oxygen were fitted with shifted Maxwellian distributions. The results show that it is possible to obtain a plasma composition with a narrow charge-state distribution as wellmore » as a narrow IED. These data may enable tailoring thin-film properties through selecting growth conditions that are characterized by predefined charge state and energy distributions.« less

Binary collision model for neon Auger spectra from neon ion bombardment of the aluminum surface

NASA Technical Reports Server (NTRS)

Pepper, S. V.

1986-01-01

A model is developed to account for the angle-resolved Auger spectra from neon ion bombardment of the aluminum surface recently obtained by Pepper and Aron. The neon is assumed to be excited in a single asymmetric neon-aluminum-collision and scattered back into the vacuum where it emits an Auger electron. The velocity of the Auger electron acquires a Doppler shift by virtue of the emission from a moving source. The dependence of the Auger peak shape and energy on the incident ion energy, angle of incidence and on the angle of Auger electron emission with respect to the surface is presented. Satisfactory agreement with the angle resolved experimental observations is obtained. The dependence of the angle-integrated Auger yield on the incident ion energy and angle of incidence is also obtained and shown to be in satisfactory agreement with available experimental evidence.

The hidden ion population - Revisited. [in outer plasmasphere

NASA Technical Reports Server (NTRS)

Olsen, R. C.; Chappell, C. R.; Gallagher, D. L.; Green, J. L.; Gurnett, D. A.

1985-01-01

In an investigation conducted by Olsen (1982) on the basis of particle data taken with an electrostatic analyzer, it was found that a cold plasma population with a density between 10 and 100 per cu cm appeared suddenly when the satellite was eclipsed, but was hidden in sunlight. The present paper has the objective to show further measurements of ordinarily 'hidden' ion populations, in order to resolve some of the questions raised in connection with the Scatha satellite data reported by Olsen. It is found that the retarding ion mass spectrometer (RIMS) detector is capable of measuring the core of the plasma distribution in sunlight and eclipse, though the task is more easily done in eclipse. There are, however, limitations concerning the ability of the detector to measure all the plasma, all the time. It is, therefore, pointed out that continuous effective measurements of the 'hidden' ion population of the magnetosphere still awaits satellites with effective means of potential control.

Spectroscopic Measurements of Collision-less Coupling Between Laser-Produced, Super-Alfvénic Debris Plasmas and Magnetized, Ambient Plasmas

NASA Astrophysics Data System (ADS)

Bondarenko, Anton; Everson, E.; Schaeffer, D.; Constantin, C.; Vincena, S.; Van Compernolle, B.; Clark, S.; Niemann, C.

2013-06-01

Emission spectroscopy is currently being utilized in order to assess collision-less momentum and energy coupling between super-Alfvénic debris plasmas and magnetized, ambient plasmas of astrophysical relevance. In a recent campaign on the Large Plasma Device (LAPD) utilizing the Phoenix laboratory Raptor laser (130 J, 25 ns FWHM), laser-ablated carbon debris plasmas were generated within magnetized, ambient helium plasmas (nelec ≈ 3×1012 cm-3, Telec ≈ 5.5 eV, B0 = 200 G), and prominent spectral lines of carbon and helium ions were studied in high resolution (˜ 0.01 nm). Time-resolved Doppler shift and width measurements of a C V ion spectral line reveal significant deceleration as the ions stream through the background plasma, which may indirectly indicate momentum coupling. Spectral lines of He II ions are observed to intensify by orders of magnitude and broaden, indicating energy transfer from the debris plasma to the background plasma.

Investigation of Ion Acoustic Wave Instabilities Near Positive Electrodes

NASA Astrophysics Data System (ADS)

Hood, Ryan; Chu, Feng; Baalrud, Scott; Merlino, Robert; Skiff, Fred

2017-10-01

Electron sheaths occur when an electrode is biased above the plasma potential, most often during the electron saturation portion of a Langmuir probe trace. Through the presheath, electrons are accelerated to velocities exceeding the electron thermal speed at the sheath edge, while ions do not develop any appreciable flow. PIC simulations have shown that ion acoustic instabilities are excited by the differential flow between ions and electrons in the presheath region of a low temperature plasma. We present the first experimental measurements investigating these instabilities using Laser-Induced Fluorescence diagnostics in a multidipole argon plasma. The plasma dispersion relation is measured from the power spectra of the imaged LIF signal and compared to the simulation results. In addition, optical pumping is measured using time-resolved LIF measurements and fit to a model in order to determine the diffusion rate, which may be enhanced due to the instability. This research was supported by the Office of Fusion Energy Sciences at the U.S. Department of Energy under contract DE-AC04-94SL85000.

First beam test of a liquid Cherenkov detector prototype for a future TOF measurements at the Super-FRS

NASA Astrophysics Data System (ADS)

Kuzminchuk-Feuerstein, Natalia; Ferber, Nadine; Rozhkova, Elena; Kaufeld, Ingo; Voss, Bernd

2017-09-01

In order to separate and identify fragmentation products with the Super-Fragment Separator (SuperFRS) at FAIR a high resolving power detector system is required for position and Time-Of-Flight (TOF) measurements. The TOF detector is used to measure the velocity of the particles and hence, in conjunction with their momentum or energy, to determine their mass and hence their identity. Aiming to develop a system with a precision down to about 50 ps in time and resistant to a high radiation rate of relativistic heavy ions of up to 107 per spill (at the second focal plane), we have shown a conceptual design for a Cherenkov detector envisioned for the future TOF measurements employing Iodine Naphthalene (C10H7I) as a fluid radiator. The application of a liquid radiator allows the circulation of the active material and therefore to greatly reduce the effects of the degradation of the optical performance expected after exposure to the high ion rates at the Super-FRS. The prototype of a TOF-Cherenkov detector was designed, constructed and its key-properties have been investigated in measurements with heavy ions at CaveC at GSI. These measurements were performed with nickel ions at 300-1500 MeV/u and ion-beam intensities of up to 4 × 106 ions/spill of 8 s. As a first result a maximum detection efficiency of 70% and a timing resolution of 267 ps (σ) was achieved. We report the first attempt of time measurements with a Cherenkov detector based on a liquid radiator. Further optimization is required.

Short intense ion pulses for materials and warm dense matter research

DOE PAGES

Seidl, Peter A.; Persaud, Arun; Waldron, William L.; ...

2015-08-14

We have commenced experiments with intense short pulses of ion beams on the Neutralized Drift Compression Experiment-II at Lawrence Berkeley National Laboratory, by generating beam spots size with radius r<1 mm within 2 ns FWHM and approximately 10 10 ions/pulse. To enable the short pulse durations and mm-scale focal spot radii, the 1.2 MeV Li + ion beam is neutralized in a 1.6-meter drift compression section located after the last accelerator magnet. An 8-Tesla short focal length solenoid compresses the beam in the presence of the large volume plasma near the end of this section before the target. The scientificmore » topics to be explored are warm dense matter, the dynamics of radiation damage in materials, and intense beam and beam-plasma physics including selected topics of relevance to the development of heavy-ion drivers for inertial fusion energy. Finally, we describe the accelerator commissioning and time-resolved ionoluminescence measurements of yttrium aluminum perovskite using the fully integrated accelerator and neutralized drift compression components.« less

Back-streaming ion emission and beam focusing on high power linear induction accelerator

NASA Astrophysics Data System (ADS)

Zhu, Jun; Chen, Nan; Yu, Haijun; Jiang, Xiaoguo; Wang, Yuan; Dai, Wenhua; Gao, Feng; Wang, Minhong; Li, Jin; Shi, Jinshui

2011-08-01

Ions released from target surfaces by impact of a high intensity and current electron beam can be accelerated and trapped in the beam potential, and further destroy the beam focus. By solving the 2D Poisson equation, we found that the charge neutralization factor of the ions to the beam under space charge limited condition is 1/3, which is large enough to disrupt the spot size. Therefore, the ion emission at the target in a single-pulse beam/target system must be source limited. Experimental results on the time-resolved beam profile measurement have also proven that. A new focus scheme is proposed in this paper to focus the beam to a small spot size with the existence of back-streaming ions. We found that the focal spot will move upstream as the charge neutralization factor increases. By comparing the theoretical and experimental focal length of the Dragon-I accelerator (20 MeV, 2.5 kA, 60 ns flattop), we found that the average neutralization factor is about 5% in the beam/target system.

Ultrafast entanglement of trapped ions

NASA Astrophysics Data System (ADS)

Neyenhuis, Brian; Mizrahi, Jonathan; Johnson, Kale; Monroe, Christopher

2013-05-01

We have demonstrated ultrafast spin-motion entanglement of a single atomic ion using a short train of intense laser pulses. This pulse train gives the ion a spin-dependent kick where each spin state receives a discrete momentum kick in opposite directions. Using a series of these spin-dependent kicks we can realize a two qubit gate. In contrast to gates using spectroscopically resolved motional sidebands, these gates may be performed faster than the trap oscillation period, making them potentially less sensitive to noise, independent of temperature, and more easily scalable to large crystals of ions. We show that multiple kicks can be strung together to create a ``Schrodinger cat'' like state, where the large separation between the two parts of the wavepacket allow us to accumulate the phase shift necessary for a gate in a shorter amount of time. We will present a realistic pulse scheme for a two ion gate, and our progress towards its realization. This work is supported by grants from the U.S. Army Research Office with funding from the DARPA OLE program, IARPA, and the MURI program; and the NSF Physics Frontier Center at JQI.

pH and chloride recordings in living cells using two-photon fluorescence lifetime imaging microscopy

NASA Astrophysics Data System (ADS)

Lahn, Mattes; Hille, Carsten; Koberling, Felix; Kapusta, Peter; Dosche, Carsten

2010-02-01

Today fluorescence lifetime imaging microscopy (FLIM) has become an extremely powerful technique in life sciences. The independency of the fluorescence decay time on fluorescence dye concentration and emission intensity circumvents many artefacts arising from intensity based measurements. To minimize cell damage and improve scan depth, a combination with two-photon (2P) excitation is quite promising. Here, we describe the implementation of a 2P-FLIM setup for biological applications. For that we used a commercial fluorescence lifetime microscope system. 2P-excitation at 780nm was achieved by a non-tuneable, but inexpensive and easily manageable mode-locked fs-fiber laser. Time-resolved fluorescence image acquisition was performed by objective-scanning with the reversed time-correlated single photon counting (TCSPC) technique. We analyzed the suitability of the pH-sensitive dye BCECF and the chloride-sensitive dye MQAE for recordings in an insect tissue. Both parameters are quite important, since they affect a plethora of physiological processes in living tissues. We performed a straight forward in situ calibration method to link the fluorescence decay time with the respective ion concentration and carried out spatially resolved measurements under resting conditions. BCECF still offered only a limited dynamic range regarding fluorescence decay time changes under physiologically pH values. However, MQAE proofed to be well suited to record chloride concentrations in the physiologically relevant range. Subsequently, several chloride transport pathways underlying the intracellular chloride homeostasis were investigated pharmacologically. In conclusion, 2P-FLIM is well suited for ion detection in living tissues due to precise and reproducible decay time measurements in combination with reduced cell and dye damages.

Commissioning of an integrated platform for time-resolved treatment delivery in scanned ion beam therapy by means of optical motion monitoring.

PubMed

Fattori, G; Saito, N; Seregni, M; Kaderka, R; Pella, A; Constantinescu, A; Riboldi, M; Steidl, P; Cerveri, P; Bert, C; Durante, M; Baroni, G

2014-12-01

The integrated use of optical technologies for patient monitoring is addressed in the framework of time-resolved treatment delivery for scanned ion beam therapy. A software application has been designed to provide the therapy control system (TCS) with a continuous geometrical feedback by processing the external surrogates tridimensional data, detected in real-time via optical tracking. Conventional procedures for phase-based respiratory phase detection were implemented, as well as the interface to patient specific correlation models, in order to estimate internal tumor motion from surface markers. In this paper, particular attention is dedicated to the quantification of time delays resulting from system integration and its compensation by means of polynomial interpolation in the time domain. Dedicated tests to assess the separate delay contributions due to optical signal processing, digital data transfer to the TCS and passive beam energy modulation actuation have been performed. We report the system technological commissioning activities reporting dose distribution errors in a phantom study, where the treatment of a lung lesion was simulated, with both lateral and range beam position compensation. The zero-delay systems integration with a specific active scanning delivery machine was achieved by tuning the amount of time prediction applied to lateral (14.61 ± 0.98 ms) and depth (34.1 ± 6.29 ms) beam position correction signals, featuring sub-millimeter accuracy in forward estimation. Direct optical target observation and motion phase (MPh) based tumor motion discretization strategies were tested, resulting in 20.3(2.3)% and 21.2(9.3)% median (IQR) percentual relative dose difference with respect to static irradiation, respectively. Results confirm the technical feasibility of the implemented strategy towards 4D treatment delivery, with negligible percentual dose deviations with respect to static irradiation.

Sub-micron resolution of localized ion beam induced charge reduction in silicon detectors damaged by heavy ions

DOE PAGES

Auden, Elizabeth C.; Pacheco, Jose L.; Bielejec, Edward; ...

2015-12-01

In this study, displacement damage reduces ion beam induced charge (IBIC) through Shockley-Read-Hall recombination. Closely spaced pulses of 200 keV Si ++ ions focused in a 40 nm beam spot are used to create damage cascades within 0.25 μm 2 areas. Damaged areas are detected through contrast in IBIC signals generated with focused ion beams of 200 keV Si ++ ions and 60 keV Li + ions. IBIC signal reduction can be resolved over sub-micron regions of a silicon detector damaged by as few as 1000 heavy ions.

Sub-micron resolution of localized ion beam induced charge reduction in silicon detectors damaged by heavy ions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Auden, Elizabeth C.; Pacheco, Jose L.; Bielejec, Edward

In this study, displacement damage reduces ion beam induced charge (IBIC) through Shockley-Read-Hall recombination. Closely spaced pulses of 200 keV Si ++ ions focused in a 40 nm beam spot are used to create damage cascades within 0.25 μm 2 areas. Damaged areas are detected through contrast in IBIC signals generated with focused ion beams of 200 keV Si ++ ions and 60 keV Li + ions. IBIC signal reduction can be resolved over sub-micron regions of a silicon detector damaged by as few as 1000 heavy ions.

Travelling-wave ion mobility mass spectrometry and negative ion fragmentation of hybrid and complex N-glycans

PubMed Central

Harvey, David J.; Scarff, Charlotte A.; Edgeworth, Matthew; Pagel, Kevin; Thalassinos, Konstantinos; Struwe, Weston B.; Crispin, Max; Scrivens, Jim

2016-01-01

Nitrogen cross sections of hybrid and complex glycans released from the glycoproteins IgG, gp120 (from human immunodeficiency virus), ovalbumin, α1-acid glycoprotein, thyroglobulin and fucosylated glycoproteins from the human parotid gland were measured with a travelling-wave ion mobility mass spectrometer using dextran as the calibrant. The utility of this instrument for isomer separation was also investigated. Some isomers, such as Man3GlcNAc3 from chicken ovalbumin and Man3GlcNAc3Fuc1 from thyroglobulin could be partially resolved and identified by their negative ion fragmentation spectra. Several other larger glycans, however, although existing as isomers, produced only asymmetric rather than separated arrival time distributions (ATDs). Nevertheless, in these cases, isomers could often be detected by plotting extracted fragment ATDs of diagnostic fragment ions from the negative ion spectra obtained in the transfer cell of the Waters Synapt mass spectrometer. Coincidence in the drift times of all fragment ions with an overall asymmetric ATD profile usually suggested that separations were due to conformers or anomers, whereas symmetrical ATDs of fragments showing differences in drift times indicated isomer separation. Although some significant differences in cross sections were found for the smaller isomeric glycans, the differences found for the larger compounds were usually too small to be analytically useful. Possible correlations between cross sections and structural types were also investigated and it was found that complex glycans tended to have slightly smaller cross sections than high-mannose glycans of comparable molecular weight. In addition, biantennary glycans containing a core fucose and/or a bisecting GlcNAc residue fell on different mobility-m/z trend lines to those glycans not so substituted with both of these substituents contributing to larger cross sections. PMID:27477117

Calibration of the OHREX high-resolution imaging crystal spectrometer at the Livermore electron beam ion traps

NASA Astrophysics Data System (ADS)

Hell, N.; Beiersdorfer, P.; Magee, E. W.; Brown, G. V.

2016-11-01

We report the calibration of the Orion High-Resolution X-ray (OHREX) imaging crystal spectrometer at the EBIT-I electron beam ion trap at Livermore. Two such instruments, dubbed OHREX-1 and OHREX-2, are fielded for plasma diagnostics at the Orion laser facility in the United Kingdom. The OHREX spectrometer can simultaneously house two spherically bent crystals with a radius of curvature of r = 67.2 cm. The focusing properties of the spectrometer allow both for larger distance to the source due to the increase in collected light and for observation of extended sources. OHREX is designed to cover a 2.5°-3° spectral range at Bragg angles around 51.3°. The typically high resolving powers at these large Bragg angles are ideally suited for line shape diagnostics. For instance, the nominal resolving power of the instrument (>10 000) is much higher than the effective resolving power associated with the Doppler broadening due to the temperature of the trapped ions in EBIT-I. The effective resolving power is only around 3000 at typical EBIT-I conditions, which nevertheless is sufficient to set up and test the instrument's spectral characteristics. We have calibrated the spectral range for a number of crystals using well known reference lines in the first and second order and derived the ion temperatures from these lines. We have also made use of the 50 μm size of the EBIT-I source width to characterize the spatial focusing of the spectrometer.

Calibration of the OHREX high-resolution imaging crystal spectrometer at the Livermore electron beam ion traps

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hell, N.; Dr. Remeis-Sternwarte and ECAP, Universität Erlangen-Nürnberg, Bamberg 96049; Beiersdorfer, P.

2016-11-15

We report the calibration of the Orion High-Resolution X-ray (OHREX) imaging crystal spectrometer at the EBIT-I electron beam ion trap at Livermore. Two such instruments, dubbed OHREX-1 and OHREX-2, are fielded for plasma diagnostics at the Orion laser facility in the United Kingdom. The OHREX spectrometer can simultaneously house two spherically bent crystals with a radius of curvature of r = 67.2 cm. The focusing properties of the spectrometer allow both for larger distance to the source due to the increase in collected light and for observation of extended sources. OHREX is designed to cover a 2.5°–3° spectral range atmore » Bragg angles around 51.3°. The typically high resolving powers at these large Bragg angles are ideally suited for line shape diagnostics. For instance, the nominal resolving power of the instrument (>10 000) is much higher than the effective resolving power associated with the Doppler broadening due to the temperature of the trapped ions in EBIT-I. The effective resolving power is only around 3000 at typical EBIT-I conditions, which nevertheless is sufficient to set up and test the instrument’s spectral characteristics. We have calibrated the spectral range for a number of crystals using well known reference lines in the first and second order and derived the ion temperatures from these lines. We have also made use of the 50 μm size of the EBIT-I source width to characterize the spatial focusing of the spectrometer.« less

A compact high-resolution X-ray ion mobility spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reinecke, T.; Kirk, A. T.; Heptner, A.

For the ionization of gaseous samples, most ion mobility spectrometers employ radioactive ionization sources, e.g., containing {sup 63}Ni or {sup 3}H. Besides legal restrictions, radioactive materials have the disadvantage of a constant radiation with predetermined intensity. In this work, we replaced the {sup 3}H source of our previously described high-resolution ion mobility spectrometer with 75 mm drift tube length with a commercially available X-ray source. It is shown that the current configuration maintains the resolving power of R = 100 which was reported for the original setup containing a {sup 3}H source. The main advantage of an X-ray source ismore » that the intensity of the radiation can be adjusted by varying its operating parameters, i.e., filament current and acceleration voltage. At the expense of reduced resolving power, the sensitivity of the setup can be increased by increasing the activity of the source. Therefore, the performance of the setup can be adjusted to the specific requirements of any application. To investigate the relation between operating parameters of the X-Ray source and the performance of the ion mobility spectrometer, parametric studies of filament current and acceleration voltage are performed and the influence on resolving power, peak height, and noise is analyzed.« less

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation.

PubMed

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho, Jr-Wei; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-28

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH 3 ) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH 3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S 1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH 3 ] + cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ∼70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Watching proton transfer in real time: Ultrafast photoionization-induced proton transfer in phenol-ammonia complex cation

NASA Astrophysics Data System (ADS)

Shen, Ching-Chi; Tsai, Tsung-Ting; Wu, Jun-Yi; Ho-Wei, Jr.; Chen, Yi-Wei; Cheng, Po-Yuan

2017-10-01

In this paper, we give a full account of our previous work [C. C. Shen et al., J. Chem. Phys. 141, 171103 (2014)] on the study of an ultrafast photoionization-induced proton transfer (PT) reaction in the phenol-ammonia (PhOH-NH3) complex using ultrafast time-resolved ion photofragmentation spectroscopy implemented by the photoionization-photofragmentation pump-probe detection scheme. Neutral PhOH-NH3 complexes prepared in a free jet are photoionized by femtosecond 1 + 1 resonance-enhanced multiphoton ionization via the S1 state. The evolving cations are then probed by delayed pulses that result in ion fragmentation, and the ionic dynamics is followed by measuring the parent-ion depletion as a function of the pump-probe delay time. By comparing with systems in which PT is not feasible and the steady-state ion photofragmentation spectra, we concluded that the observed temporal evolutions of the transient ion photofragmentation spectra are consistent with an intracomplex PT reaction after photoionization from the initial non-PT to the final PT structures. Our experiments revealed that PT in [PhOH-NH3]+ cation proceeds in two distinct steps: an initial impulsive wave-packet motion in ˜70 fs followed by a slower relaxation of about 1 ps that stabilizes the system into the final PT configuration. These results indicate that for a barrierless PT system, even though the initial PT motions are impulsive and ultrafast, the time scale to complete the reaction can be much slower and is determined by the rate of energy dissipation into other modes.

Parallel Spectral Acquisition with an Ion Cyclotron Resonance Cell Array.

PubMed

Park, Sung-Gun; Anderson, Gordon A; Navare, Arti T; Bruce, James E

2016-01-19

Mass measurement accuracy is a critical analytical figure-of-merit in most areas of mass spectrometry application. However, the time required for acquisition of high-resolution, high mass accuracy data limits many applications and is an aspect under continual pressure for development. Current efforts target implementation of higher electrostatic and magnetic fields because ion oscillatory frequencies increase linearly with field strength. As such, the time required for spectral acquisition of a given resolving power and mass accuracy decreases linearly with increasing fields. Mass spectrometer developments to include multiple high-resolution detectors that can be operated in parallel could further decrease the acquisition time by a factor of n, the number of detectors. Efforts described here resulted in development of an instrument with a set of Fourier transform ion cyclotron resonance (ICR) cells as detectors that constitute the first MS array capable of parallel high-resolution spectral acquisition. ICR cell array systems consisting of three or five cells were constructed with printed circuit boards and installed within a single superconducting magnet and vacuum system. Independent ion populations were injected and trapped within each cell in the array. Upon filling the array, all ions in all cells were simultaneously excited and ICR signals from each cell were independently amplified and recorded in parallel. Presented here are the initial results of successful parallel spectral acquisition, parallel mass spectrometry (MS) and MS/MS measurements, and parallel high-resolution acquisition with the MS array system.

Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS)more » ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. As a result, controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the presence of the organosulfate functional group.« less

Ion mobility spectrometry–mass spectrometry (IMS–MS) for on- and offline analysis of atmospheric gas and aerosol species

DOE PAGES

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; ...

2016-07-25

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS–MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS–MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI–IMS–MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS)more » ambient field campaign in the forested SE US. The ambient IMS–MS signals are consistent with laboratory IMS–MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS–MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS–MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. As a result, controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the presence of the organosulfate functional group.« less

Ion mobility spectrometry-mass spectrometry (IMS-MS) for on- and offline analysis of atmospheric gas and aerosol species

NASA Astrophysics Data System (ADS)

Krechmer, Jordan E.; Groessl, Michael; Zhang, Xuan; Junninen, Heikki; Massoli, Paola; Lambe, Andrew T.; Kimmel, Joel R.; Cubison, Michael J.; Graf, Stephan; Lin, Ying-Hsuan; Budisulistiorini, Sri H.; Zhang, Haofei; Surratt, Jason D.; Knochenmuss, Richard; Jayne, John T.; Worsnop, Douglas R.; Jimenez, Jose-Luis; Canagaratna, Manjula R.

2016-07-01

Measurement techniques that provide molecular-level information are needed to elucidate the multiphase processes that produce secondary organic aerosol (SOA) species in the atmosphere. Here we demonstrate the application of ion mobility spectrometry-mass spectrometry (IMS-MS) to the simultaneous characterization of the elemental composition and molecular structures of organic species in the gas and particulate phases. Molecular ions of gas-phase organic species are measured online with IMS-MS after ionization with a custom-built nitrate chemical ionization (CI) source. This CI-IMS-MS technique is used to obtain time-resolved measurements (5 min) of highly oxidized organic molecules during the 2013 Southern Oxidant and Aerosol Study (SOAS) ambient field campaign in the forested SE US. The ambient IMS-MS signals are consistent with laboratory IMS-MS spectra obtained from single-component carboxylic acids and multicomponent mixtures of isoprene and monoterpene oxidation products. Mass-mobility correlations in the 2-D IMS-MS space provide a means of identifying ions with similar molecular structures within complex mass spectra and are used to separate and identify monoterpene oxidation products in the ambient data that are produced from different chemical pathways. Water-soluble organic carbon (WSOC) constituents of fine aerosol particles that are not resolvable with standard analytical separation methods, such as liquid chromatography (LC), are shown to be separable with IMS-MS coupled to an electrospray ionization (ESI) source. The capability to use ion mobility to differentiate between isomers is demonstrated for organosulfates derived from the reactive uptake of isomers of isoprene epoxydiols (IEPOX) onto wet acidic sulfate aerosol. Controlled fragmentation of precursor ions by collisionally induced dissociation (CID) in the transfer region between the IMS and the MS is used to validate MS peak assignments, elucidate structures of oligomers, and confirm the presence of the organosulfate functional group.

The influence of prepulse level on the 3p-3s XUV laser output from Ne-like ions of Zn, Cu and Ni

NASA Astrophysics Data System (ADS)

MacPhee, A. G.; Lewis, C. L. S.; Warwick, P. J.; Weaver, I.; Jaeglé, P.; Carillon, A.; Jamelot, G.; Klisnick, A.; Rus, B.; Zeitoun, Ph.; Nantel, M.; Goedkindt, P.; Sebban, S.; Tallents, G. J.; Demir, A.; Holden, M.; Krishnan, J.

1997-02-01

We have studied the effect of prepulses in enhancing the efficiency of generating ASE beams in soft X-ray laser plasma amplifiers based on pumping Ne-like ions. Slab targets were irradiated with a weak prepulse followed by a main plasma heating pulse of nanosecond duration. Time-integrated: time and spectrally resolved and time and angularly resolved lasing emissions on the 3p-3s ( J = 0-1) XUV lasing lines of Ne-like Ni, Cu and Zn at wavelengths 232 Å, 221 Å and 212 Å respectively have been monitored. Measurements were made for pre-pulse/main-pulse intensity ratios from 10 -5-10 -1 and for pump delay times of 2 ns and 4.5 ns. Zinc is shown to exhibit a peak in output intensity at ˜ 2 × 10 -3 pre-pulse fraction for a 4.5 ns pump delay, with a main pulse pump intensity of ˜ 1.3 × 10 13W cm -2 on a 20 mm target. The Zn lasing emission had a duration of ˜ 240 ps and this was insensitive to prepulse fraction. The J = 0-1 XUV laser output for nickel and copper increased monotonically with prepulse fraction, with copper targets showing least sensitivity to either prepulse level or prepulse to main pulse delay. Under the conditions of the study, the pre-pulse level was observed to have no significant influence on the output intensity of the 3p-3s ( J = 2-1) lines of any of the elements investigated.

An angle-resolved, wavelength-dispersive x-ray fluorescence spectrometer for depth profile analysis of ion-implanted semiconductors using synchrotron radiation

NASA Astrophysics Data System (ADS)

Schmitt, W.; Hormes, J.; Kuetgens, U.; Gries, W. H.

1992-01-01

An apparatus for angle-resolved, wavelength-dispersive x-ray fluorescence spectroscopy with synchrotron radiation has been built and tested at the beam line BN2 of the Bonn electron stretcher and accelerator (ELSA). The apparatus is to be used for nondestructive depth profile analysis of ion-implanted semiconductors as part of the multinational Versailles Project of Advanced Materials and Standards (VAMAS) project on ion-implanted reference materials. In particular, the centroid depths of depth profiles of various implants is to be determined by use of the angle-resolved signal ratio technique. First results of measurements on implants of phosphorus (100 keV, 1016 cm-2) and sulfur (200 keV, 1014 cm-2) in silicon wafers using ``white'' synchrotron radiation are presented and suggest that it should be generally possible to measure the centroid depth of an implant at dose densities as low as 1014 cm-2. Some of the apparative and technical requirements are discussed which are peculiar to the use of synchrotron radiation in general and to the use of nonmonochromatized radiation in particular.

Functional nicotinic acetylcholine receptor reconstitution in Au(111)-supported thiolipid monolayers

NASA Astrophysics Data System (ADS)

Pissinis, Diego E.; Diaz, Carolina; Maza, Eliana; Bonini, Ida C.; Barrantes, Francisco J.; Salvarezza, Roberto C.; Schilardi, Patricia L.

2015-09-01

The insertion and function of the muscle-type nicotinic acetylcholine receptor (nAChR) in Au(111)-supported thiolipid self-assembled monolayers have been studied by atomic force microscopy (AFM), surface plasmon resonance (SPR), and electrochemical techniques. It was possible for the first time to resolve the supramolecular arrangement of the protein spontaneously inserted in a thiolipid monolayer in an aqueous solution. Geometric supramolecular arrays of nAChRs were observed, most commonly in a triangular form compatible with three nAChR dimers of ~20 nm each. Addition of the full agonist carbamoylcholine activated and opened the nAChR ion channel, as revealed by the increase in capacitance relative to that of the nAChR-thiolipid system under basal conditions. Thus, the self-assembled system appears to be a viable biomimetic model to measure ionic conductance mediated by ion-gated ion channels under different experimental conditions, with potential applications in biotechnology and pharmacology.

High-resolution spectroscopy for Doppler-broadening ion temperature measurements of implosions at the National Ignition Facility.

PubMed

Koch, J A; Stewart, R E; Beiersdorfer, P; Shepherd, R; Schneider, M B; Miles, A R; Scott, H A; Smalyuk, V A; Hsing, W W

2012-10-01

Future implosion experiments at the national ignition facility (NIF) will endeavor to simultaneously measure electron and ion temperatures with temporal and spatial resolution in order to explore non-equilibrium temperature distributions and their relaxation toward equilibrium. In anticipation of these experiments, and with understanding of the constraints of the NIF facility environment, we have explored the use of Doppler broadening of mid-Z dopant emission lines, such as krypton He-α at 13 keV, as a diagnostic of time- and potentially space-resolved ion temperature. We have investigated a number of options analytically and with numerical raytracing, and we have identified several promising candidate spectrometer designs that meet the expected requirements of spectral and temporal resolution and data signal-to-noise ratio for gas-filled exploding pusher implosions, while providing maximum flexibility for use on a variety of experiments that potentially include burning plasma.

Status of the Frankfurt low energy electrostatic storage ring (FLSR)

NASA Astrophysics Data System (ADS)

King, F.; Kruppi, T.; Müller, J.; Dörner, R.; Schmidt, L. Ph H.; Schmidt-Böcking, H.; Stiebing, K. E.

2015-11-01

Frankfurt low-energy storage ring (FLSR) is an electrostatic storage ring for low-energy ions up to q · 80 keV (q being the ion charge state) at Institut für Kernphysik der Goethe-Universität, Frankfurt am Main, Germany. It has especially been designed to provide a basis for experiments on the dynamics of ionic and molecular collisions in complete kinematics, as well as for high precision and time resolved laser spectroscopy. The ring has ‘racetrack’ geometry with a circumference of 14.23 m. It comprises four experimental/diagnostic sections with regions of enhanced ion density (interaction regions). First beam has successfully been stored in FLSR in summer 2013. Since then the performance of the ring has continuously been improved and an electron target for experiments on dissociative recombination has been installed in one of the experimental sections.

Inter- and intraconfigurational luminescence of Er3+ ions in BaY2F8 under VUV excitation

NASA Astrophysics Data System (ADS)

Kirm, M.; Lichtenberg, H.; Makhov, V. N.; Negodin, E.; Ouvarova, T. V.; Suljoti, E.; True, M.; Zimmerer, G.

Using energy- and time-resolved spectroscopy the luminescence properties of Er3+ doped BaY2F8 crystals were investigated at 10 K under VUV synchrotron radiation excitation. Radiative intraconfigurational f - f and interconfigurational d - f transitions in Er3+ ions were observed under f - d excitation. Whereas the onset of S-4(3/2) population via f - d excitation starts at 59 900 cm(-1) , efficient excitation of emissions arising from the P-2(3/2) state begins only above 67 000 cm(-1) in VUV region. Such behaviour can be explained by a cross-relaxation process of the type (F-2(2)(5/2) , I-4(15/2))-->(P-2(3/2) , P-2(3/2)) taking place within f -states of Er3+ ions finally populating the emitting P-2(3/2) state.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, Xing; Ibrahim, Yehia M.; Chen, Tsung-Chi

We report the first evaluation of a platform coupling a high speed field asymmetric ion mobility spectrometry microchip (µFAIMS) with drift tube ion mobility and mass spectrometry (IMS-MS). The µFAIMS/IMS-MS platform was used to analyze biological samples and simultaneously acquire multidimensional information of detected features from the measured FAIMS compensation fields and IMS drift times, while also obtaining accurate ion masses. These separations thereby increase the overall separation power, resulting increased information content, and provide more complete characterization of more complex samples. The separation conditions were optimized for sensitivity and resolving power by the selection of gas compositions and pressuresmore » in the FAIMS and IMS separation stages. The resulting performance provided three dimensional separations, benefitting both broad complex mixture studies and targeted analyses by e.g. improving isomeric separations and allowing detection of species obscured by “chemical noise” and other interfering peaks.« less

Experimental characterization of a transition from collisionless to collisional interaction between head-on-merging supersonic plasma jets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moser, Auna L., E-mail: mosera@fusion.gat.com; Hsu, Scott C., E-mail: scotthsu@lanl.gov

We present results from experiments on the head-on merging of two supersonic plasma jets in an initially collisionless regime for the counter-streaming ions. The plasma jets are of either an argon/impurity or hydrogen/impurity mixture and are produced by pulsed-power-driven railguns. Based on time- and space-resolved fast-imaging, multi-chord interferometry, and survey-spectroscopy measurements of the overlapping region between the merging jets, we observe that the jets initially interpenetrate, consistent with calculated inter-jet ion collision lengths, which are long. As the jets interpenetrate, a rising mean-charge state causes a rapid decrease in the inter-jet ion collision length. Finally, the interaction becomes collisional andmore » the jets stagnate, eventually producing structures consistent with collisional shocks. These experimental observations can aid in the validation of plasma collisionality and ionization models for plasmas with complex equations of state.« less

Evaluation of the Sequential Spot Sampler (S3) for time-resolved measurement of PM2.5 sulfate and nitrate through lab and field measurements

NASA Astrophysics Data System (ADS)

Hecobian, A.; Evanoski-Cole, A.; Eiguren-Fernandez, A.; Sullivan, A. P.; Lewis, G. S.; Hering, S. V.; Collett, J. L., Jr.

2016-02-01

The Sequential Spot Sampler (S3), a newly developed instrument to collect aerosols for time-resolved chemical composition measurements, was evaluated in the laboratory and field for the measurement of particulate sulfate and nitrate. The S3 uses a multi-temperature condensation growth tube to grow individual aerosols to droplets which are then deposited as a ˜ 1 mm diameter dry spot at the end of the growth tube in a 100 µL well of a multi-well plate. The well plate advances automatically to provide a sequence of time-resolved samples. The collected aerosols are subsequently analyzed in the laboratory. The sample is concentrated during the collection process, and the laboratory extraction and analysis steps can be automated. The well plate, as received from the field, is placed onto a needle-based autosampler that adds liquid for sample extraction and injects sample extract from each well onto an ion chromatograph for analysis. Laboratory evaluation for sulfate and nitrate ions showed that poly ether ether ketone (PEEK) used as well plate material does not contribute any artifacts; a 60 min extraction procedure leads to the recovery of sulfate and nitrate from the dry spots at above 95 % extraction efficiency; and samples stored frozen and analyzed up to 23 months later show less than a 10 % change in sulfate and nitrate concentrations. The limit of detection was 0.5 µg m-3 for sulfate and 0.2 µg m-3 for nitrate for a 1 h sampling period. In a month-long field study conducted in southern California, two S3s were deployed alongside a URG denuder-filter-pack and a Particle-Into-Liquid Sampler combined with an Ion Chromatograph (PILS-IC). Collocated S3 sampler concentrations compared by linear regression show good agreement, with r2 = 0.99 and slope = 0.99 (±0.004) µg m-3 for sulfate and r2 = 0.99 and slope = 1.0 (±0.006) µg m-3 for nitrate. When compared to the URG denuder-filter-pack and the PILS-IC, the S3 sulfate and nitrate concentrations yielded correlations above 0.84 for the square of the correlation coefficient and regression slopes close to 1.

Ultrafast nuclear dynamics in halomethanes studied with time-resolved Coulomb explosion imaging and channel-selective Fourier spectroscopy

NASA Astrophysics Data System (ADS)

Malakar, Y.; Kaderiya, B.; Pearson, W. L.; Ziaee, F.; Kanaka Raju, P.; Zohrabi, M.; Jensen, K.; Rajput, J.; Ben-Itzhak, I.; Rolles, D.; Rudenko, A.

2016-05-01

Halomethanes have recently attracted considerable attention since they often serve as prototype systems for laser-controlled chemistry (e.g., selective bond breaking or concerted elimination reactions), and are important molecules in atmospheric chemistry. Here we combine a femtosecond laser pump-probe setup with coincident 3D ion momentum imaging apparatus to study strong-field induced nuclear dynamics in methane and several of its halogenated derivatives (CH3 I, CH2 I2, CH2 ICl). We apply a time-resolved Coulomb explosion imaging technique to map the nuclear motion on both, bound and continuum potential surfaces, disentangle different fragmentation pathways and, for halogenated molecules, observe clear signatures of vibrational wave packets in neutral or ionized states. Channel-selective and kinetic-energy resolved Fourier analysis of these data allows for unique identification of different electronic states and vibrational modes responsible for a particular structure. Supported by the Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U. S. DOE. K. R. P. and W. L. P. supported by NSF Award No. IIA-143049. K.J. supported by the NSF-REU Grant No. PHYS-1461251.

Spectral and Atomic Physics Analysis of Xenon L-Shell Emission From High Energy Laser Produced Plasmas

NASA Astrophysics Data System (ADS)

Thorn, Daniel; Kemp, G. E.; Widmann, K.; Benjamin, R. D.; May, M. J.; Colvin, J. D.; Barrios, M. A.; Fournier, K. B.; Liedahl, D.; Moore, A. S.; Blue, B. E.

2016-10-01

The spectrum of the L-shell (n =2) radiation in mid to high-Z ions is useful for probing plasma conditions in the multi-keV temperature range. Xenon in particular with its L-shell radiation centered around 4.5 keV is copiously produced from plasmas with electron temperatures in the 5-10 keV range. We report on a series of time-resolved L-shell Xe spectra measured with the NIF X-ray Spectrometer (NXS) in high-energy long-pulse (>10 ns) laser produced plasmas at the National Ignition Facility. The resolving power of the NXS is sufficiently high (E/ ∂E >100) in the 4-5 keV spectral band that the emission from different charge states is observed. An analysis of the time resolved L-shell spectrum of Xe is presented along with spectral modeling by detailed radiation transport and atomic physics from the SCRAM code and comparison with predictions from HYDRA a radiation-hydrodynamics code with inline atomic-physics from CRETIN. This work was performed under the auspices of the U.S. Department of Energy by LLNL under Contract DE-AC52-07NA27344.

Correlation ion mobility spectroscopy

DOEpatents

Pfeifer, Kent B [Los Lunas, NM; Rohde, Steven B [Corrales, NM

2008-08-26

Correlation ion mobility spectrometry (CIMS) uses gating modulation and correlation signal processing to improve IMS instrument performance. Closely spaced ion peaks can be resolved by adding discriminating codes to the gate and matched filtering for the received ion current signal, thereby improving sensitivity and resolution of an ion mobility spectrometer. CIMS can be used to improve the signal-to-noise ratio even for transient chemical samples. CIMS is especially advantageous for small geometry IMS drift tubes that can otherwise have poor resolution due to their small size.

Interplanetary shocks, Plasma waves and turbulence, Kinetic waves and instabilities, STEREO spacecraft

NASA Astrophysics Data System (ADS)

Cohen, Z.; Breneman, A. W.; Cattell, C. A.; Davis, L.; Grul, P.; Kersten, K.; Wilson, L. B., III

2017-12-01

Determining the role of plasma waves in providing energy dissipation at shock waves is of long-standing interest. Interplanetary (IP) shocks serve as a large database of low Mach number shocks. We examine electric field waveforms captured by the Time Domain Sampler (TDS) on the STEREO spacecraft during the ramps of IP shocks, with emphasis on captures lasting 2.1 seconds. Previous work has used captures of shorter duration (66 and 131 ms on STEREO, and 17 ms on WIND), which allowed for observation of waves with maximum (minimum) frequencies of 125 kHz (15 Hz), 62.5 kHz (8 Hz), and 60 kHz (59 Hz), respectively. The maximum frequencies are comparable to 2-8 times the plasma frequency in the solar wind, enabling observation of Langmuir waves, ion acoustic, and some whistler-mode waves. The 2 second captures resolve lower frequencies ( few Hz), which allows us to analyze packet structure of the whistler-mode waves and some ion acoustic waves. The longer capture time also improves the resolvability of simultaneous wave modes and of waves with frequencies on the order of 10s of Hz. Langmuir waves, however, cannot be identified at this sampling rate, since the plasma frequency is usually higher than 3.9 kHz. IP shocks are identified from multiple databases (Helsinki heliospheric shock database at http://ipshocks.fi, and the STEREO level 3 shock database at ftp://stereoftp.nascom.nasa.gov/pub/ins_data/impact/level3/). Our analysis focuses on TDS captures in shock ramp regions, with ramp durations determined from magnetic field data taken at 8 Hz. Software is used to identify multiple wave modes in any given capture and classify waves as Langmuir, ion acoustic, whistler, lower hybrid, electron cyclotron drift instability, or electrostatic solitary waves. Relevant frequencies are determined from density and magnetic field data collected in situ. Preliminary results suggest that large amplitude (∼ 5 mV/m) ion acoustic waves are most prevalent in the ramp, in agreement with Wilson, et al. Other modes are also observed. Statistical results will be presented and compared with previous studies and theoretical predictions.

STEREO Observations of Waves in the Ramp Regions of Interplanetary Shocks

NASA Astrophysics Data System (ADS)

Cohen, Z.; Breneman, A. W.; Cattell, C. A.; Davis, L.; Grul, P.; Kersten, K.; Wilson, L. B., III

2017-12-01

Determining the role of plasma waves in providing energy dissipation at shock waves is of long-standing interest. Interplanetary (IP) shocks serve as a large database of low Mach number shocks. We examine electric field waveforms captured by the Time Domain Sampler (TDS) on the STEREO spacecraft during the ramps of IP shocks, with emphasis on captures lasting 2.1 seconds. Previous work has used captures of shorter duration (66 and 131 ms on STEREO, and 17 ms on WIND), which allowed for observation of waves with maximum (minimum) frequencies of 125 kHz (15 Hz), 62.5 kHz (8 Hz), and 60 kHz (59 Hz), respectively. The maximum frequencies are comparable to 2-8 times the plasma frequency in the solar wind, enabling observation of Langmuir waves, ion acoustic, and some whistler-mode waves. The 2 second captures resolve lower frequencies ( few Hz), which allows us to analyze packet structure of the whistler-mode waves and some ion acoustic waves. The longer capture time also improves the resolvability of simultaneous wave modes and of waves with frequencies on the order of 10s of Hz. Langmuir waves, however, cannot be identified at this sampling rate, since the plasma frequency is usually higher than 3.9 kHz. IP shocks are identified from multiple databases (Helsinki heliospheric shock database at http://ipshocks.fi, and the STEREO level 3 shock database at ftp://stereoftp.nascom.nasa.gov/pub/ins_data/impact/level3/). Our analysis focuses on TDS captures in shock ramp regions, with ramp durations determined from magnetic field data taken at 8 Hz. Software is used to identify multiple wave modes in any given capture and classify waves as Langmuir, ion acoustic, whistler, lower hybrid, electron cyclotron drift instability, or electrostatic solitary waves. Relevant frequencies are determined from density and magnetic field data collected in situ. Preliminary results suggest that large amplitude (≥ 5 mV/m) ion acoustic waves are most prevalent in the ramp, in agreement with Wilson, et al. Other modes are also observed. Statistical results will be presented and compared with previous studies and theoretical predictions.

Communication—indentation of Li-ion pouch cell: Effect of material homogenization on prediction of internal short circuit

DOE PAGES

Kumar, A.; Kalnaus, Sergiy; Simunovic, Srdjan; ...

2016-09-12

We performed finite element simulations of spherical indentation of Li-ion pouch cells. Our model fully resolves different layers in the cell. The results of the layer resolved models were compared to the models available in the literature that treat the cell as an equivalent homogenized continuum material. Simulations were carried out for different sizes of the spherical indenter. Here, we show that calibration of a failure criterion for the cell in the homogenized model depends on the indenter size, whereas in the layer-resoled model, such dependency is greatly diminished.

FLSR - The Frankfurt low energy storage ring

NASA Astrophysics Data System (ADS)

Stiebing, K. E.; Alexandrov, V.; Dörner, R.; Enz, S.; Kazarinov, N. Yu.; Kruppi, T.; Schempp, A.; Schmidt Böcking, H.; Völp, M.; Ziel, P.; Dworak, M.; Dilfer, W.

2010-02-01

An electrostatic storage ring for low-energy ions with a design energy of 50 keV is presently being set up at the Institut für Kernphysik der Johann Wolfgang Goethe-Universität Frankfurt am Main, Germany (IKF). This new device will provide a basis for new experiments on the dynamics of ionic and molecular collisions, as well as for high precision and time resolved laser spectroscopy. In this article, the design parameters of this instrument are reported.

Ultrafast Structural Dynamics in Combustion Relevant Model Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Weber, Peter M.

2014-03-31

The research project explored the time resolved structural dynamics of important model reaction system using an array of novel methods that were developed specifically for this purpose. They include time resolved electron diffraction, time resolved relativistic electron diffraction, and time resolved Rydberg fingerprint spectroscopy. Toward the end of the funding period, we also developed time-resolved x-ray diffraction, which uses ultrafast x-ray pulses at LCLS. Those experiments are just now blossoming, as the funding period expired. In the following, the time resolved Rydberg Fingerprint Spectroscopy is discussed in some detail, as it has been a very productive method. The binding energymore » of an electron in a Rydberg state, that is, the energy difference between the Rydberg level and the ground state of the molecular ion, has been found to be a uniquely powerful tool to characterize the molecular structure. To rationalize the structure sensitivity we invoke a picture from electron diffraction: when it passes the molecular ion core, the Rydberg electron experiences a phase shift compared to an electron in a hydrogen atom. This phase shift requires an adjustment of the binding energy of the electron, which is measurable. As in electron diffraction, the phase shift depends on the molecular, geometrical structure, so that a measurement of the electron binding energy can be interpreted as a measurement of the molecule’s structure. Building on this insight, we have developed a structurally sensitive spectroscopy: the molecule is first elevated to the Rydberg state, and the binding energy is then measured using photoelectron spectroscopy. The molecule’s structure is read out as the binding energy spectrum. Since the photoionization can be done with ultrafast laser pulses, the technique is inherently capable of a time resolution in the femtosecond regime. For the purpose of identifying the structures of molecules during chemical reactions, and for the analysis of molecular species in the hot environments of combustion processes, there are several features that make the Rydberg ionization spectroscopy uniquely useful. First, the Rydberg electron’s orbit is quite large and covers the entire molecule for most molecular structures of combustion interest. Secondly, the ionization does not change vibrational quantum numbers, so that even complicated and large molecules can be observed with fairly well resolved spectra. In fact, the spectroscopy is blind to vibrational excitation of the molecule. This has the interesting consequence for the study of chemical dynamics, where the molecules are invariably very energetic, that the molecular structures are observed unobstructed by the vibrational congestion that dominates other spectroscopies. This implies also that, as a tool to probe the time-dependent structural dynamics of chemically interesting molecules, Rydberg spectroscopy may well be better suited than electron or x-ray diffraction. With recent progress in calculating Rydberg binding energy spectra, we are approaching the point where the method can be evolved into a structure determination method. To implement the Rydberg ionization spectroscopy we use a molecular beam based, time-resolved pump-probe multi-photon ionization/photoelectron scheme in which a first laser pulse excites the molecule to a Rydberg state, and a probe pulse ionizes the molecule. A time-of-flight detector measures the kinetic energy spectrum of the photoelectrons. The photoelectron spectrum directly provides the binding energy of the electron, and thereby reveals the molecule’s time-dependent structural fingerprint. Only the duration of the laser pulses limits the time resolution. With a new laser system, we have now reached time resolutions better than 100 fs, although very deep UV wavelengths (down to 190 nm) have slightly longer instrument functions. The structural dynamics of molecules in Rydberg-excited states is obtained by delaying the probe ionization photon from the pump photon; the structural dynamics of molecules in their ground state or excited valence states is measured by inducing the dynamics using a near UV laser pulse, and employing a multi-photon ionization scheme via the Rydberg states as a probe process. Thus, the technique is capable of measuring the reaction dynamics in any electronic state of neutral molecules.« less

Focal overlap gating in velocity map imaging to achieve high signal-to-noise ratio in photo-ion pump-probe experiments

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shivaram, Niranjan; Champenois, Elio G.; Cryan, James P.

We demonstrate a technique in velocity map imaging (VMI) that allows spatial gating of the laser focal overlap region in time resolved pump-probe experiments. This significantly enhances signal-to-noise ratio by eliminating background signal arising outside the region of spatial overlap of pump and probe beams. This enhancement is achieved by tilting the laser beams with respect to the surface of the VMI electrodes which creates a gradient in flight time for particles born at different points along the beam. By suitably pulsing our microchannel plate detector, we can select particles born only where the laser beams overlap. Furthermore, this spatialmore » gating in velocity map imaging can benefit nearly all photo-ion pump-probe VMI experiments especially when extreme-ultraviolet light or X-rays are involved which produce large background signals on their own.« less

Generation and Evolution of High-Mach-Number Laser-Driven Magnetized Collisionless Shocks in the Laboratory.

PubMed

Schaeffer, D B; Fox, W; Haberberger, D; Fiksel, G; Bhattacharjee, A; Barnak, D H; Hu, S X; Germaschewski, K

2017-07-14

We present the first laboratory generation of high-Mach-number magnetized collisionless shocks created through the interaction of an expanding laser-driven plasma with a magnetized ambient plasma. Time-resolved, two-dimensional imaging of plasma density and magnetic fields shows the formation and evolution of a supercritical shock propagating at magnetosonic Mach number M_{ms}≈12. Particle-in-cell simulations constrained by experimental data further detail the shock formation and separate dynamics of the multi-ion-species ambient plasma. The results show that the shocks form on time scales as fast as one gyroperiod, aided by the efficient coupling of energy, and the generation of a magnetic barrier between the piston and ambient ions. The development of this experimental platform complements present remote sensing and spacecraft observations, and opens the way for controlled laboratory investigations of high-Mach number collisionless shocks, including the mechanisms and efficiency of particle acceleration.

Transient, Small-Scale Field-Aligned Currents in the Plasma Sheet Boundary Layer During Storm Time Substorms

NASA Technical Reports Server (NTRS)

Nakamura, R.; Sergeev, V. A.; Baumjohann, W.; Plaschke, F.; Magnes, W.; Fischer, D.; Varsani, A.; Schmid, D.; Nakamura, T. K. M.; Russell, C. T.;

Communication: Electron ionization of DNA bases

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rahman, M. A.; Krishnakumar, E., E-mail: ekkumar@tifr.res.in

2016-04-28

No reliable experimental data exist for the partial and total electron ionization cross sections for DNA bases, which are very crucial for modeling radiation damage in genetic material of living cell. We have measured a complete set of absolute partial electron ionization cross sections up to 500 eV for DNA bases for the first time by using the relative flow technique. These partial cross sections are summed to obtain total ion cross sections for all the four bases and are compared with the existing theoretical calculations and the only set of measured absolute cross sections. Our measurements clearly resolve themore » existing discrepancy between the theoretical and experimental results, thereby providing for the first time reliable numbers for partial and total ion cross sections for these molecules. The results on fragmentation analysis of adenine supports the theory of its formation in space.« less

Transient, small-scale field-aligned currents in the plasma sheet boundary layer during storm time substorms.

PubMed

Nakamura, R; Sergeev, V A; Baumjohann, W; Plaschke, F; Magnes, W; Fischer, D; Varsani, A; Schmid, D; Nakamura, T K M; Russell, C T; Strangeway, R J; Leinweber, H K; Le, G; Bromund, K R; Pollock, C J; Giles, B L; Dorelli, J C; Gershman, D J; Paterson, W; Avanov, L A; Fuselier, S A; Genestreti, K; Burch, J L; Torbert, R B; Chutter, M; Argall, M R; Anderson, B J; Lindqvist, P-A; Marklund, G T; Khotyaintsev, Y V; Mauk, B H; Cohen, I J; Baker, D N; Jaynes, A N; Ergun, R E; Singer, H J; Slavin, J A; Kepko, E L; Moore, T E; Lavraud, B; Coffey, V; Saito, Y

2016-05-28

We report on field-aligned current observations by the four Magnetospheric Multiscale (MMS) spacecraft near the plasma sheet boundary layer (PSBL) during two major substorms on 23 June 2015. Small-scale field-aligned currents were found embedded in fluctuating PSBL flux tubes near the separatrix region. We resolve, for the first time, short-lived earthward (downward) intense field-aligned current sheets with thicknesses of a few tens of kilometers, which are well below the ion scale, on flux tubes moving equatorward/earthward during outward plasma sheet expansion. They coincide with upward field-aligned electron beams with energies of a few hundred eV. These electrons are most likely due to acceleration associated with a reconnection jet or high-energy ion beam-produced disturbances. The observations highlight coupling of multiscale processes in PSBL as a consequence of magnetotail reconnection.

Focal overlap gating in velocity map imaging to achieve high signal-to-noise ratio in photo-ion pump-probe experiments

DOE PAGES

Shivaram, Niranjan; Champenois, Elio G.; Cryan, James P.; ...

2016-12-19

We demonstrate a technique in velocity map imaging (VMI) that allows spatial gating of the laser focal overlap region in time resolved pump-probe experiments. This significantly enhances signal-to-noise ratio by eliminating background signal arising outside the region of spatial overlap of pump and probe beams. This enhancement is achieved by tilting the laser beams with respect to the surface of the VMI electrodes which creates a gradient in flight time for particles born at different points along the beam. By suitably pulsing our microchannel plate detector, we can select particles born only where the laser beams overlap. Furthermore, this spatialmore » gating in velocity map imaging can benefit nearly all photo-ion pump-probe VMI experiments especially when extreme-ultraviolet light or X-rays are involved which produce large background signals on their own.« less

Heavy ion beams from an Alphatross source for use in calibration and testing of diagnostics

NASA Astrophysics Data System (ADS)

Ward, R. J.; Brown, G. M.; Ho, D.; Stockler, B. F. O. F.; Freeman, C. G.; Padalino, S. J.; Regan, S. P.

2016-10-01

Ion beams from the 1.7 MV Pelletron Accelerator at SUNY Geneseo have been used to test and calibrate many inertial confinement fusion (ICF) diagnostics and high energy density physics (HEDP) diagnostics used at the Laboratory for Laser Energetics (LLE). The ion source on this accelerator, a radio-frequency (RF) alkali-metal charge exchange source called an Alphatross, is designed to produce beams of hydrogen and helium isotopes. There is interest in accelerating beams of carbon, oxygen, argon, and other heavy ions for use in testing several diagnostics, including the Time Resolved Tandem Faraday Cup (TRTF). The feasibility of generating these heavy ion beams using the Alphatross source will be reported. Small amounts of various gases are mixed into the helium plasma in the ion source bottle. A velocity selector is used to allow the desired ions to pass into the accelerator. As the heavy ions pass through the stripper canal of the accelerator, they emerge in a variety of charge states. The energy of the ion beam at the high-energy end of the accelerator will vary as a function of the charge state, however the maximum energy deliverable to target is limited by the maximum achievable magnetic field produced by the accelerator's steering magnet. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

Effect of magnetic field inhomogeneity on ion cyclotron motion coherence at high magnetic field.

PubMed

Vladimirov, Gleb; Kostyukevich, Yury; Hendrickson, Christopher L; Blakney, Greg T; Nikolaev, Eugene

2015-01-01

A three-dimensional code based on the particle-in-cell algorithm modified to account for the inhomogeneity of the magnetic field was applied to determine the effect of Z(1), Z(2), Z(3), Z(4), X, Y, ZX, ZY, XZ(2) YZ(2), XY and X(2)-Y(2) components of an orthogonal magnetic field expansion on ion motion during detection in an FT-ICR cell. Simulations were performed for magnetic field strengths of 4.7, 7, 14.5 and 21 Tesla, including experimentally determined magnetic field spatial distributions for existing 4.7 T and 14.5 T magnets. The effect of magnetic field inhomogeneity on ion cloud stabilization ("ion condensation") at high numbers of ions was investigated by direct simulations of individual ion trajectories. Z(1), Z(2), Z(3) and Z(4) components have the largest effect (especially Z(1)) on ion cloud stability. Higher magnetic field strength and lower m/z demand higher relative magnetic field homogeneity to maintain cloud coherence for a fixed time period. The dependence of mass resolving power upper limit on Z(1) inhomogeneity is evaluated for different magnetic fields and m/z. The results serve to set the homogeneity requirements for various orthogonal magnetic field components (shims) for future FT-ICR magnet design.

Shell- and subshell-resolved projectile excitation of hydrogenlike Au{sup 78+} ions in relativistic ion-atom collisions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gumberidze, A.; Frankfurt Institute for Advanced Studies FIAS, D-60438 Frankfurt am Main; Fritzsche, S.

2010-11-15

The projectile excitation of high-Z ions has been investigated in relativistic ion-atoms collisions by observing the subsequent x-ray emission. The x-ray spectra from the projectile excitation have been separated from the x-ray emission following electron capture into the excited states using a novel anticoincidence technique. For the particular case of hydrogenlike Au{sup 78+} ions colliding with Ar atoms, Coulomb excitation from the ground state into the fine-structure-resolved n=2 levels as well as into levels with principal quantum number n{>=}3 has been measured with excellent statistics. The observed spectra agree well with simulated spectra that are based on Dirac's relativistic equationmore » and the proper inclusion of the magnetic interaction into the amplitudes for projectile excitation. It is shown that a coherent inclusion of the magnetic part of the Lienard-Wiechert potential leads to the lowering of the excitation cross section by up to 35%. This effect is more pronounced for excitation into states with high angular momentum and is confirmed by our experimental data.« less

Highly Resolved Measurements of a Developing Strong Collisional Plasma Shock

NASA Astrophysics Data System (ADS)

Rinderknecht, Hans G.; Park, H.-S.; Ross, J. S.; Amendt, P. A.; Higginson, D. P.; Wilks, S. C.; Haberberger, D.; Katz, J.; Froula, D. H.; Hoffman, N. M.; Kagan, G.; Keenan, B. D.; Vold, E. L.

2018-03-01

The structure of a strong collisional shock front forming in a plasma is directly probed for the first time in laser-driven gas-jet experiments. Thomson scattering of a 526.5 nm probe beam was used to diagnose temperature and ion velocity distribution in a strong shock (M ˜11 ) propagating through a low-density (ρ ˜0.01 mg /cc ) plasma composed of hydrogen. A forward-streaming population of ions traveling in excess of the shock velocity was observed to heat and slow down on an unmoving, unshocked population of cold protons, until ultimately the populations merge and begin to thermalize. Instabilities are observed during the merging, indicating a uniquely plasma-phase process in shock front formation.

Enabling High Fidelity Measurements of Energy and Pitch Angle for Escaping Energetic Ions with a Fast Ion Loss Detector

NASA Astrophysics Data System (ADS)

Chaban, R.; Pace, D. C.; Marcy, G. R.; Taussig, D.

2016-10-01

Energetic ion losses must be minimized in burning plasmas to maintain fusion power, and existing tokamaks provide access to energetic ion parameter regimes that are relevant to burning machines. A new Fast Ion Loss Detector (FILD) probe on the DIII-D tokamak has been optimized to resolve beam ion losses across a range of 30 - 90 keV in energy and 40° to 80° in pitch angle, thereby providing valuable measurements during many different experiments. The FILD is a magnetic spectrometer; once inserted into the tokamak, the magnetic field allows energetic ions to pass through a collimating aperture and strike a scintillator plate that is imaged by a wide view camera and narrow view photomultiplier tubes (PMTs). The design involves calculating scintillator strike patterns while varying probe geometry. Calculated scintillator patterns are then used to design an optical system that allows adjustment of the focus regions for the 1 MS/s resolved PMTs. A synthetic diagnostic will be used to determine the energy and pitch angle resolution that can be attained in DIII-D experiments. Work supported in part by US DOE under the Science Undergraduate Laboratory Internship (SULI) program and under DE-FC02-04ER54698.

Ion Energy Distribution Studies of Ions and Radicals in an Ar/H2 Radio Frequency Magnetron Discharge During a-Si:H Deposition Using Energy-Resolved Mass Spectrometry

NASA Astrophysics Data System (ADS)

Mensah, Samuel; Abu-Safe, Husam; Naseem, Hameed; Gordon, Matt

2012-02-01

Ion energy distributions of sputtered Si particles have been measured by an energy-resolved mass spectrometer, and we correlate the results with measured thin film properties. The plasmas have been generated in a conventional magnetron chamber powered at 150W, 13.56MHz at hydrogen flow rates ranging from 0-25sccm. Various Hn^+, SiHn^+, SiHn fragments (with n = 1, 2, 3) together with Ar^+ and ArH^+ species were detected in the discharge. The most important species for the film deposition is SiHn with n = 0,1,2, and H fragments affect the hydrogen content in the material. The flux of Ar^+ decreases and that of ArH^+ increases when the hydrogen flow rate was increased. However both fluxes saturate at hydrogen flow rates above 15sccm. Plasma parameters, such as plasma potential Vp, electron density ne and electron energy Te, are measured with the Langmuir probe. The ion energy distribution (IED) of all prominent species in the plasma is measured with an energy resolved mass analyzer. The plasma parameters decreased with increasing hydrogen flow rate; Vp, ne and Te decreased from 36.5V, 7.2x10^15 m-3, 5.6eV to 32.8, 2.2x10^15m-3 and 3.8eV respectively. The ion energy of the heavy species, Ar, Ar^+, ArH, ArH^+, SiHn and SiHn^+ radicals have ion energies comparable to the plasma potential. Analysis of the IEDs shows an inter-dependence of the species and their contribution to the thin film growth and properties.

Exploring the dynamics of kinetic/multi-ion effects and ion-electron equilibration rates in ICF plasmas at OMEGA

NASA Astrophysics Data System (ADS)

Sio, H.

2017-10-01

During the last few years, an increasing number of experiments have shown that kinetic and multi-ion-fluid effects do impact the performance of an ICF implosion. Observations include: increasing yield degradation as the implosion becomes more kinetic; thermal decoupling between ion species; anomalous yield scaling for different fuel mixtures; ion diffusion; and fuel stratification. The common theme in these experiments is that the results are based on time-integrated nuclear observables that are affected by an accumulation of effects throughout the implosion, which complicate interpretation of the data. A natural extension of these studies is therefore to conduct time-resolved measurements of multiple nuclear-burn histories to explore the dynamics of kinetic/multi-ion effects in the fuel and their impact on the implosion performance. This was accomplished through simultaneous, high-precision measurements of the relative timing of the onset, bang time and duration of DD, D3He, DT and T3He burn from T3He (with trace D) or D3He gas-filled implosions using the new Particle X-ray Temporal Diagnostic (PXTD) on OMEGA. As the different reactions have different temperature sensitivities, Ti(t) was determined from the data. Uniquely to the PXTD, several x-ray emission histories (in different energy bands) were also measured, from which a spatially averaged Te(t) was also determined. The inferred Ti(t) and Te(t) data have been used to experimentally explore ion-electron equilibration rates and the Coulomb Logarithm for various plasma conditions. Finally, the implementation and use of PXTD, which represents a significant advance at OMEGA, have laid the foundation for implementing a Te(t) measurement in support of the main cryogenic DT programs at OMEGA and the NIF. This work was supported in part by the US DOE, LLE, LLNL, and DOE NNSA SSGF.

Signal and background considerations for the MRSt on the National Ignition Facility (NIF).

PubMed

Wink, C W; Frenje, J A; Hilsabeck, T J; Bionta, R; Khater, H Y; Gatu Johnson, M; Kilkenny, J D; Li, C K; Séguin, F H; Petrasso, R D

2016-11-01

A Magnetic Recoil Spectrometer (MRSt) has been conceptually designed for time-resolved measurements of the neutron spectrum at the National Ignition Facility. Using the MRSt, the goals are to measure the time-evolution of the spectrum with a time resolution of ∼20-ps and absolute accuracy better than 5%. To meet these goals, a detailed understanding and optimization of the signal and background characteristics are required. Through ion-optics, MCNP simulations, and detector-response calculations, it is demonstrated that the goals and a signal-to background >5-10 for the down-scattered neutron measurement are met if the background, consisting of ambient neutrons and gammas, at the MRSt is reduced 50-100 times.

Temporally and spatially resolved plasma spectroscopy in pulsed laser deposition of ultra-thin boron nitride films

DOE Office of Scientific and Technical Information (OSTI.GOV)

Glavin, Nicholas R., E-mail: nicholas.glavin.1@us.af.mil, E-mail: andrey.voevodin@us.af.mil; School of Mechanical Engineering and Birck Nanotechnology Center, Purdue University, West Lafayette, Indiana 47907; Muratore, Christopher

2015-04-28

Physical vapor deposition (PVD) has recently been investigated as a viable, alternative growth technique for two-dimensional materials with multiple benefits over other vapor deposition synthesis methods. The high kinetic energies and chemical reactivities of the condensing species formed from PVD processes can facilitate growth over large areas and at reduced substrate temperatures. In this study, chemistry, kinetic energies, time of flight data, and spatial distributions within a PVD plasma plume ablated from a boron nitride (BN) target by a KrF laser at different pressures of nitrogen gas were investigated. Time resolved spectroscopy and wavelength specific imaging were used to identifymore » and track atomic neutral and ionized species including B{sup +}, B*, N{sup +}, N*, and molecular species including N{sub 2}*, N{sub 2}{sup +}, and BN. Formation and decay of these species formed both from ablation of the target and from interactions with the background gas were investigated and provided insights into fundamental growth mechanisms of continuous, amorphous boron nitride thin films. The correlation of the plasma diagnostic results with film chemical composition and thickness uniformity studies helped to identify that a predominant mechanism for BN film formation is condensation surface recombination of boron ions and neutral atomic nitrogen species. These species arrive nearly simultaneously to the substrate location, and BN formation occurs microseconds before arrival of majority of N{sup +} ions generated by plume collisions with background molecular nitrogen. The energetic nature and extended dwelling time of incident N{sup +} ions at the substrate location was found to negatively impact resulting BN film stoichiometry and thickness. Growth of stoichiometric films was optimized at enriched concentrations of ionized boron and neutral atomic nitrogen in plasma near the condensation surface, providing few nanometer thick films with 1:1 BN stoichiometry and good thicknesses uniformity over macroscopic areas.« less

Top-down MALDI-in-source decay-FTICR mass spectrometry of isotopically resolved proteins.

PubMed

Nicolardi, Simone; Switzar, Linda; Deelder, André M; Palmblad, Magnus; van der Burgt, Yuri E M

2015-03-17

An accurate mass measurement of a known protein provides information on potential amino acid deletions and post-translational modifications. Although this field is dominated by strategies based on electrospray ionization, mass spectrometry (MS) methods using matrix-assisted laser desorption/ionization (MALDI) have the advantage of yielding predominantly singly charged precursor ions, thus avoiding peak overlap from different charge states of multiple species. Such MALDI-MS methods require mass measurement at ultrahigh resolution, which is provided by Fourier transform ion cyclotron resonance (FTICR) mass analyzers. Recently, using a MALDI-FTICR-MS platform equipped with a 15 T magnet, we reported on the mass analysis of intact human serum peptides and small proteins with isotopic resolution up to ∼15 kDa and identified new proteoforms from an accurate measurement of mass distances. In the current study, we have used this FTICR system after an upgrade with a novel dynamically harmonized ICR cell, i.e., ParaCell, for mapping isotopically resolved intact proteins up to about 17 kDa and performed top-down MALDI in-source decay (ISD) analysis. Standard proteins myoglobin (m/z-value 16,950) and ribonuclease B (m/z-value 14,900) were measured with resolving powers of 62,000 and 61,000, respectively. Furthermore, it will be shown that (singly charged) MALDI-ISD fragment ions can be measured at isotopic resolution up to m/z-value 12,000 (e.g., resolving power 39,000 at m/z-value 12,000) providing more reliable identifications. Moreover, examples are presented of pseudo-MS(3) experiments on ISD fragment ions from RNase B by collisional-induced dissociation (CID).

Spatially resolved chemical analysis of cicada wings using laser-ablation electrospray ionization (LAESI) imaging mass spectrometry (IMS).

PubMed

Román, Jessica K; Walsh, Callee M; Oh, Junho; Dana, Catherine E; Hong, Sungmin; Jo, Kyoo D; Alleyne, Marianne; Miljkovic, Nenad; Cropek, Donald M

2018-03-01

Laser-ablation electrospray ionization (LAESI) imaging mass spectrometry (IMS) is an emerging bioanalytical tool for direct imaging and analysis of biological tissues. Performing ionization in an ambient environment, this technique requires little sample preparation and no additional matrix, and can be performed on natural, uneven surfaces. When combined with optical microscopy, the investigation of biological samples by LAESI allows for spatially resolved compositional analysis. We demonstrate here the applicability of LAESI-IMS for the chemical analysis of thin, desiccated biological samples, specifically Neotibicen pruinosus cicada wings. Positive-ion LAESI-IMS accurate ion-map data was acquired from several wing cells and superimposed onto optical images allowing for compositional comparisons across areas of the wing. Various putative chemical identifications were made indicating the presence of hydrocarbons, lipids/esters, amines/amides, and sulfonated/phosphorylated compounds. With the spatial resolution capability, surprising chemical distribution patterns were observed across the cicada wing, which may assist in correlating trends in surface properties with chemical distribution. Observed ions were either (1) equally dispersed across the wing, (2) more concentrated closer to the body of the insect (proximal end), or (3) more concentrated toward the tip of the wing (distal end). These findings demonstrate LAESI-IMS as a tool for the acquisition of spatially resolved chemical information from fragile, dried insect wings. This LAESI-IMS technique has important implications for the study of functional biomaterials, where understanding the correlation between chemical composition, physical structure, and biological function is critical. Graphical abstract Positive-ion laser-ablation electrospray ionization mass spectrometry coupled with optical imaging provides a powerful tool for the spatially resolved chemical analysis of cicada wings.

Calibration of the OHREX high-resolution imaging crystal spectrometer at the Livermore electron beam ion traps [Calibration of the OHREX high-resolution imaging crystal spectrometer at the Livermore EBIT

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hell, N.; Beiersdorfer, P.; Magee, E. W.

2016-08-04

Here, we report the calibration of the Orion High-Resolution X-ray (OHREX) imaging crystal spectrometer at the EBIT-I electron beam ion trap at Livermore. Two such instruments, dubbed OHREX-1 and OHREX-2, are fielded for plasma diagnostics at the Orion laser facility in the United Kingdom. The OHREX spectrometer can simultaneously house two spherically bent crystals with a radius of curvature of r=67.2 cm. The focusing properties of the spectrometer allow both for larger distance to the source due to the increase in collected light and for observation of extended sources. OHREX is designed to cover a 2.5–3 degree spectral range atmore » Bragg angles around 51.3 degree. The typically high resolving powers at these large Bragg angles are ideally suited for line shape diagnostics. For instance, the nominal resolving power of the instrument (> 10000) is much higher than the effective resolving power associated with the Doppler broadening due to the temperature of the trapped ions in EBIT-I. The effective resolving power is only around 3000 at typical EBIT-I conditions, which nevertheless is sufficient to set up and test the instrument’s spectral characteristics. We have calibrated the spectral range for a number of crystals using well known reference lines in first and second order, and derived the ion temperatures from these lines. We have also made use of the 50µm size of the EBIT-I source width to characterize the spatial focusing of the spectrometer.« less

Development of a new corona discharge based ion source for high resolution time-of-flight chemical ionization mass spectrometer to measure gaseous H2SO4 and aerosol sulfate

NASA Astrophysics Data System (ADS)

Zheng, Jun; Yang, Dongsen; Ma, Yan; Chen, Mindong; Cheng, Jin; Li, Shizheng; Wang, Ming

2015-10-01

A new corona discharge (CD) based ion source was developed for a commercial high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS) (Aerodyne Research Inc.) to measure both gaseous sulfuric acid (H2SO4) and aerosol sulfate after thermal desorption. Nitrate core ions (NO3-) were used as reagent ions and were generated by a negative discharge in zero air followed by addition of excess nitrogen dioxide (NO2) to convert primary ions and hydroxyl radicals (OH) into NO3- ions and nitric acid (HNO3). The CD-HRToF-CIMS showed no detectable interference from hundreds parts per billion by volume (ppbv) of sulfur dioxide (SO2). Unlike the atmospheric pressure ionization (API) ToF-CIMS, the CD ion source was integrated onto the ion-molecule reaction (IMR) chamber and which made it possible to measure aerosol sulfate by coupling to a filter inlet for gases and aerosols (FIGAERO). Moreover, compared with a quadrupole-based mass spectrometer, the desired HSO4- signal was detected by its exact mass of m/z 96.960, which was well resolved from the potential interferences of HCO3-ṡ(H2O)2 (m/z 97.014) and O-ṡH2OṡHNO3 (m/z 97.002). In this work, using laboratory-generated standards the CD-HRToF-CIMS was demonstrated to be able to detect as low as 3.1 × 105 molecules cm-3 gaseous H2SO4 and 0.5 μg m-3 ammonium sulfate based on 10-s integration time and two times of the baseline noise. The CD ion source had the advantages of low cost and a simple but robust structure. Since the system was non-radioactive and did not require corrosive HNO3 gas, it can be readily field deployed. The CD-HRToF-CIMS can be a powerful tool for both field and laboratory studies of aerosol formation mechanism and the chemical processes that were critical to understand the evolution of aerosols in the atmosphere.

Growth and optical characteristics of Tm-doped AlGaN layer grown by organometallic vapor phase epitaxy

NASA Astrophysics Data System (ADS)

Takatsu, J.; Fuji, R.; Tatebayashi, J.; Timmerman, D.; Lesage, A.; Gregorkiewicz, T.; Fujiwara, Y.

2018-04-01

We report on the growth and optical properties of Tm-doped AlGaN layers by organometallic vapor phase epitaxy (OMVPE). The morphological and optical properties of Tm-doped GaN (GaN:Tm) and Tm-doped AlGaN (AlGaN:Tm) were investigated by Nomarski differential interference contrast microscopy and photoluminescence (PL) characterization. Nomarski images reveal an increase of surface roughness upon doping Tm into both GaN and AlGaN layers. The PL characterization of GaN:Tm shows emission in the near-infrared range originating from intra-4f shell transitions of Tm3+ ions. In contrast, AlGaN:Tm also exhibits blue light emission from Tm3+ ions. In that case, the wider band gap of the AlGaN host allows energy transfer to higher states of the Tm3+ ions. With time-resolved PL measurements, we could distinguish three types of luminescent sites of Tm3+ in the AlGaN:Tm layer, having different decay times. Our results confirm that Tm ions can be doped into GaN and AlGaN by OMVPE, and show potential for the fabrication of novel high-color-purity blue light emitting diodes.

4D offline PET-based treatment verification in scanned ion beam therapy: a phantom study

NASA Astrophysics Data System (ADS)

Kurz, Christopher; Bauer, Julia; Unholtz, Daniel; Richter, Daniel; Stützer, Kristin; Bert, Christoph; Parodi, Katia

2015-08-01

At the Heidelberg Ion-Beam Therapy Center, patient irradiation with scanned proton and carbon ion beams is verified by offline positron emission tomography (PET) imaging: the {β+} -activity measured within the patient is compared to a prediction calculated on the basis of the treatment planning data in order to identify potential delivery errors. Currently, this monitoring technique is limited to the treatment of static target structures. However, intra-fractional organ motion imposes considerable additional challenges to scanned ion beam radiotherapy. In this work, the feasibility and potential of time-resolved (4D) offline PET-based treatment verification with a commercial full-ring PET/CT (x-ray computed tomography) device are investigated for the first time, based on an experimental campaign with moving phantoms. Motion was monitored during the gated beam delivery as well as the subsequent PET acquisition and was taken into account in the corresponding 4D Monte-Carlo simulations and data evaluation. Under the given experimental conditions, millimeter agreement between the prediction and measurement was found. Dosimetric consequences due to the phantom motion could be reliably identified. The agreement between PET measurement and prediction in the presence of motion was found to be similar as in static reference measurements, thus demonstrating the potential of 4D PET-based treatment verification for future clinical applications.

Investigating ion channel conformational changes using voltage clamp fluorometry.

PubMed

Talwar, Sahil; Lynch, Joseph W

2015-11-01

Ion channels are membrane proteins whose functions are governed by conformational changes. The widespread distribution of ion channels, coupled with their involvement in most physiological and pathological processes and their importance as therapeutic targets, renders the elucidation of these conformational mechanisms highly compelling from a drug discovery perspective. Thanks to recent advances in structural biology techniques, we now have high-resolution static molecular structures for members of the major ion channel families. However, major questions remain to be resolved about the conformational states that ion channels adopt during activation, drug modulation and desensitization. Patch-clamp electrophysiology has long been used to define ion channel conformational states based on functional criteria. It achieves this by monitoring conformational changes at the channel gate and cannot detect conformational changes occurring in regions distant from the gate. Voltage clamp fluorometry involves labelling cysteines introduced into domains of interest with environmentally sensitive fluorophores and inferring structural rearrangements from voltage or ligand-induced fluorescence changes. Ion channel currents are monitored simultaneously to verify the conformational status. By defining real time conformational changes in domains distant from the gate, this technique provides unexpected new insights into ion channel structure and function. This review aims to summarise the methodology and highlight recent innovative applications of this powerful technique. This article is part of the Special Issue entitled 'Fluorescent Tools in Neuropharmacology'. Copyright © 2015 Elsevier Ltd. All rights reserved.

Optimum Waveforms for Differential Ion Mobility Spectrometry (FAIMS)

PubMed Central

Shvartsburg, Alexandre A.; Smith, Richard D.

2009-01-01

Differential mobility spectrometry or field asymmetric waveform ion mobility spectrometry (FAIMS) is a new tool for separation and identification of gas-phase ions, particularly in conjunction with mass-spectrometry. In FAIMS, ions are filtered by the difference between mobilities in gases (K) at high and low electric field intensity (E) using asymmetric waveforms. An infinite number of possible waveform profiles make maximizing the performance within engineering constraints a major issue for FAIMS technology refinement. Earlier optimizations assumed the non-constant component of mobility to scale as E2, producing the same result for all ions. Here we show that the optimum profiles are defined by the full series expansion of K(E) that includes terms beyond the 1st that is proportional to E2. For many ion/gas pairs, the first two terms have different signs, and the optimum profiles at sufficiently high E in FAIMS may differ substantially from those previously reported, improving the resolving power by up to 2.2 times. This situation arises for some ions in all FAIMS systems, but becomes more common in recent miniaturized devices that employ higher E. With realistic K(E) dependences, the maximum waveform amplitude is not necessarily optimum and reducing it by up to ∼20 – 30% is beneficial in some cases. The present findings are particularly relevant to targeted analyses where separation depends on the difference between K(E) functions for specific ions. PMID:18585054

Thomson-Scattering Study of the Subharmonic Decay of Ion-Acoustic Waves Driven by the Brillouin Instability

NASA Astrophysics Data System (ADS)

Bandulet, H. C.; Labaune, C.; Lewis, K.; Depierreux, S.

2004-07-01

Thomson scattering (TS) has been used to investigate the two-ion decay instability of ion acoustic waves generated by stimulated Brillouin scattering in an underdense CH plasma. Two complementary TS diagnostics, spectrally and spatially resolved, demonstrate the occurrence of the subharmonic decay of the primary ion acoustic wave into two secondary waves. The study of the laser intensity dependence shows that the secondary ion acoustic waves are correlated with the SBS reflectivity saturation, at a level of a few percent.

Terminal Forecast Reference Notebook (TFRN) for George AFB, California.

DTIC Science & Technology

1980-09-04

Sierrai Ne-vadal ranEgo to thle northi. Seventy mi les west-northwest Is Tehachapi Pass (ci cv. 3,800’ MSI.) * lie gnteWay Loii t lo I.wer San Joia ~qin... designed to provide aIgencieos soift icient time. to accomplish protect ive mteasures. Under Phasie 1, non-destructive weather condit ions (scich as...orge AFB. Action Taken to Resolve Problem: a. Trljectory htlletIn Information Is being plott.I for po;sible storm signatures as des - cribed on page 36

Observation of Interspecies Ion Separation in Inertial-Confinement-Fusion Implosions via Imaging X-ray spectroscopy

NASA Astrophysics Data System (ADS)

Joshi, Tirtha Raj

2016-10-01

Interspecies ion separation has been proposed as a yield-degradation mechanism in inertial-confinement-fusion (ICF) experiments. We present direct experimental evidence of interspecies ion separation in direct-drive ICF experiments performed at the OMEGA laser facility. These experiments were designed based on the fact that interspecies ion thermo-diffusion would be strongest for species with large mass and charge difference. The targets were spherical plastic shells filled with D2 and Ar (1% by atom). Ar K-shell spectral features were observed primarily between the time of first-shock convergence and slightly before neutron bang time, using a time- and space-integrated spectrometer, streaked crystal spectrometer, and two gated multi-monochromatic X-ray imagers fielded along quasi-orthogonal lines-of-sight. Detailed spectroscopic analyses of spatially resolved Ar K-shell lines reveal deviation from the initial 1%-Ar gas fill and show both Ar-concentration enhancement and depletion at different times and radial positions of the implosion. The experimental results are interpreted with radiation-hydrodynamic simulations that include recently implemented, first-principles models of interspecies ion diffusion. The experimentally inferred Ar-atom-fraction profiles agree gently with calculated profiles associated with the incoming and rebounding first shock. This work was done in collaboration with P. Hakel, S. C. Hsu, E. L. Vold, M. J. Schmitt, N. M. Hoffman, R. M. Rauenzahn, G. Kagan, X.-Z. Tang, Y. Kim, and H. W. Herrmann of LANL, and R. C. Mancini of UNR. LA-UR-16-24804. Supported by the LANL ICF and ASC Programs under US-DoE contract no. DE-AC52-06NA25396.

Effects of a static inhomogeneous magnetic field acting on a laser-produced carbon plasma plume

NASA Astrophysics Data System (ADS)

Favre, M.; Ruiz, H. M.; Bendixsen, L. S. Caballero; Reyes, S.; Veloso, F.; Wyndham, E.; Bhuyan, H.

2017-08-01

We present time- and space-resolved observations of the dynamics of a laser-produced carbon plasma, propagating in a sub-Tesla inhomogeneous magnetic field, with both, axial and radial field gradients. An Nd:YAG laser pulse, 340 mJ, 3.5 ns, at 1.06 μ m, with a fluence of 7 J/cm2, is used to generate the plasma from a solid graphite target, in vacuum. The magnetic field is produced using two coaxial sets of two NeFeB ring magnets, parallel to the laser target surface. The diagnostics include plasma imaging with 50 ns time resolution, spatially resolved optical emission spectroscopy and Faraday cup. Based on our observations, evidence of radial and axial plasma confinement due to magnetic field gradients is presented. Formation of C2 molecules, previously observed in the presence of a low pressure neutral gas background, and enhanced on-axis ion flux, are ascribed to finite Larmor radius effects and reduced radial transport due to the presence of the magnetic field.

Advance in multi-hit detection and quantization in atom probe tomography.

PubMed

Da Costa, G; Wang, H; Duguay, S; Bostel, A; Blavette, D; Deconihout, B

2012-12-01

The preferential retention of high evaporation field chemical species at the sample surface in atom-probe tomography (e.g., boron in silicon or in metallic alloys) leads to correlated field evaporation and pronounced pile-up effects on the detector. The latter severely affects the reliability of concentration measurements of current 3D atom probes leading to an under-estimation of the concentrations of the high-field species. The multi-hit capabilities of the position-sensitive time-resolved detector is shown to play a key role. An innovative method based on Fourier space signal processing of signals supplied by an advance delay-line position-sensitive detector is shown to drastically improve the time resolving power of the detector and consequently its capability to detect multiple events. Results show that up to 30 ions on the same evaporation pulse can be detected and properly positioned. The major impact of this new method on the quantization of chemical composition in materials, particularly in highly-doped Si(B) samples is highlighted.

Using gas chromatography with ion mobility spectrometry to resolve explosive compounds in the presence of interferents.

PubMed

Cook, Greg W; LaPuma, Peter T; Hook, Gary L; Eckenrode, Brian A

2010-11-01

Ion mobility spectrometry (IMS) is a valued field detection technology because of its speed and high sensitivity, but IMS cannot easily resolve analytes of interest within mixtures. Coupling gas chromatography (GC) to IMS adds a separation capability to resolve complex matrices. A GC-IONSCAN® operated in IMS and GC⁄ IMS modes was evaluated with combinations of five explosives and four interferents. In 100 explosive/interferent combinations, IMS yielded 21 false positives while GC⁄ IMS substantially reduced the occurrence of false positives to one. In addition, the results indicate that through redesign or modification of the preconcentrator there would be significant advantages to using GC⁄ IMS, such as enhancement of the linear dynamic range (LDR) in some situations. By balancing sensitivity with LDR, GC⁄ IMS could prove to be a very advantageous tool when addressing real world complex mixture situations.

Improved ion optics for introduction of ions into a 9.4-T Fourier transform ion cyclotron resonance mass spectrometer

DOE PAGES

Chen, Yu; Leach, Franklin E.; Kaiser, Nathan K.; ...

2015-01-19

Fourier transform ion cyclotron resonance (FT-ICR) mass spectrometry provides unparalleled mass accuracy and resolving power.[1],[2] With electrospray ionization (ESI), ions are typically transferred into the mass spectrometer through a skimmer, which serves as a conductance-limiting orifice. However, the skimmer allows only a small fraction of incoming ions to enter the mass spectrometer. An ion funnel, originally developed by Smith and coworkers at Pacific Northwest National Laboratory (PNNL)[3-5] provides much more efficient ion focusing and transfer. The large entrance aperture of the ion funnel allows almost all ions emanating from a heated capillary to be efficiently captured and transferred, resulting inmore » nearly lossless transmission.« less

A Spatially Resolving X-ray Crystal Spectrometer for Measurement of Ion-temperature and Rotation-velocity Profiles on the AlcatorC-Mod Tokamak

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hill, K. W.; Bitter, M. L.; Scott, S. D.

2009-03-24

A new spatially resolving x-ray crystal spectrometer capable of measuring continuous spatial profiles of high resolution spectra (λ/dλ > 6000) of He-like and H-like Ar Kα lines with good spatial (~1 cm) and temporal (~10 ms) resolutions has been installed on the Alcator C-Mod tokamak. Two spherically bent crystals image the spectra onto four two-dimensional Pilatus II pixel detectors. Tomographic inversion enables inference of local line emissivity, ion temperature (Ti), and toroidal plasma rotation velocity (vφ) from the line Doppler widths and shifts. The data analysis techniqu

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging.

PubMed

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui; Savelyev, Evgeny; Obaid, Razib; Kaderiya, Balram; Augustin, Sven; Schnorr, Kirsten; Dumitriu, Ileana; Osipov, Timur; Bilodeau, René; Kilcoyne, David; Kumarappan, Vinod; Rudenko, Artem; Berrah, Nora; Rolles, Daniel

2016-12-02

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C 2 H 2 Br 2 ). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. The experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model.

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

PubMed Central

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui; Savelyev, Evgeny; Obaid, Razib; Kaderiya, Balram; Augustin, Sven; Schnorr, Kirsten; Dumitriu, Ileana; Osipov, Timur; Bilodeau, René; Kilcoyne, David; Kumarappan, Vinod; Rudenko, Artem; Berrah, Nora; Rolles, Daniel

2016-01-01

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C2H2Br2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. The experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model. PMID:27910943

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C 2H 2Br 2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. Lastly, the experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model.

Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging

DOE PAGES

Ablikim, Utuq; Bomme, Cédric; Xiong, Hui; ...

2016-12-02

An experimental route to identify and separate geometric isomers by means of coincident Coulomb explosion imaging is presented, allowing isomer-resolved photoionization studies on isomerically mixed samples. We demonstrate the technique on cis/trans 1,2-dibromoethene (C 2H 2Br 2). The momentum correlation between the bromine ions in a three-body fragmentation process induced by bromine 3d inner-shell photoionization is used to identify the cis and trans structures of the isomers. Lastly, the experimentally determined momentum correlations and the isomer-resolved fragment-ion kinetic energies are matched closely by a classical Coulomb explosion model.

A dual-ion imprinted polymer embedded in sol-gel matrix for the ultra trace simultaneous analysis of cadmium and copper.

PubMed

Bali Prasad, Bhim; Jauhari, Darshika; Verma, Archana

2014-03-01

In simultaneous determination of group of elements, there are inter-metallic interactions which result in a non-linear relationship between the peak current and ionic concentration for each of the element, at bare (unmodified) electrode. To resolve this problem, we have resorted, for the first time, to develop a modified pencil graphite electrode using a typical ion imprinted polymer network (dual-ion imprinted polymer embedded in sol-gel matrix (inorganic-organic hybrid nano-material)) for the simultaneous analysis of a binary mixture of Cd(II) and Cu(II) ions, without any complication of inter-metallic interactions and competitive bindings, in real samples. The adequate resolution of differential pulse anodic stripping voltammetry peaks by 725 mV (cf, 615 mV with unmodified electrode), without any cross-reactivity and the stringent detection limits as low as, 0.050 and 0.034 ng mL(-1) (S/N=3) for Cd(II) and Cu(II) ions, respectively by the proposed sensor can be considered useful for the primitive diagnosis of several chronic diseases in clinical settings. Copyright © 2013 Elsevier B.V. All rights reserved.

Ultrafast entanglement of trapped ions

NASA Astrophysics Data System (ADS)

Neyenhuis, Brian; Johnson, Kale; Mizrahi, Jonathan; Wong-Campos, David; Monroe, Christopher

2014-05-01

We have demonstrated ultrafast spin-motion entanglement of a single atomic ion using a short train of intense laser pulses. This pulse train gives the ion a spin-dependent kick where each spin state receives a discrete momentum kick in opposite directions. Using a series of these spin-dependent kicks we can realize a two qubit gate. In contrast to gates using spectroscopically resolved motional sidebands, these gates may be performed faster than the trap oscillation period, making them potentially less sensitive to noise. Additionally this gate is temperature insensitive and does not require the ions to be cooled to the Lamb-Dicke limit. We show that multiple kicks can be strung together to create a ``Schrodinger cat'' like state, where the large separation between the two parts of the wavepacket allow us to accumulate the phase shift necessary for a gate in a shorter amount of time. We will present a realistic pulse scheme for a two ion gate, and our progress towards its realization. This work is supported by grants from the U.S. Army Research Office with funding from the DARPA OLE program, IARPA, and the MURI program; and the NSF Physics Frontier Center at JQI.

Static harmonization of dynamically harmonized Fourier transform ion cyclotron resonance cell.

PubMed

Zhdanova, Ekaterina; Kostyukevich, Yury; Nikolaev, Eugene

2017-08-01

Static harmonization in the Fourier transform ion cyclotron resonance cell improves the resolving power of the cell and prevents dephasing of the ion cloud in the case of any trajectory of the charged particle, not necessarily axisymmetric cyclotron (as opposed to dynamic harmonization). We reveal that the Fourier transform ion cyclotron resonance cell with dynamic harmonization (paracell) is proved to be statically harmonized. The volume of the statically harmonized potential distribution increases with an increase in the number of trap segments.

Photodissociation spectroscopy of the dysprosium monochloride molecular ion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dunning, Alexander, E-mail: alexander.dunning@gmail.com; Schowalter, Steven J.; Puri, Prateek

2015-09-28

We have performed a combined experimental and theoretical study of the photodissociation cross section of the molecular ion DyCl{sup +}. The photodissociation cross section for the photon energy range 35 500 cm{sup −1} to 47 500 cm{sup −1} is measured using an integrated ion trap and time-of-flight mass spectrometer; we observe a broad, asymmetric profile that is peaked near 43 000 cm{sup −1}. The theoretical cross section is determined from electronic potentials and transition dipole moments calculated using the relativistic configuration-interaction valence-bond and coupled-cluster methods. The electronic structure of DyCl{sup +} is extremely complex due to the presence of multiple open electronic shells,more » including the 4f{sup 10} configuration. The molecule has nine attractive potentials with ionically bonded electrons and 99 repulsive potentials dissociating to a ground state Dy{sup +} ion and Cl atom. We explain the lack of symmetry in the cross section as due to multiple contributions from one-electron-dominated transitions between the vibrational ground state and several resolved repulsive excited states.« less

Thick electrodes for Li-ion batteries: A model based analysis

NASA Astrophysics Data System (ADS)

Danner, Timo; Singh, Madhav; Hein, Simon; Kaiser, Jörg; Hahn, Horst; Latz, Arnulf

2016-12-01

Li-ion batteries are commonly used in portable electronic devices due to their outstanding energy and power density. A remaining issue which hinders the breakthrough e.g. in the automotive sector is the high production cost. For low power applications, such as stationary storage, batteries with electrodes thicker than 300 μm were suggested. High energy densities can be attained with only a few electrode layers which reduces production time and cost. However, mass and charge transport limitations can be severe at already small C-rates due to long transport pathways. In this article we use a detailed 3D micro-structure resolved model to investigate limiting factors for battery performance. The model is parametrized with data from the literature and dedicated experiments and shows good qualitative agreement with experimental discharge curves of thick NMC-graphite Li-ion batteries. The model is used to assess the effect of inhomogeneities in carbon black distribution and gives answers to the possible occurrence of lithium plating during battery charge. Based on our simulations we can predict optimal operation strategies and improved design concepts for future Li-ion batteries employing thick electrodes.

Investigation of electronically excited indole relaxation dynamics via photoionization and fragmentation pump-probe spectroscopy.

PubMed

Godfrey, T J; Yu, Hui; Ullrich, Susanne

2014-07-28

The studies herein investigate the involvement of the low-lying (1)La and (1)Lb states with (1)ππ(*) character and the (1)πσ(*) state in the deactivation process of indole following photoexcitation at 201 nm. Three gas-phase, pump-probe spectroscopic techniques are employed: (1) Time-resolved photoelectron spectroscopy (TR-PES), (2) hydrogen atom (H-atom) time-resolved kinetic energy release (TR-KER), and (3) time-resolved ion yield (TR-IY). Each technique provides complementary information specific to the photophysical processes in the indole molecule. In conjunction, a thorough examination of the electronically excited states in the relaxation process, with particular focus on the involvement of the (1)πσ(*) state, is afforded. Through an extensive analysis of the TR-PES data presented here, it is deduced that the initial excitation of the (1)Bb state decays to the (1)La state on a timescale beyond the resolution of the current experimental setup. Relaxation proceeds on the (1)La state with an ultrafast decay constant (<100 femtoseconds (fs)) to the lower-lying (1)Lb state, which is found to possess a relatively long lifetime of 23 ± 5 picoseconds (ps) before regressing to the ground state. These studies also manifest an additional component with a relaxation time of 405 ± 76 fs, which is correlated with activity along the (1)πσ(*) state. TR-KER and TR-IY experiments, both specifically probing (1)πσ(*) dynamics, exhibit similar decay constants, further validating these observations.

Femtosecond Beam Sources and Applications

DOE Office of Scientific and Technical Information (OSTI.GOV)

Uesaka, Mitsuru

2004-12-07

Short particle beam science has been promoted by electron linac and radiation chemistry up to picoseconds. Recently, table-top TW laser enables several kinds of short particle beams and pump-and-probe analyses. 4th generation SR sources aim to generation and application of about 100 fs X-ray. Thus, femtosecond beam science has become one of the important field in advanced accelerator concepts. By using electron linac with photoinjector, about 200 fs single bunch and 3 fs multi-bunches are available. Tens femtoseconds monoenergetic electron bunch is expected by laser plasma cathode. Concerning the electron bunch diagnosis, we have seen remarkable progress in streak camera,more » coherent radiation spectroscopy, fluctuation method and E/O crystal method. Picosecond time-resolved pump-and-probe analysis by synchronizing electron linac and laser is now possible, but the timing jitter and drift due to several fluctuations in electronic devices and environment are still in picoseconds. On the other hand, the synchronization between laser and secondary beam is done passively by an optical beam-splitter in the system based on one TW laser. Therefore, the timing jitter and drift do not intrinsically exist there. The author believes that the femtosecond time-resolved pump-and-probe analysis must be initiated by the laser plasma beam sources. As to the applications, picosecond time-resolved system by electron photoinjector/linac and femtosecond laser are operating in more than 5 facilities for radiation chemistry in the world. Ti:Sapphire-laser-based repetitive pump-and-probe analysis started by time-resolved X-ray diffraction to visualize the atomic motion. Nd:Glass-laser-based single-shot analysis was performed to visualize the laser ablation via the single-shot ion imaging. The author expects that protein dynamics and ultrafast nuclear physics would be the next interesting targets. Monograph titled 'Femtosecond Beam Science' is published by Imperial College Press/World Scientific in 2004.« less

Comprehensive and accurate tracking of carbon origin of LC-tandem mass spectrometry collisional fragments for 13C-MFA.

PubMed

Kappelmann, Jannick; Klein, Bianca; Geilenkirchen, Petra; Noack, Stephan

2017-03-01

In recent years the benefit of measuring positionally resolved 13 C-labeling enrichment from tandem mass spectrometry (MS/MS) collisional fragments for improved precision of 13 C-Metabolic Flux Analysis ( 13 C-MFA) has become evident. However, the usage of positional labeling information for 13 C-MFA faces two challenges: (1) The mass spectrometric acquisition of a large number of potentially interfering mass transitions may hamper accuracy and sensitivity. (2) The positional identity of carbon atoms of product ions needs to be known. The present contribution addresses the latter challenge by deducing the maximal positional labeling information contained in LC-ESI-MS/MS spectra of product anions of central metabolism as well as product cations of amino acids. For this purpose, we draw on accurate mass spectrometry, selectively labeled standards, and published fragmentation pathways to structurally annotate all dominant mass peaks of a large collection of metabolites, some of which with a complete fragmentation pathway. Compiling all available information, we arrive at the most detailed map of carbon atom fate of LC-ESI-MS/MS collisional fragments yet, comprising 170 intense and structurally annotated product ions with unique carbon origin from 76 precursor ions of 72 metabolites. Our 13 C-data proof that heuristic fragmentation rules often fail to yield correct fragment structures and we expose common pitfalls in the structural annotation of product ions. We show that the positionally resolved 13 C-label information contained in the product ions that we structurally annotated allows to infer the entire isotopomer distribution of several central metabolism intermediates, which is experimentally demonstrated for malate using quadrupole-time-of-flight MS technology. Finally, the inclusion of the label information from a subset of these fragments improves flux precision in a Corynebacterium glutamicum model of the central carbon metabolism.

A Survey of Cassini CAPS Ion Observations During Titan Flybys TA-T83

NASA Astrophysics Data System (ADS)

Woodson, A. K.; Johnson, R. E.; Smith, H. T.; Crary, F. J.

2015-12-01

The Cassini Plasma Spectrometer (CAPS) sampled Titan's plasma environment during each of 83 encounters with the moon between orbit insertion on June 30, 2004 and June 1, 2012. The CAPS Ion Mass Spectrometer (IMS) acquired energy- and mass-per-charge-discriminated time-of-flight (TOF) spectra associated with ionospheric H+, H2+, H3+, CHx+, and C2Hx+ during at least 68 of those encounters. Herein we discuss ion energy distributions extracted from these spectra, each accumulated over an ~4 minute interval along the spacecraft trajectory. This is accomplished by fitting calibration peak models to TOF spectra in order to determine the TOF range associated with each aforementioned ion group, and then summing counts over each TOF range to obtain well-resolved energy peaks for each group. Energy distributions are determined by fitting the logistic power peak function to each of the resulting energy spectra. We then plot the resulting distribution parameters (peak energy, peak amplitude, and peak width or temperature) for each species and each encounter against Titan latitude, longitude, and altitude to generate a map of ion parameters. In addition, the encounters are grouped according to ambient plasma and magnetic field measurements in order to characterize the ion distribution parameters in different regions of Saturn's magnetosphere.

Simulations as a tool for higher mass resolution spectrometer: Lessons from existing observations

NASA Astrophysics Data System (ADS)

Nicolaou, Georgios; Yamauchi, Masatoshi; Nilsson, Hans; Wieser, Martin; Fedorov, Andrei

2017-04-01

Scientific requirements of each mission are crucial for the instrument's design. Ion tracing simulations of instruments can be helpful to characterize their performance, identify their limitations and improving the design for future missions. However, simulations provide the best performance in ideal case, and the actual response is determined by many other factors. Therefore, simulations should be compared with observations when possible. Characterizing the actual response of a running instrument gives valuable lessons for the future design of test instruments with the same detection principle before spending resources to build and calibrate them. In this study we use an ion tracing simulation of the Ion Composition Analyser (ICA) on board ROSETTA, in order to characterize its response and to compare it with the observations. It turned out that, due to the complicated unexpected response of the running instrument, the heavy cometary ions and molecules are sometimes difficult to be resolved. However, preliminary simulation of a slightly modified design predicts much higher mass resolution. Even after considering the complicated unexpected response, we safely expect that the modified design can resolve most abundant heavy atomic ions (e.g., O^+) and molecular ions (e.g., N_2+ and O_2^+). We show the simulation results for both designs and ICA data.

The spatial-temporal ambiguity in auroral modeling

NASA Technical Reports Server (NTRS)

Rees, M. H.; Roble, R. G.; Kopp, J.; Abreu, V. J.; Rusch, D. W.; Brace, L. H.; Brinton, H. C.; Hoffman, R. A.; Heelis, R. A.; Kayser, D. C.

1980-01-01

The paper examines the time-dependent models of the aurora which show that various ionospheric parameters respond to the onset of auroral ionization with different time histories. A pass of the Atmosphere Explorer C satellite over Poker Flat, Alaska, and ground based photometric and photographic observations have been used to resolve the time-space ambiguity of a specific auroral event. The density of the O(+), NO(+), O2(+), and N2(+) ions, the electron density, and the electron temperature observed at 280 km altitude in a 50 km wide segment of an auroral arc are predicted by the model if particle precipitation into the region commenced about 11 min prior to the overpass.

Advanced analytical electron microscopy for alkali-ion batteries

DOE PAGES

Qian, Danna; Ma, Cheng; Meng, Ying Shirley; ...

2015-06-26

Lithium-ion batteries are a leading candidate for electric vehicle and smart grid applications. However, further optimizations of the energy/power density, coulombic efficiency and cycle life are still needed, and this requires a thorough understanding of the dynamic evolution of each component and their synergistic behaviors during battery operation. With the capability of resolving the structure and chemistry at an atomic resolution, advanced analytical transmission electron microscopy (AEM) is an ideal technique for this task. The present review paper focuses on recent contributions of this important technique to the fundamental understanding of the electrochemical processes of battery materials. A detailed reviewmore » of both static (ex situ) and real-time (in situ) studies will be given, and issues that still need to be addressed will be discussed.« less

Highly Resolved Measurements of a Developing Strong Collisional Plasma Shock

DOE PAGES

Rinderknecht, Hans G.; Park, H. -S.; Ross, J. S.; ...

2018-03-02

In this paper, the structure of a strong collisional shock front forming in a plasma is directly probed for the first time in laser-driven gas-jet experiments. Thomson scattering of a 526.5 nm probe beam was used to diagnose temperature and ion velocity distribution in a strong shock (more » $$M{\\sim}11$$) propagating through a low-density ($${\\rho}{\\sim}0.01\\text{ }\\text{ }\\mathrm{mg}/\\mathrm{cc}$$) plasma composed of hydrogen. A forward-streaming population of ions traveling in excess of the shock velocity was observed to heat and slow down on an unmoving, unshocked population of cold protons, until ultimately the populations merge and begin to thermalize. Finally, instabilities are observed during the merging, indicating a uniquely plasma-phase process in shock front formation.« less

Highly Resolved Measurements of a Developing Strong Collisional Plasma Shock

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rinderknecht, Hans G.; Park, H. -S.; Ross, J. S.

In this paper, the structure of a strong collisional shock front forming in a plasma is directly probed for the first time in laser-driven gas-jet experiments. Thomson scattering of a 526.5 nm probe beam was used to diagnose temperature and ion velocity distribution in a strong shock (more » $$M{\\sim}11$$) propagating through a low-density ($${\\rho}{\\sim}0.01\\text{ }\\text{ }\\mathrm{mg}/\\mathrm{cc}$$) plasma composed of hydrogen. A forward-streaming population of ions traveling in excess of the shock velocity was observed to heat and slow down on an unmoving, unshocked population of cold protons, until ultimately the populations merge and begin to thermalize. Finally, instabilities are observed during the merging, indicating a uniquely plasma-phase process in shock front formation.« less

Cassini Ion Mass Spectrometer Peak Calibrations from Statistical Analysis of Flight Data

NASA Astrophysics Data System (ADS)

Woodson, A. K.; Johnson, R. E.

2017-12-01

The Cassini Ion Mass Spectrometer (IMS) is an actuating time-of-flight (TOF) instrument capable of resolving ion mass, energy, and trajectory over a field of view that captures nearly the entire sky. One of three instruments composing the Cassini Plasma Spectrometer, IMS sampled plasma throughout the Kronian magnetosphere from 2004 through 2012 when it was permanently disabled due to an electrical malfunction. Initial calibration of the flight instrument at Southwest Research Institute (SwRI) was limited to a handful of ions and energies due to time constraints, with only about 30% of planned measurements carried out prior to launch. Further calibration measurements were subsequently carried out after launch at SwRI and Goddard Space Flight Center using the instrument prototype and engineering model, respectively. However, logistical differences among the three calibration efforts raise doubts as to how accurately the post-launch calibrations describe the behavior of the flight instrument. Indeed, derived peak parameters for some ion species differ significantly from one calibration to the next. In this study we instead perform a statistical analysis on 8 years of flight data in order to extract ion peak parameters that depend only on the response of the flight instrument itself. This is accomplished by first sorting the TOF spectra based on their apparent compositional similarities (e.g. primarily water group ions, primarily hydrocarbon ions, etc.) and normalizing each spectrum. The sorted, normalized data are then binned according to TOF, energy, and counts in order to generate energy-dependent probability density maps of each ion peak contour. Finally, by using these density maps to constrain a stochastic peak fitting algorithm we extract confidence intervals for the model parameters associated with various measured ion peaks, establishing a logistics-independent calibration of the body of IMS data gathered over the course of the Cassini mission.

Single-Ion Deconvolution of Mass Peak Overlaps for Atom Probe Microscopy.

PubMed

London, Andrew J; Haley, Daniel; Moody, Michael P

2017-04-01

Due to the intrinsic evaporation properties of the material studied, insufficient mass-resolving power and lack of knowledge of the kinetic energy of incident ions, peaks in the atom probe mass-to-charge spectrum can overlap and result in incorrect composition measurements. Contributions to these peak overlaps can be deconvoluted globally, by simply examining adjacent peaks combined with knowledge of natural isotopic abundances. However, this strategy does not account for the fact that the relative contributions to this convoluted signal can often vary significantly in different regions of the analysis volume; e.g., across interfaces and within clusters. Some progress has been made with spatially localized deconvolution in cases where the discrete microstructural regions can be easily identified within the reconstruction, but this means no further point cloud analyses are possible. Hence, we present an ion-by-ion methodology where the identity of each ion, normally obscured by peak overlap, is resolved by examining the isotopic abundance of their immediate surroundings. The resulting peak-deconvoluted data are a point cloud and can be analyzed with any existing tools. We present two detailed case studies and discussion of the limitations of this new technique.

Operando observations of solid-state electrochemical reactions in Li-ion batteries by spatially resolved TEM EELS and electron holography.

PubMed

Yamamoto, Kazuo; Iriyama, Yasutoshi; Hirayama, Tsukasa

2017-02-08

All-solid-state Li-ion batteries having incombustible solid electrolytes are promising energy storage devices because they have significant advantages in terms of safety, lifetime and energy density. Electrochemical reactions, namely, Li-ion insertion/extraction reactions, commonly occur around the nanometer-scale interfaces between the electrodes and solid electrolytes. Thus, transmission electron microscopy (TEM) is an appropriate technique to directly observe such reactions, providing important information for understanding the fundamental solid-state electrochemistry and improving battery performance. In this review, we introduce two types of TEM techniques for operando observations of battery reactions, spatially resolved electron energy-loss spectroscopy in a TEM mode for direct detection of the Li concentration profiles and electron holography for observing the electric potential changes due to Li-ion insertion/extraction reactions. We visually show how Li-ion insertion/extractions affect the crystal structures, electronic structures, and local electric potential during the charge-discharge processes in these batteries. © The Author 2016. Published by Oxford University Press on behalf of The Japanese Society of Microscopy. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

K-Shell Photoionization of Nickel Ions Using R-Matrix

NASA Technical Reports Server (NTRS)

Witthoeft, M. C.; Bautista, M. A.; Garcia, J.; Kallman, T. R.; Mendoza, C.; Palmeri, P.; Quinet, P.

2011-01-01

We present R-matrix calculations of photoabsorption and photoionization cross sections across the K edge of the Li-like to Ca-like ions stages of Ni. Level-resolved, Breit-Pauli calculations were performed for the Li-like to Na-like stages. Term-resolved calculations, which include the mass-velocity and Darwin relativistic corrections, were performed for the Mg-like to Ca-like ion stages. This data set is extended up to Fe-like Ni using the distorted wave approximation as implemented by AUTOSTRUCTURE. The R-matrix calculations include the effects of radiative and Auger dampings by means of an optical potential. The damping processes affect the absorption resonances converging to the K thresholds causing them to display symmetric profiles of constant width that smear the otherwise sharp edge at the K-shell photoionization threshold. These data are important for the modeling of features found in photoionized plasmas.

A fast plasma analyser for the study of the solar wind interaction with Mars

NASA Astrophysics Data System (ADS)

James, Adrian Martin

This thesis describes the design and development of the FONEMA instrument to be flown aboard the Russian mission to Mars in 1996. Many probes have flown to Mars yet despite this many mysteries still remain, among them the nature of the interaction of the solar wind with the planetary obstacle. In this thesis I will present some of the results from earlier spacecraft and the models of the interaction that they suggest paying particular attention to the contribution of ion analysers. From these results it will become clear that a fast ion sensor is needed to resolve many of the questions about the magnetosphere of Mars. The FONEMA instrument was designed for this job making use of a novel electrostatic mirror and particle collimator combined with parallel magnetic and electrostatic fields to resolve the ions into mass and energy bins. Development and production of the individual elements is discussed in detail.

Development of a ratiometric time-resolved luminescence sensor for pH based on lanthanide complexes.

PubMed

Liu, Mingjing; Ye, Zhiqiang; Xin, Chenglong; Yuan, Jingli

2013-01-25

Time-resolved luminescence bioassay technique using lanthanide complexes as luminescent probes/sensors has shown great utilities in clinical diagnostics and biotechnology discoveries. In this work, a novel terpyridine polyacid derivative that can form highly stable complexes with lanthanide ions in aqueous media, (4'-hydroxy-2,2':6',2''-terpyridine-6,6''-diyl) bis(methylenenitrilo) tetrakis(acetic acid) (HTTA), was designed and synthesized for developing time-resolved luminescence pH sensors based on its Eu(3+) and Tb(3+) complexes. The luminescence characterization results reveal that the luminescence intensity of HTTA-Eu(3+) is strongly dependent on the pH values in weakly acidic to neutral media (pK(a) = 5.8, pH 4.8-7.5), while that of HTTA-Tb(3+) is pH-independent. This unique luminescence response allows the mixture of HTTA-Eu(3+) and HTTA-Tb(3+) (the HTTA-Eu(3+)/Tb(3+) mixture) to be used as a ratiometric luminescence sensor for the time-resolved luminescence detection of pH with the intensity ratio of its Tb(3+) emission at 540 nm to its Eu(3+) emission at 610 nm, I(540 nm)/I(610 nm), as a signal. Moreover, the UV absorption spectrum changes of the HTTA-Eu(3+)/Tb(3+) mixture at different pHs (pH 4.0-7.0) also display a ratiometric response to the pH changes with the ratio of absorbance at 290 nm to that at 325 nm, A(290 nm)/A(325 nm), as a signal. This feature enables the HTTA-Eu(3+)/Tb(3+) mixture to have an additional function for the pH detection with the absorption spectrometry technique. For loading the complexes into the living cells, the acetoxymethyl ester of HTTA was synthesized and used for loading HTTA-Eu(3+) and HTTA-Tb(3+) into the cultured HeLa cells. The luminescence imaging results demonstrated the practical utility of the new sensor for the time-resolved luminescence cell imaging application. Copyright © 2012 Elsevier B.V. All rights reserved.

Signal and background considerations for the MRSt on the National Ignition Facility (NIF)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wink, C. W., E-mail: cwink@mit.edu; Frenje, J. A.; Gatu Johnson, M.

2016-11-15

A Magnetic Recoil Spectrometer (MRSt) has been conceptually designed for time-resolved measurements of the neutron spectrum at the National Ignition Facility. Using the MRSt, the goals are to measure the time-evolution of the spectrum with a time resolution of ∼20-ps and absolute accuracy better than 5%. To meet these goals, a detailed understanding and optimization of the signal and background characteristics are required. Through ion-optics, MCNP simulations, and detector-response calculations, it is demonstrated that the goals and a signal-to background >5–10 for the down-scattered neutron measurement are met if the background, consisting of ambient neutrons and gammas, at the MRStmore » is reduced 50–100 times.« less

Signal and background considerations for the MRSt on the National Ignition Facility (NIF)

DOE PAGES

Wink, C. W.; Frenje, J. A.; Hilsabeck, T. J.; ...

2016-08-03

A Magnetic Recoil Spectrometer (MRSt) has been conceptually designed for time-resolved measurements of the neutron spectrum at the National Ignition Facility. Using the MRSt, the goals are to measure the time-evolution of the spectrum with a time resolution of ~20-ps and absolute accuracy better than 5%. To meet these goals, a detailed understanding and optimization of the signal and background characteristics are required. Through ion-optics, MCNP simulations, and detector-response calculations, we demonstrate that the goals and a signal-to background >5-10 for the down-scattered neutron measurement are met if the background, consisting of ambient neutrons and gammas, at the MRSt ismore » reduced 50-100 times.« less

Improved mass resolution and mass accuracy in TOF-SIMS spectra and images using argon gas cluster ion beams.

PubMed

Shon, Hyun Kyong; Yoon, Sohee; Moon, Jeong Hee; Lee, Tae Geol

2016-06-09

The popularity of argon gas cluster ion beams (Ar-GCIB) as primary ion beams in time-of-flight secondary ion mass spectrometry (TOF-SIMS) has increased because the molecular ions of large organic- and biomolecules can be detected with less damage to the sample surfaces. However, Ar-GCIB is limited by poor mass resolution as well as poor mass accuracy. The inferior quality of the mass resolution in a TOF-SIMS spectrum obtained by using Ar-GCIB compared to the one obtained by a bismuth liquid metal cluster ion beam and others makes it difficult to identify unknown peaks because of the mass interference from the neighboring peaks. However, in this study, the authors demonstrate improved mass resolution in TOF-SIMS using Ar-GCIB through the delayed extraction of secondary ions, a method typically used in TOF mass spectrometry to increase mass resolution. As for poor mass accuracy, although mass calibration using internal peaks with low mass such as hydrogen and carbon is a common approach in TOF-SIMS, it is unsuited to the present study because of the disappearance of the low-mass peaks in the delayed extraction mode. To resolve this issue, external mass calibration, another regularly used method in TOF-MS, was adapted to enhance mass accuracy in the spectrum and image generated by TOF-SIMS using Ar-GCIB in the delayed extraction mode. By producing spectra analyses of a peptide mixture and bovine serum albumin protein digested with trypsin, along with image analyses of rat brain samples, the authors demonstrate for the first time the enhancement of mass resolution and mass accuracy for the purpose of analyzing large biomolecules in TOF-SIMS using Ar-GCIB through the use of delayed extraction and external mass calibration.

Continuous Flow Liquid Microjunction Surface Sampling Probe Connected On-line with HPLC/MS for Spatially Resolved Analysis of Small Molecules and Proteins

DOE Office of Scientific and Technical Information (OSTI.GOV)

Van Berkel, Gary J; Kertesz, Vilmos

RATIONALE: A continuous flow liquid microjunction surface sampling probe extracts soluble material from surfaces for direct ionization and detection by MS. Demonstrated here is the on-line coupling of such a probe with HPLC/MS enabling extraction, separation and detection of small molecules and proteins from surfaces in a spatially resolved (~0.5 mm diameter spots) manner. Methods: A continuous flow liquid microjunction surface sampling probe was connected to a 6-port, 2-position valve for extract collection and injection to an HPLC column. A QTRAP 5500 hybrid triple quadrupole linear ion trap equipped with a Turbo V ion source operated in positive ESI modemore » was used for all experiments. System operation was tested with extraction, separation and detection of propranolol and associated metabolites from drug dosed tissues and proteins from dried sheep blood spots on paper. Results: Confirmed in the tissue were the parent drug and two different hydroxypropranolol glucuronides. The mass spectrometric response for these compounds from different locations in the liver showed an increase with increasing extraction time (5, 20 and 40 s extractions). For on-line separation and detection/identification of extracted proteins from dried sheep blood spots, two major protein peaks dominated the chromatogram and could be correlated with the expected masses for the hemoglobin and chains. Conclusions: Spatially resolved sampling, separation, and detection of small molecules and proteins from surfaces can be accomplished using a continuous flow liquid microjunction surface sampling probe coupled on-line with HPLC/MS detection.« less

Comprehensive lipidomic analysis of human plasma using multidimensional liquid- and gas-phase separations: Two-dimensional liquid chromatography-mass spectrometry vs. liquid chromatography-trapped-ion-mobility-mass spectrometry.

PubMed

Baglai, Anna; Gargano, Andrea F G; Jordens, Jan; Mengerink, Ynze; Honing, Maarten; van der Wal, Sjoerd; Schoenmakers, Peter J

2017-12-29

Recent advancements in separation science have resulted in the commercialization of multidimensional separation systems that provide higher peak capacities and, hence, enable a more-detailed characterization of complex mixtures. In particular, two powerful analytical tools are increasingly used by analytical scientists, namely online comprehensive two-dimensional liquid chromatography (LC×LC, having a second-dimension separation in the liquid phase) and liquid chromatography-ion mobility-spectrometry (LC-IMS, second dimension separation in the gas phase). The goal of the current study was a general assessment of the liquid-chromatography-trapped-ion-mobility-mass spectrometry (LC-TIMS-MS) and comprehensive two-dimensional liquid chromatography-mass spectrometry (LC×LC-MS) platforms for untargeted lipid mapping in human plasma. For the first time trapped-ion-mobility spectrometry (TIMS) was employed for the separation of the major lipid classes and ion-mobility-derived collision-cross-section values were determined for a number of lipid standards. The general effects of a number of influencing parameters have been inspected and possible directions for improvements are discussed. We aimed to provide a general indication and practical guidelines for the analyst to choose an efficient multidimensional separation platform according to the particular requirements of the application. Analysis time, orthogonality, peak capacity, and an indicative measure for the resolving power are discussed as main characteristics for multidimensional separation systems. Copyright © 2017 Elsevier B.V. All rights reserved.

The Use of Laser-Induced Fluorescence to Characterize Discharge Cathode Erosion in a 30 cm Ring-Cusp Ion Thruster

NASA Technical Reports Server (NTRS)

Sovey, James S. (Technical Monitor); Williams, George J., Jr.

2004-01-01

Relative erosion rates and impingement ion production mechanisms have been identified for the discharge cathode of a 30 cm ion engine using laser-induced fluorescence (LIF). Mo and W erosion products as well as neutral and singly ionized xenon were interrogated. The erosion increased with both discharge current and voltage and spatially resolved measurements agreed with observed erosion patters. Ion velocity mapping identified back-flowing ions near the regions of erosion with energies potentially sufficient to generate the level of observed erosion. Ion production regions downstream of the cathode were indicated and were suggested as possible sources of the erosion causing ions.

Time-Resolved Transient Optical Absorption Study of Bis(terpyridyl)oligothiophenes and Their Metallo-Supramolecular Polymers with Zn(II) Ion Couplers.

PubMed

Rais, David; Menšík, Miroslav; Štenclová-Bláhová, Pavla; Svoboda, Jan; Vohlídal, Jiří; Pfleger, Jiří

2015-06-18

α,ω-Bis(terpyridyl)oligothiophenes spontaneously assemble with Zn(II) ions giving conjugated constitutional dynamic polymers (dynamers) of the metallo-supramolecular class, which potentially might be utilized in optoelectronics. Their photophysical properties, which are of great importance in this field of application, are strongly influenced by the dynamic morphology. It was assessed in this study by using ultrafast pump-probe optical absorption spectroscopy. We identified and characterized relaxation processes running in photoexcited molecules of these oligomers and dynamers and show impacts of disturbed coplanarity of adjacent rings (twisting the thiophene-thiophene and thiophene-terpyridyl bonds by attached hexyl side groups) and Zn(II) ion couplers on these processes. Major effects are seen in the time constants of rotational relaxation, intersystem crossing, and de-excitation lifetimes. The photoexcited states formed on different repeating units within the same dynamer chain do not interact with each other even at very high excitation density. The method is presented that allows determining the equilibrium fraction of unbound oligothiophene species in a dynamer solution, from which otherwise hardly accessible values of the average degree of polymerization of constitutionally dynamic chains in solution can be estimated.

(abstract) Optical Scattering and Surface Microroughness of Ion Beam Deposited Au and Pt Thin Films

NASA Technical Reports Server (NTRS)

Al-Jumaily, Ghanim A.; Raouf, Nasrat A.; Edlou, Samad M.; Simons, John C.

1994-01-01

Thin films of gold and platinum have been deposited onto superpolished fused silica substrates using thermal evaporation, ion assisted deposition (IAD), and ion assisted sputtering. The influence of ion beam flux, thin film material, and deposition rate on the films microroughness have been investigated. Short range surface microroughness of the films has been examined using scanning tunneling microscopy (STM) and atomic force microscopy (AFM). Long range surface microroughness has been characterized using an angle resolved optical scatterometer. Results indicate that ion beam deposited coatings have improved microstructure over thermally evaporated films.

Motion of the Ca2+-pump captured.

PubMed

Yokokawa, Masatoshi; Takeyasu, Kunio

2011-09-01

Studies of ion pumps, such as ATP synthetase and Ca(2+)-ATPase, have a long history. The crystal structures of several kinds of ion pump have been resolved, and provide static pictures of mechanisms of ion transport. In this study, using fast-scanning atomic force microscopy, we have visualized conformational changes in the sarcoplasmic reticulum Ca(2+)-ATPase (SERCA) in real time at the single-molecule level. The analyses of individual SERCA molecules in the presence of both ATP and free Ca(2+) revealed up-down structural changes corresponding to the Albers-Post scheme. This fluctuation was strongly affected by the ATP and Ca(2+) concentrations, and was prevented by an inhibitor, thapsigargin. Interestingly, at a physiological ATP concentrations, the up-down motion disappeared completely. These results indicate that SERCA does not transit through the shortest structure, and has a catalytic pathway different from the ordinary Albers-Post scheme under physiological conditions. © 2011 The Authors Journal compilation © 2011 FEBS.

Proton acceleration: new developments for focusing and energy selection, and applications in plasma physics

NASA Astrophysics Data System (ADS)

Audebert, P.

2007-11-01

In the last few years, intense research has been conducted on laser-accelerated ion sources and their applications. These sources have exceptional properties, i.e. high brightness and high spectral cut-off, high directionality and laminarity, short burst duration. We have shown that for proton energies >10 MeV, the transverse and longitudinal emittance are respectively <0.004 mm-mrad and <10-4 eV-s, i.e. at least 100-fold and may be as much as 10^4-fold better than conventional accelerators beams. Thanks to these properties, these sources allow for example point-projection radiography with unprecedented resolution. We will show example of such time and space-resolved radiography of fast evolving fields, either of associated with the expansion of a plasma in vacuum [*] or with the propagation of a ICF-relevant laser beam in an underdense plasma. These proton sources also open new opportunities for ion beam generation and control, and could stimulate development of compact ion accelerators for many applications.

Experimental characterization of a transition from collisionless to collisional interaction between head-on-merging supersonic plasma jets a)

DOE PAGES

Moser, Auna L.; Hsu, Scott C.

2015-05-01

We present results from experiments on the head-on merging of two supersonic plasma jets in an initially collisionless regime for the counter-streaming ions [A. L. Moser & S. C. Hsu, Phys. Plasmas, submitted (2014)]. The plasma jets are of either an argon/impurity or hydrogen/impurity mixture and are produced by pulsed-power-driven railguns. Based on time- and space-resolved fast-imaging, multi-chord interferometry, and survey-spectroscopy measurements of the overlapping region between the merging jets, we observe that the jets initially interpenetrate, consistent with calculated inter-jet ion collision lengths, which are long. As the jets interpenetrate, a rising mean-charge state causes a rapid decrease inmore » the inter-jet ion collision length. Finally, the interaction becomes collisional and the jets stagnate, eventually producing structures consistent with collisional shocks. These experimental observations can aid in the validation of plasma collisionality and ionization models for plasmas with complex equations of state.« less

Laser characterization of electric field oscillations in the Hall thruster breathing mode

NASA Astrophysics Data System (ADS)

Young, Christopher; Lucca Fabris, Andrea; MacDonald-Tenenbaum, Natalia; Hargus, William, Jr.; Cappelli, Mark

2016-10-01

Hall thrusters are a mature technology for space propulsion applications that exhibit a wide array of dynamic behavior, including plasma waves, instabilities and turbulence. One common low frequency (10-50 kHz) discharge current oscillation is the breathing mode, a cycle of neutral propellant injection, strong ionization, and ion acceleration by a steep potential gradient. A time-resolved laser-induced fluorescence diagnostic non-intrusively captures this propagating ionization front in the channel of a commercial BHT-600 Hall thruster manufactured by Busek Co. Measurements of ion velocity and relative ion density (using the 5 d[ 4 ] 7 / 2 - 6 p[ 3 ] 5 / 2 Xe II transition at 834.95 nm, vacuum) reveal a dynamic electric field structure traversing the channel throughout the breathing mode cycle. This work is sponsored by the U.S. Air Force Office of Scientific Research, with Dr. M. Birkan as program manager. C.Y. acknowledges support from the DOE NSSA Stewardship Science Graduate Fellowship under contract DE-FC52-08NA28752.

Fabrication of solid-state secondary battery using semiconductors and evaluation of its charge/discharge characteristics

NASA Astrophysics Data System (ADS)

Sasaki, Atsuya; Sasaki, Akito; Hirabayashi, Hideaki; Saito, Shuichi; Aoki, Katsuaki; Kataoka, Yoshinori; Suzuki, Koji; Yabuhara, Hidehiko; Ito, Takahiro; Takagi, Shigeyuki

2018-04-01

Li-ion batteries have attracted interest for use as storage batteries. However, the risk of fire has not yet been resolved. Although solid Li-ion batteries are possible alternatives, their performance characteristics are unsatisfactory. Recently, research on utilizing the accumulation of carriers at the trap levels of semiconductors has been performed. However, the detailed charge/discharge characteristics and principles have not been reported. In this report, we attempted to form new n-type oxide semiconductor/insulator/p-type oxide semiconductor structures. The battery characteristics of these structures were evaluated by charge/discharge measurements. The obtained results clearly indicated the characteristics of rechargeable batteries. Furthermore, the fabricated structure accumulated an approximately 5000 times larger number of carriers than a parallel plate capacitor. Additionally, by constructing circuit models based on the experimental results, the charge/discharge mechanisms were considered. This is the first detailed experimental report on a rechargeable battery that operates without the double injection of ions and electrons.

The current status of the MASHA setup

NASA Astrophysics Data System (ADS)

Vedeneev, V. Yu.; Rodin, A. M.; Krupa, L.; Belozerov, A. V.; Chernysheva, E. V.; Dmitriev, S. N.; Gulyaev, A. V.; Gulyaeva, A. V.; Kamas, D.; Kliman, J.; Komarov, A. B.; Motycak, S.; Novoselov, A. S.; Salamatin, V. S.; Stepantsov, S. V.; Podshibyakin, A. V.; Yukhimchuk, S. A.; Granja, C.; Pospisil, S.

2017-11-01

The MASHA setup designed as the mass-separator with the resolving power of about 1700, which allows mass identification of superheavy nuclides is described. The setup uses solid ISOL (Isotope Separation On-Line) method. In the present article the upgrade of some parts of MASHA are described: target box (rotating target + hot catcher), ion source based on electron cyclotron resonance, data acquisition, beam diagnostics and control systems. The upgrade is undertaken in order to increase the total separation efficiency, reduce the separation time, of the installation and working stability and make possible continuous measurements at high beam currents. Ion source efficiency was measured in autonomous regime with using calibrated gas leaks of Kr and Xe injected directly to ion source. Some results of the first experiments for production of radon isotopes using the multi-nucleon transfer reaction 48Ca+242Pu are described in the present article. The using of TIMEPIX detector with MASHA setup for neutron-rich Rn isotopes identification is also described.

Experimental characterization of a transition from collisionless to collisional interaction between head-on-merging supersonic plasma jets a)

DOE Office of Scientific and Technical Information (OSTI.GOV)

Moser, Auna L.; Hsu, Scott C.

We present results from experiments on the head-on merging of two supersonic plasma jets in an initially collisionless regime for the counter-streaming ions [A. L. Moser & S. C. Hsu, Phys. Plasmas, submitted (2014)]. The plasma jets are of either an argon/impurity or hydrogen/impurity mixture and are produced by pulsed-power-driven railguns. Based on time- and space-resolved fast-imaging, multi-chord interferometry, and survey-spectroscopy measurements of the overlapping region between the merging jets, we observe that the jets initially interpenetrate, consistent with calculated inter-jet ion collision lengths, which are long. As the jets interpenetrate, a rising mean-charge state causes a rapid decrease inmore » the inter-jet ion collision length. Finally, the interaction becomes collisional and the jets stagnate, eventually producing structures consistent with collisional shocks. These experimental observations can aid in the validation of plasma collisionality and ionization models for plasmas with complex equations of state.« less

Online differentiation of mineral phase in aerosol particles by ion formation mechanism using a LAAP-TOF single-particle mass spectrometer

NASA Astrophysics Data System (ADS)

Marsden, Nicholas A.; Flynn, Michael J.; Allan, James D.; Coe, Hugh

2018-01-01

Mineralogy of silicate mineral dust has a strong influence on climate and ecosystems due to variation in physiochemical properties that result from differences in composition and crystal structure (mineral phase). Traditional offline methods of analysing mineral phase are labour intensive and the temporal resolution of the data is much longer than many atmospheric processes. Single-particle mass spectrometry (SPMS) is an established technique for the online size-resolved measurement of particle composition by laser desorption ionisation (LDI) followed by time-of-flight mass spectrometry (TOF-MS). Although non-quantitative, the technique is able to identify the presence of silicate minerals in airborne dust particles from markers of alkali metals and silicate molecular ions in the mass spectra. However, the differentiation of mineral phase in silicate particles by traditional mass spectral peak area measurements is not possible. This is because instrument function and matrix effects in the ionisation process result in variations in instrument response that are greater than the differences in composition between common mineral phases.In this study, we introduce a novel technique that enables the differentiation of mineral phase in silicate mineral particles by ion formation mechanism measured from subtle changes in ion arrival times at the TOF-MS detector. Using a combination of peak area and peak centroid measurements, we show that the arrangement of the interstitial alkali metals in the crystal structure, an important property in silicate mineralogy, influences the ion arrival times of elemental and molecular ion species in the negative ion mass spectra. A classification scheme is presented that allowed for the differentiation of illite-smectite, kaolinite and feldspar minerals on a single-particle basis. Online analysis of mineral dust aerosol generated from clay mineral standards produced mineral fractions that are in agreement with bulk measurements reported by traditional XRD (X-ray diffraction) analysis.

Initial clinical evaluation of PET-based ion beam therapy monitoring under consideration of organ motion

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kurz, Christopher, E-mail: christopher.kurz@physik.uni-muenchen.de; Bauer, Julia; Unholtz, Daniel

2016-02-15

Purpose: Intrafractional organ motion imposes considerable challenges to scanned ion beam therapy and demands for a thorough verification of the applied treatment. At the Heidelberg Ion-Beam Therapy Center (HIT), the scanned ion beam delivery is verified by means of postirradiation positron-emission-tomography (PET) imaging. This work presents a first clinical evaluation of PET-based treatment monitoring in ion beam therapy under consideration of target motion. Methods: Three patients with mobile liver lesions underwent scanned carbon ion irradiation at HIT and postirradiation PET/CT (x-ray-computed-tomography) imaging with a commercial scanner. Respiratory motion was recorded during irradiation and subsequent image acquisition. This enabled a time-resolvedmore » (4D) calculation of the expected irradiation-induced activity pattern and, for one patient where an additional 4D CT was acquired at the PET/CT scanner after treatment, a motion-compensated PET image reconstruction. For the other patients, PET data were reconstructed statically. To verify the treatment, calculated prediction and reconstructed measurement were compared with a focus on the ion beam range. Results: Results in the current three patients suggest that for motion amplitudes in the order of 2 mm there is no benefit from incorporating respiratory motion information into PET-based treatment monitoring. For a target motion in the order of 10 mm, motion-related effects become more severe and a time-resolved modeling of the expected activity distribution can lead to an improved data interpretation if a sufficient number of true coincidences is detected. Benefits from motion-compensated PET image reconstruction could not be shown conclusively at the current stage. Conclusions: The feasibility of clinical PET-based treatment verification under consideration of organ motion has been shown for the first time. Improvements in noise-robust 4D PET image reconstruction are deemed necessary to enhance the clinical potential.« less

X-ray microprobe of orbital alignment in strong-field ionized atoms.

PubMed

Young, L; Arms, D A; Dufresne, E M; Dunford, R W; Ederer, D L; Höhr, C; Kanter, E P; Krässig, B; Landahl, E C; Peterson, E R; Rudati, J; Santra, R; Southworth, S H

2006-08-25

We have developed a synchrotron-based, time-resolved x-ray microprobe to investigate optical strong-field processes at intermediate intensities (10(14) - 10(15) W/cm2). This quantum-state specific probe has enabled the direct observation of orbital alignment in the residual ion produced by strong-field ionization of krypton atoms via resonant, polarized x-ray absorption. We found strong alignment to persist for a period long compared to the spin-orbit coupling time scale (6.2 fs). The observed degree of alignment can be explained by models that incorporate spin-orbit coupling. The methodology is applicable to a wide range of problems.

Long-lived and Well-resolved Mn2+ Ion Emissions in CuInS-ZnS Quantum Dots

PubMed Central

Cao, Sheng; Li, Chengming; Wang, Lin; Shang, Minghui; Wei, Guodong; Zheng, Jinju; Yang, Weiyou

2014-01-01

CuInS2 (CIS) quantum dots (QDs) have tunable photoluminescence (PL) behaviors in the visible and near infrared spectral range with markedly lower toxicity than the cadmium-based counterparts, making them very promising applications in light emitting and solar harvesting. However, there still remain material- and fabrication- related obstacles in realizing the high-performance CIS-based QDs with well-resolved Mn2+ d-d emission, long emission lifetimes as well as high efficiencies. Here, we demonstrate the growth of high-quality Mn2+-doped CuInS-ZnS (CIS-ZnS) QDs based on a multi-step hot-injection strategy. The resultant QDs exhibit a well-resolved Mn2+ d-d emission with a high PL quantum yield (QY) up to 66% and an extremely long excited state lifetime up to ~3.78 ms, which is nearly two times longer than the longest one of “green” QDs ever reported. It is promising that the synthesized Mn2+-doped CIS-ZnS QDs might open new doors for their practical applications in bioimaging and opto/electronic devices. PMID:25515207

Mass cytometry: technique for real time single cell multitarget immunoassay based on inductively coupled plasma time-of-flight mass spectrometry.

PubMed

Bandura, Dmitry R; Baranov, Vladimir I; Ornatsky, Olga I; Antonov, Alexei; Kinach, Robert; Lou, Xudong; Pavlov, Serguei; Vorobiev, Sergey; Dick, John E; Tanner, Scott D

2009-08-15

A novel instrument for real time analysis of individual biological cells or other microparticles is described. The instrument is based on inductively coupled plasma time-of-flight mass spectrometry and comprises a three-aperture plasma-vacuum interface, a dc quadrupole turning optics for decoupling ions from neutral components, an rf quadrupole ion guide discriminating against low-mass dominant plasma ions, a point-to-parallel focusing dc quadrupole doublet, an orthogonal acceleration reflectron analyzer, a discrete dynode fast ion detector, and an 8-bit 1 GHz digitizer. A high spectrum generation frequency of 76.8 kHz provides capability for collecting multiple spectra from each particle-induced transient ion cloud, typically of 200-300 micros duration. It is shown that the transients can be resolved and characterized individually at a peak frequency of 1100 particles per second. Design considerations and optimization data are presented. The figures of merit of the instrument are measured under standard inductively coupled plasma (ICP) operating conditions (<3% cerium oxide ratio). At mass resolution (full width at half-maximum) M/DeltaM > 900 for m/z = 159, the sensitivity with a standard sample introduction system of >1.4 x 10(8) ion counts per second per mg L(-1) of Tb and an abundance sensitivity of (6 x 10(-4))-(1.4 x 10(-3)) (trailing and leading masses, respectively) are shown. The mass range (m/z = 125-215) and abundance sensitivity are sufficient for elemental immunoassay with up to 60 distinct available elemental tags. When <15 elemental tags are used, a higher sensitivity mode at lower resolution (M/DeltaM > 500) can be used, which provides >2.4 x 10(8) cps per mg L(-1) of Tb, at (1.5 x 10(-3))-(5.0 x 10(-3)) abundance sensitivity. The real-time simultaneous detection of multiple isotopes from individual 1.8 microm polystyrene beads labeled with lanthanides is shown. A real time single cell 20 antigen expression assay of model cell lines and leukemia patient samples immuno-labeled with lanthanide-tagged antibodies is presented.

Simulation of plasma loading of high-pressure RF cavities

NASA Astrophysics Data System (ADS)

Yu, K.; Samulyak, R.; Yonehara, K.; Freemire, B.

2018-01-01

Muon beam-induced plasma loading of radio-frequency (RF) cavities filled with high pressure hydrogen gas with 1% dry air dopant has been studied via numerical simulations. The electromagnetic code SPACE, that resolves relevant atomic physics processes, including ionization by the muon beam, electron attachment to dopant molecules, and electron-ion and ion-ion recombination, has been used. Simulations studies have been performed in the range of parameters typical for practical muon cooling channels.

Science of Decision Making: A Data-Modeling Approach

DTIC Science & Technology

2013-10-01

were separated on a capillary column using the Dionex UltiMate 3000 (Sunnyvale, CA). The resolved peptides were then sprayed into a linear ion trap...database (3–5). These algorithms assign a peptide sequence, along with a matching score of the experimental ion product mass spectrum, to a theoretical ion ...Bacterial Sample Processing Samples were prepared for liquid chromatography (LC) tandem MS (LC– MS/MS) in a similar manner to that previously reported

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lehmann, C. S.; Picón, A.; Bostedt, C.

The availability at x-ray free electron lasers of generating two intense, femtosecond x-ray pulses with controlled time delay opens the possibility of performing time-resolved experiments for x-ray induced phenomena. We have applied this capability to molecular dynamics. In diatomic molecules composed of low-Z elements, K-shell ionization creates a core-hole state in which the main decay is an Auger process involving two electrons in the valence shell. After Auger decay, the nuclear wavepackets of the transient two-valence-hole states continue evolving on the femtosecond timescale, leading either to separated atomic ions or long-lived quasi-bound states. By using an x-ray pump and anmore » x-ray probe pulse tuned above the K-shell ionization threshold of the nitrogen molecule, we are able to observe ion dissociation in progress by measuring the time-dependent kinetic energy releases of different breakup channels. We simulated the measurements on N2 with a molecular dynamics model that accounts for K-shell ionization, Auger decay, and time evolution of the nuclear wavepackets. In addition to explaining the time-dependent feature in the measured kinetic energy release distributions from the dissociative states, the simulation also reveals the contributions of quasi-bound states.« less

Infrared Photodissociation Spectroscopy of Metal Ion -WATER Complexes

NASA Astrophysics Data System (ADS)

Bandyopadhyay, B.; Carnegie, P. D.; Duncan, M. A.

2011-06-01

Metal ion-water complexes are produced in a supersonic expansion cluster source via laser vaporization technique. Infrared photodissociation spectroscopy has been performed in the O-H stretch region. DFT calculations have also been carried out to obtain the structures and vibrational frequencies. Infrared spectra show partially resolved rotational structures which will be analyzed.

Laser fluence dependence on emission dynamics of ultrafast laser induced copper plasma

DOE PAGES

Anoop, K. K.; Harilal, S. S.; Philip, Reji; ...

2016-11-14

The characteristic emission features of a laser-produced plasma strongly depend strongly on the laser fluence. We investigated the spatial and temporal dynamics of neutrals and ions in femtosecond laser (800 nm, ≈ 40 fs, Ti:Sapphire) induced copper plasma in vacuum using both optical emission spectroscopy (OES) and spectrally resolved two-dimensional (2D) imaging methods over a wide fluence range of 0.5 J/cm 2-77.5 J/cm 2. 2D fast gated monochromatic images showed distinct plume splitting between the neutral and ions especially at moderate to higher fluence ranges. OES studies at low to moderate laser fluence regime confirm intense neutral line emission overmore » the ion emission whereas this trend changes at higher laser fluence with dominance of the latter. This evidences a clear change in the physical processes involved in femtosecond laser matter interaction at high input laser intensity. The obtained ion dynamics resulting from the OES, and spectrally resolved 2D imaging are compared with charged particle measurement employing Faraday cup and Langmuir probe and results showed good correlation.« less

Time-resolved optically stimulated luminescence of Al2O3:C for ion beam therapy dosimetry

NASA Astrophysics Data System (ADS)

Yukihara, Eduardo G.; Doull, Brandon A.; Ahmed, Md; Brons, Stephan; Tessonnier, Thomas; Jäkel, Oliver; Greilich, Steffen

2015-09-01

The objective of this study was to characterize the time-resolved (TR) optically stimulated luminescence (OSL) from Al2O3:C detectors and investigate methodologies to improve the accuracy of these detectors in ion beam therapy dosimetry, addressing the reduction in relative response to high linear energy transfer (LET) particles common to solid-state detectors. Al2O3:C OSL detectors (OSLDs) were exposed to proton, 4He, 12C and 16O beams in 22 particle/energy combinations and read using a custom-built TR-OSL reader. The OSL response {{r}\\text{OSL}} , relative to 60Co gamma dose to water, and the ratio between the UV and blue OSL emission bands of Al2O3:C (UV/blue ratio) were determined as a function of the LET. Monte-Carlo simulations with the multi-purpose interaction and transport code FLUKA were used to estimate the absorbed doses and particle energy spectra in the different irradiation conditions. The OSL responses {{r}\\text{OSL}} varied from 0.980 (0.73 keV μm-1) to 0.288 (120.8 keV μm-1). The OSL UV/blue ratio varied by a factor of two in the investigated LET range, but the variation for 12C beams was only 11%. OSLDs were also irradiated at different depths of carbon ion spread-out Bragg peaks (SOBPs), where it was shown that doses could be obtained with an accuracy of  ±2.0% at the entrance channel and within the SOBP using correction factors calculated based on the OSL responses obtained in this study. The UV/blue ratio did not allow accurate estimation of the dose-averaged LET for 12C SOBPs, although the values obtained can be explained with the data obtained in this study and the additional information provided by the Monte-Carlo simulations. The results demonstrate that accurate OSLD dosimetry can be performed in ion beam therapy using appropriate corrections for the OSL response.

Simple area determination of strongly overlapping ion mobility peaks.

PubMed

Borovcová, Lucie; Hermannová, Martina; Pauk, Volodymyr; Šimek, Matěj; Havlíček, Vladimír; Lemr, Karel

2017-08-15

Coupling of ion mobility with mass spectrometry has brought new frontiers in separation and quantitation of a wide range of isobaric/isomeric compounds. Ion mobility spectrometry may separate ions possessing the identical molecular formula but having different molecular shapes. The separation space in most commercially available instruments is limited and rarely the mobility resolving power exceeds one hundred. From this perspective, new approaches allowing for extracting individual compound signals out of a more complex mixture are needed. In this work we present a new simple analytical approach based on fitting of arrival time distribution (ATD) profiles by Gaussian functions and generating of ATD functions. These ATD functions well describe even distorted ion mobility peaks of individual compounds and allow for extracting their peaks from mobilograms of mixtures. Contrary to classical integration, our approach works well with irregular overlapping peaks. Using mobilograms of standards to generate ATD functions, poorly separated compounds, e.g. isomers, with identical mass spectra representing a hard to solve task for various chemometric methods can be easily distinguished by our procedure. Alternatively ATD functions can be obtained from ATD profiles of ions unique to individual mixture components (if such ions exist) and mobilograms of standards are not required. On a set of hyaluronan-derived oligosaccharides we demonstrated excellent ATD repeatability enabling the resolution of binary mixtures, including mixtures with minor component level about 5%. Ion mobility quantitative data of isomers were confirmed by high performance liquid chromatography. Copyright © 2017 Elsevier B.V. All rights reserved.

Identification of Ion-Pair Structures in Solution by Vibrational Stark Effects.

PubMed

Hack, John; Grills, David C; Miller, John R; Mani, Tomoyasu

2016-02-18

Ion pairing is a fundamental consideration in many areas of chemistry and has implications in a wide range of sciences and technologies that include batteries and organic photovoltaics. Ions in solution are known to inhabit multiple possible states, including free ions (FI), contact ion pairs (CIP), and solvent-separated ion pairs (SSIP). However, in solutions of organic radicals and nonmetal electrolytes, it is often difficult to distinguish between these states. In the first part of this work, we report evidence for the formation of SSIPs in low-polarity solvents and distinct measurements of CIP, SSIP, and FI, by using the ν(C≡N) infrared (IR) band of a nitrile-substituted fluorene radical anion. Use of time-resolved IR detection following pulse radiolysis allowed us to unambiguously assign the peak of the FI. In the presence of nonmetal electrolytes, two distinct red-shifted peaks were observed and assigned to the CIP and SSIP. The assignments are interpreted in the framework of the vibrational Stark effect (VSE) and are supported by (1) the solvent dependence of ion-pair populations, (2) the observation of a cryptand-separated sodium ion pair that mimics the formation of SSIPs, and (3) electronic structure calculations. In the second part of this work, we show that a blue-shift of the ν(C≡N) IR band due to the VSE can be induced in a nitrile-substituted fluorene radical anion by covalently tethering it to a metal-chelating ligand that forms an intramolecular ion pair upon reduction and complexation with sodium ion. This adds support to the conclusion that the shift in IR absorptions by ion pairing originates from the VSE. These results combined show that we can identify ion-pair structures by using the VSE, including the existence of SSIPs in a low-polarity solvent.

Generation and Evolution of High-Mach-Number Laser-Driven Magnetized Collisionless Shocks in the Laboratory

DOE PAGES

Schaeffer, D. B.; Fox, W.; Haberberger, D.; ...

2017-07-13

Here, we present the first laboratory generation of high-Mach-number magnetized collisionless shocks created through the interaction of an expanding laser-driven plasma with a magnetized ambient plasma. Time-resolved, two-dimensional imaging of plasma density and magnetic fields shows the formation and evolution of a supercritical shock propagating at magnetosonic Mach number M ms ≈ 12. Particle-in-cell simulations constrained by experimental data further detail the shock formation and separate dynamics of the multi-ion-species ambient plasma. The results show that the shocks form on time scales as fast as one gyroperiod, aided by the efficient coupling of energy, and the generation of a magneticmore » barrier between the piston and ambient ions. The development of this experimental platform complements present remote sensing and spacecraft observations, and opens the way for controlled laboratory investigations of high-Mach number collisionless shocks, including the mechanisms and efficiency of particle acceleration.« less

Generation and Evolution of High-Mach-Number Laser-Driven Magnetized Collisionless Shocks in the Laboratory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Schaeffer, D. B.; Fox, W.; Haberberger, D.

Here, we present the first laboratory generation of high-Mach-number magnetized collisionless shocks created through the interaction of an expanding laser-driven plasma with a magnetized ambient plasma. Time-resolved, two-dimensional imaging of plasma density and magnetic fields shows the formation and evolution of a supercritical shock propagating at magnetosonic Mach number M ms ≈ 12. Particle-in-cell simulations constrained by experimental data further detail the shock formation and separate dynamics of the multi-ion-species ambient plasma. The results show that the shocks form on time scales as fast as one gyroperiod, aided by the efficient coupling of energy, and the generation of a magneticmore » barrier between the piston and ambient ions. The development of this experimental platform complements present remote sensing and spacecraft observations, and opens the way for controlled laboratory investigations of high-Mach number collisionless shocks, including the mechanisms and efficiency of particle acceleration.« less

Coherent control at its most fundamental: carrier-envelope-phase-dependent electron localization in photodissociation of a H2(+) molecular ion beam target.

PubMed

Rathje, T; Sayler, A M; Zeng, S; Wustelt, P; Figger, H; Esry, B D; Paulus, G G

2013-08-30

Measurements and calculations of the absolute carrier-envelope-phase (CEP) effects in the photodissociation of the simplest molecule, H2(+), with a 4.5-fs Ti:sapphire laser pulse at intensities up to (4±2)×10(14)  W/cm2 are presented. Localization of the electron with respect to the two nuclei (during the dissociation process) is controlled via the CEP of the ultrashort laser pulses. In contrast to previous CEP-dependent experiments with neutral molecules, the dissociation of the molecular ions is not preceded by a photoionization process, which strongly influences the CEP dependence. Kinematically complete data are obtained by time- and position-resolved coincidence detection. The phase dependence is determined by a single-shot phase measurement correlated to the detection of the dissociation fragments. The experimental results show quantitative agreement with ab initio 3D time-dependent Schrödinger equation calculations that include nuclear vibration and rotation.

A method to visualize transdermal nickel permeation in mouse skin using a nickel allergy patch

PubMed Central

Sugiyama, Tomoko; Uo, Motohiro; Wada, Takahiro; Hongo, Toshio; Omagari, Daisuke; Komiyama, Kazuo; Oikawa, Masakazu; Kusama, Mikio; Mori, Yoshiyuki

2015-01-01

Metal patch test is often used in clinical settings when metal-induced contact dermatitis is suspected. However, the transdermal permeation behavior of metal ions from the patch test remains unclear. Current patch tests using high concentrations of metal salt solutions have some side effects, e.g. acute skin reactions to high concentrations of metal salt. To resolve these, estimating metal ion transdermal permeation is wished. In this study, synchrotron radiation X-ray fluorescence (SR-XRF) and micro-focused particle-induced X-ray emission (micro-PIXE) were used to visualize the time-dependent Ni permeation in mouse skin. The cross-sectional diffusion of Ni was visualized in a time-dependent manner. Our results indicate that maximum Ni permeation occurs after 24 h of patch treatment, and the permeated Ni content was high in the epidermis and spread into the dermis beyond the basal layer. This method may be useful to determine the appropriate solution concentration and duration of administration for the patch test. PMID:26484550

Surface-Induced Dissociation of Protein Complexes in a Hybrid Fourier Transform Ion Cyclotron Resonance Mass Spectrometer.

PubMed

Yan, Jing; Zhou, Mowei; Gilbert, Joshua D; Wolff, Jeremy J; Somogyi, Árpád; Pedder, Randall E; Quintyn, Royston S; Morrison, Lindsay J; Easterling, Michael L; Paša-Tolić, Ljiljana; Wysocki, Vicki H

2017-01-03

Mass spectrometry continues to develop as a valuable tool in the analysis of proteins and protein complexes. In protein complex mass spectrometry studies, surface-induced dissociation (SID) has been successfully applied in quadrupole time-of-flight (Q-TOF) instruments. SID provides structural information on noncovalent protein complexes that is complementary to other techniques. However, the mass resolution of Q-TOF instruments can limit the information that can be obtained for protein complexes by SID. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) provides ultrahigh resolution and ultrahigh mass accuracy measurements. In this study, an SID device was designed and successfully installed in a hybrid FT-ICR instrument in place of the standard gas collision cell. The SID-FT-ICR platform has been tested with several protein complex systems (homooligomers, a heterooligomer, and a protein-ligand complex, ranging from 53 to 85 kDa), and the results are consistent with data previously acquired on Q-TOF platforms, matching predictions from known protein interface information. SID fragments with the same m/z but different charge states are well-resolved based on distinct spacing between adjacent isotope peaks, and the addition of metal cations and ligands can also be isotopically resolved with the ultrahigh mass resolution available in FT-ICR.

The addition of a second lanthanide ion to increase the luminescence of europium(III) macrocyclic complexes

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bromm, A.J. Jr.; Vallarino, L.M.; Leif, R.C.

At present, the microscopic visualization of luminescent labels containing lanthanide(III) ions, primarily europium(III), as light-emitting centers is best performed with time-gated instrumentation, which by virtually eliminating the background fluorescence results in an improved signal to noise ratio. However, the use of the europium(III) macrocycle, Quantum Dye{trademark}, in conjunction with the strong luminescence enhancing effect (cofluorescence) of yttrium(III) or gadolinium(III), can eliminate the need for such specialized instrumentation. In the presence of Gd(III), the luminescence of the Eu(III)-macrocycles can be conveniently observed with conventional fluorescence instrumentation at previously unattainable low levels. The Eu(III) {sup 5}D{sub 0} {r_arrow} {sup 7}F{sub 2} emissionmore » of the Eu(III)-macrocycles was observed as an extremely sharp band with a maximum at 619 nm and a clearly resolved characteristic pattern. At very low Eu(III)-macrocycle concentrations, another sharp emission was detected at 614 nm, arising from traces of Eu(III) present in even the purest commercially available gadolinium products. Discrimination of the resolved emissions of the Eu(III)-macrocycle and Eu(III) contaminant should provide a means to further lower the limit of detection of the Eu(III)-macrocycle.« less

David Robichaud | NREL

Science.gov Websites

Upgrading," Green Chemistry (2018) "Group Additivity Determination for Oxygenates, Oxonium Ions ," Green Chemistry (2015) "Biomass Particle Models with Realistic Morphology and Resolved

On the time behaviour of the concentration of pyrazinium radical cations in the early stage of the Maillard reaction

NASA Astrophysics Data System (ADS)

Stoesser, Reinhard; Klein, Jeannette; Peschke, Simone; Zehl, Andrea; Cämmerer, Bettina; Kroh, Lothar W.

2007-08-01

During the early stage of the Maillard reaction pyrazinium radical cations were detected by ESR within the reaction system D-glucose/glycine. The spectra were characterized by completely resolved hyperfine structure. The partial pressure of oxygen and the radical concentrations were measured directly in the reaction mixture by ESR using solutions of the spin probe TEMPOL and of DPPH, respectively. There are quantitative and qualitative relations of the actual concentration of the radical ions to the partial pressure of oxygen, the temperature-time regime and the mechanical mixing of the reaction system. These macroscopic parameters significantly affect both the induction period and the velocity of the time-dependent formation of free radicals. From in situ variations of p(O 2) and p(Ar) including the connected mixing effects caused by the passing the gases through the reaction mixture, steric and chemical effects of the stabilization of the radical ions were established. The determination of suitable and relevant conditions for stabilization and subsequent radical reactions contributes to the elucidation of the macroscopically known antioxidant activity of Maillard products.

Particle model of a cylindrical inductively coupled ion source

NASA Astrophysics Data System (ADS)

Ippolito, N. D.; Taccogna, F.; Minelli, P.; Cavenago, M.; Veltri, P.

2017-08-01

In spite of the wide use of RF sources, a complete understanding of the mechanisms regulating the RF-coupling of the plasma is still lacking so self-consistent simulations of the involved physics are highly desirable. For this reason we are developing a 2.5D fully kinetic Particle-In-Cell Monte-Carlo-Collision (PIC-MCC) model of a cylindrical ICP-RF source, keeping the time step of the simulation small enough to resolve the plasma frequency scale. The grid cell dimension is now about seven times larger than the average Debye length, because of the large computational demand of the code. It will be scaled down in the next phase of the development of the code. The filling gas is Xenon, in order to minimize the time lost by the MCC collision module in the first stage of development of the code. The results presented here are preliminary, with the code already showing a good robustness. The final goal will be the modeling of the NIO1 (Negative Ion Optimization phase 1) source, operating in Padua at Consorzio RFX.

Scintillator based detector for fast-ion losses induced by magnetohydrodynamic instabilities in the ASDEX upgrade tokamak.

PubMed

García-Muñoz, M; Fahrbach, H-U; Zohm, H

2009-05-01

A scintillator based detector for fast-ion losses has been designed and installed on the ASDEX upgrade (AUG) tokamak [A. Herrmann and O. Gruber, Fusion Sci. Technol. 44, 569 (2003)]. The detector resolves in time the energy and pitch angle of fast-ion losses induced by magnetohydrodynamics (MHD) fluctuations. The use of a novel scintillator material with a very short decay time and high quantum efficiency allows to identify the MHD fluctuations responsible for the ion losses through Fourier analysis. A Faraday cup (secondary scintillator plate) has been embedded behind the scintillator plate for an absolute calibration of the detector. The detector is mounted on a manipulator to vary its radial position with respect to the plasma. A thermocouple on the inner side of the graphite protection enables the safety search for the most adequate radial position. To align the scintillator light pattern with the light detectors a system composed by a lens and a vacuum-compatible halogen lamp has been allocated within the detector head. In this paper, the design of the scintillator probe, as well as the new technique used to analyze the data through spectrograms will be described. A last section is devoted to discuss the diagnosis prospects of this method for ITER [M. Shimada et al., Nucl. Fusion 47, S1 (2007)].

Heat Effect of the Protonation of Glycine and the Enthalpies of Resolvation of Participating Chemical Species in Water-Dimethylsulfoxide Solvent Mixtures

NASA Astrophysics Data System (ADS)

Isaeva, V. A.; Sharnin, V. A.

2018-02-01

Enthalpies of the protonation of glycine in water‒dimethylsulfoxide (DMSO) mixed solvents are determined calorimetrically in the range of DMSO mole fractions of 0.0 to 0.9, at T = 298.15 K and an ionic strength μ = 0.3 (NaClO4). It is established that the protonation of glycine becomes more exothermic with an increasing mole fraction of DMSO, and the enthalpies of resolvation of glycine and glycinium ions in water‒DMSO solvent mixtures are calculated. It is shown that the small changes in the enthalpy of protonation observed at low mole fractions of DMSO are caused by the contributions from the solvation of proton and protonated glycine cancelling each other out. The enthalpy term of the Gibbs energy of the reaction leading to the formation of glycinium ion is estimated along with the enthalpy of resolvation of the reacting species in the water‒DMSO mixed solvent.

Characterization of spatially resolved high resolution x-ray spectrometers for HEDP and light-source experiments

NASA Astrophysics Data System (ADS)

Hill, K. W.; Bitter, M.; Delgado-Aparicio, L.; Efthimion, P.; Pablant, N.; Lu, J.; Beiersdorfer, P.; Chen, H.; Magee, E.

2014-10-01

A high resolution 1D imaging x-ray spectrometer concept comprising a spherically bent crystal and a 2D pixelated detector is being optimized for diagnostics of small sources such as high energy density physics (HEDP) and synchrotron radiation or x-ray free electron laser experiments. This instrument is used on tokamak experiments for measurement of spatial profiles of Doppler ion temperature and plasma flow velocity, as well as electron temperature. Laboratory measurements demonstrate a resolving power, E/ ΔE of 10,000 and spatial resolution better than 10 μm. Good performance is obtained for Bragg angles ranging from 23 to 63 degrees. Initial tests of the instrument on HEDP plasmas are being performed with a goal of developing spatially resolved ion and electron temperature diagnostics. This work was performed under the auspices of the US DOE by PPPL under Contract DE-AC02-09CH11466 and by LLNL under Contract DE-AC52-07NA27344.

Calibration of BAS-TR image plate response to high energy (3-300 MeV) carbon ions

NASA Astrophysics Data System (ADS)

Doria, D.; Kar, S.; Ahmed, H.; Alejo, A.; Fernandez, J.; Cerchez, M.; Gray, R. J.; Hanton, F.; MacLellan, D. A.; McKenna, P.; Najmudin, Z.; Neely, D.; Romagnani, L.; Ruiz, J. A.; Sarri, G.; Scullion, C.; Streeter, M.; Swantusch, M.; Willi, O.; Zepf, M.; Borghesi, M.

2015-12-01

The paper presents the calibration of Fuji BAS-TR image plate (IP) response to high energy carbon ions of different charge states by employing an intense laser-driven ion source, which allowed access to carbon energies up to 270 MeV. The calibration method consists of employing a Thomson parabola spectrometer to separate and spectrally resolve different ion species, and a slotted CR-39 solid state detector overlayed onto an image plate for an absolute calibration of the IP signal. An empirical response function was obtained which can be reasonably extrapolated to higher ion energies. The experimental data also show that the IP response is independent of ion charge states.

Calibration of BAS-TR image plate response to high energy (3-300 MeV) carbon ions.

PubMed

Doria, D; Kar, S; Ahmed, H; Alejo, A; Fernandez, J; Cerchez, M; Gray, R J; Hanton, F; MacLellan, D A; McKenna, P; Najmudin, Z; Neely, D; Romagnani, L; Ruiz, J A; Sarri, G; Scullion, C; Streeter, M; Swantusch, M; Willi, O; Zepf, M; Borghesi, M

2015-12-01

The paper presents the calibration of Fuji BAS-TR image plate (IP) response to high energy carbon ions of different charge states by employing an intense laser-driven ion source, which allowed access to carbon energies up to 270 MeV. The calibration method consists of employing a Thomson parabola spectrometer to separate and spectrally resolve different ion species, and a slotted CR-39 solid state detector overlayed onto an image plate for an absolute calibration of the IP signal. An empirical response function was obtained which can be reasonably extrapolated to higher ion energies. The experimental data also show that the IP response is independent of ion charge states.

High Resolution PTR-TOFMS: A New Instrument for Organic Compound Measurements

NASA Astrophysics Data System (ADS)

Hansel, A.; Graus, M.; Mueller, M.; Wisthaler, A.

2007-12-01

Over the last decade proton transfer reaction mass spectrometry (PTR-MS) has become very popular in many scientific fields. PTR-MS allows for the quantitative detection of volatile organic compounds (VOCs) at pptv-level virtually in real time. Monitoring of VOCs with a time resolution of typically a second per compound has, for instance, enabled the tracking of pollution plumes by air-borne measurements, thus revealing the photo- chemical fate of pollutants. It has also been employed in direct eddy covariant flux measurements. This rapidity, however, has been achieved at the cost of the number of compounds to be analyzed and compound selectivity. Conventional PTR-MS can, for example, not distinguish between hydrocarbons and their oxygenated isobaric species, e.g. between naphthalene and octanal or between isoprene and furan. In a mass range up to 200 Dalton, such a task would require a mass resolving power of 5500. The use of a time of flight (TOF) instead of a quadrupole mass analyzer in PTR-MS provides a sufficient high mass resolution to identify the atomic composition of product ions by their exact mass and their characteristic isotope patterns. In addition PTR-TOF-MS can record full mass spectra within a fraction of a second which is a dramatically increase in duty cycle. At the University of Innsbruck a high resolution PTR-TOFMS has recently been developed, coupling a PTR-ion source and a high resolution TOFMS. We achieved a mass resolving power of 6000 (FWHM), and a detection limit of tens to a few hundreds of pptv if integrating mass spectra for one minute. First results and future directions will be discussed in this paper.

Simulation of plasma loading of high-pressure RF cavities

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yu, K.; Samulyak, R.; Yonehara, K.

2018-01-11

Muon beam-induced plasma loading of radio-frequency (RF) cavities filled with high pressure hydrogen gas with 1% dry air dopant has been studied via numerical simulations. The electromagnetic code SPACE, that resolves relevant atomic physics processes, including ionization by the muon beam, electron attachment to dopant molecules, and electron-ion and ion-ion recombination, has been used. Simulations studies have also been performed in the range of parameters typical for practical muon cooling channels.

Validation of nonlinear gyrokinetic simulations of L- and I-mode plasmas on Alcator C-Mod

DOE Office of Scientific and Technical Information (OSTI.GOV)

Creely, A. J.; Howard, N. T.; Rodriguez-Fernandez, P.

New validation of global, nonlinear, ion-scale gyrokinetic simulations (GYRO) is carried out for L- and I-mode plasmas on Alcator C-Mod, utilizing heat fluxes, profile stiffness, and temperature fluctuations. Previous work at C-Mod found that ITG/TEM-scale GYRO simulations can match both electron and ion heat fluxes within error bars in I-mode [White PoP 2015], suggesting that multi-scale (cross-scale coupling) effects [Howard PoP 2016] may be less important in I-mode than in L-mode. New results presented here, however, show that global, nonlinear, ion-scale GYRO simulations are able to match the experimental ion heat flux, but underpredict electron heat flux (at most radii),more » electron temperature fluctuations, and perturbative thermal diffusivity in both L- and I-mode. Linear addition of electron heat flux from electron scale runs does not resolve this discrepancy. These results indicate that single-scale simulations do not sufficiently describe the I-mode core transport, and that multi-scale (coupled electron- and ion-scale) transport models are needed. In conclusion a preliminary investigation with multi-scale TGLF, however, was unable to resolve the discrepancy between ion-scale GYRO and experimental electron heat fluxes and perturbative diffusivity, motivating further work with multi-scale GYRO simulations and a more comprehensive study with multi-scale TGLF.« less

Validation of nonlinear gyrokinetic simulations of L- and I-mode plasmas on Alcator C-Mod

DOE PAGES

Creely, A. J.; Howard, N. T.; Rodriguez-Fernandez, P.; ...

2017-03-02

New validation of global, nonlinear, ion-scale gyrokinetic simulations (GYRO) is carried out for L- and I-mode plasmas on Alcator C-Mod, utilizing heat fluxes, profile stiffness, and temperature fluctuations. Previous work at C-Mod found that ITG/TEM-scale GYRO simulations can match both electron and ion heat fluxes within error bars in I-mode [White PoP 2015], suggesting that multi-scale (cross-scale coupling) effects [Howard PoP 2016] may be less important in I-mode than in L-mode. New results presented here, however, show that global, nonlinear, ion-scale GYRO simulations are able to match the experimental ion heat flux, but underpredict electron heat flux (at most radii),more » electron temperature fluctuations, and perturbative thermal diffusivity in both L- and I-mode. Linear addition of electron heat flux from electron scale runs does not resolve this discrepancy. These results indicate that single-scale simulations do not sufficiently describe the I-mode core transport, and that multi-scale (coupled electron- and ion-scale) transport models are needed. In conclusion a preliminary investigation with multi-scale TGLF, however, was unable to resolve the discrepancy between ion-scale GYRO and experimental electron heat fluxes and perturbative diffusivity, motivating further work with multi-scale GYRO simulations and a more comprehensive study with multi-scale TGLF.« less

Short Intense Ion Pulses for Materials and Warm Dense Matter Research

NASA Astrophysics Data System (ADS)

Seidl, Peter; Ji, Q.; Lidia, S. M.; Persaud, A.; Stettler, M.; Takakuwa, J. H.; Waldron, W. L.; Schenkel, T.; Barnard, J. J.; Friedman, A.; Grote, D. P.; Davidson, R. C.; Gilson, E. P.; Kaganovich, I. D.

2015-11-01

We have commenced experiments with intense short pulses of ion beams on the Neutralized Drift Compression Experiment-II at Lawrence Berkeley National Laboratory, by generating beam spots size with radius r <1 mm within 2 ns FWHM and approximately 1010 ions/pulse. To enable the short pulse durations and mm-scale focal spot radii, the 1.2 MeV Li + ion beam is neutralized in a 1.6-meter drift compression section located after the last accelerator magnet. An 8-Tesla short focal length solenoid compresses the beam in the presence of the large volume plasma near the end of this section before the target. The scientific topics to be explored are warm dense matter, the dynamics of radiation damage in materials, and intense beam and beam-plasma physics including selected topics of relevance to the development of heavy-ion drivers for inertial fusion energy. We will describe the accelerator commissioning and time-resolved ionoluminescence measurements of yttrium aluminium perovskite using the fully integrated accelerator and neutralized drift compression components (arXiv:1506.05839). This work was supported by the Director, Office of Science, Office of Fusion Energy Sciences, of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

Formation, stability and dissociation dynamics of {{\\rm{N}}}_{2}{}^{{\\rm{n}}+} cations (n = 1 - 2) in 3.5 keV e - -N2 collisions studied using the energy resolved electron-ion coincidence technique

NASA Astrophysics Data System (ADS)

Kumar, S.; Prajapati, S.; Singh, B.; Singh, B. K.; Shanker, R.

2018-04-01

Coincidences between energy selected electrons and ions produced in the decay of a core hole ionized (excited) state in a free nitrogen molecule have been measured at three specified energies of emitted electrons to reveal the individual pathways produced in 3.5 keV electron-induced fragmentation processes. From these measurements, it has been possible to show, for the first time, that in addition to the normal Auger decay, the resonant Auger excitation channels also share their appreciable contributions in producing singly charged parent ions in an electron-induced collision system. The correlations between ion fragmentation products and electronic structures with a hole configuration in singly-, doubly- and possibly in triply charged molecular electronic states populated in the electronic decay of the initial core hole have been studied and discussed. KER values obtained from our experiments are found to be consistent with the previous results of photo absorption experiments for fragmentation channel {{{{N}}}2}2+ → N+ + N+ however, N2+ fragment ions are found to arise mainly from the fragmentation channel {{{{N}}}2}2+ → N2+ + N and to possess relatively low kinetic energies in the considered region of binding energies.

Plasma observations near jupiter: initial results from voyager 1.

PubMed

Bridge, H S; Belcher, J W; Lazarus, A J; Sullivan, J D; McNutt, R L; Bagenal, F; Scudder, J D; Sittler, E C; Siscoe, G L; Vasyliunas, V M; Goertz, C K; Yeates, C M

1979-06-01

Extensive measurements of low-energy positive ions and electrons were made throughout the Jupiter encounter of Voyager 1. The bow shock and magneto-pause were crossed several times at distances consistent with variations in the upstream solar wind pressure measured on Voyager 2. During the inbound pass, the number density increased by six orders of magnitude between the innermost magnetopause crossing at approximately 47 Jupiter radii and near closest approach at approximately 5 Jupiter radii; the plasma flow during this period was predominately in the direction of corotation. Marked increases in number density were observed twice per planetary rotation, near the magnetic equator. Jupiterward of the Io plasma torus, a cold, corotating plasma was observed and the energylcharge spectra show well-resolved, heavy-ion peaks at mass-to-charge ratios A/Z* = 8, 16, 32, and 64.

Plasma observations near Jupiter - Initial results from Voyager 1

NASA Technical Reports Server (NTRS)

Bridge, H. S.; Belcher, J. W.; Lazarus, A. J.; Sullivan, J. D.; Mcnutt, R. L.; Bagenal, F.; Scudder, J. D.; Sittler, E. C.; Siscoe, G. L.; Vasyliunas, V. M.

1979-01-01

Extensive measurements of low-energy positive ions and electrons were made throughout the Jupiter encounter of Voyager 1. The bow shock and magnetopause were crossed several times at distances consistent with variations in the upstream solar wind pressure measured on Voyager 2. During the inbound pass, the number density increased by six orders of magnitude between the innermost magnetopause crossing at approximately 47 Jupiter radii and near closest approach at approximately 5 Jupiter radii; the plasma flow during this period was predominately in the direction of corotation. Marked increases in number density were observed twice per planetary rotation, near the magnetic equator. Jupiterward of the Io plasma torus, a cold, corotating plasma was observed and the energy/charge spectra show well-resolved, heavy-ion peaks at mass-to-charge ratios equal to 8, 16, 32, and 64.

A neutron camera system for MAST.

PubMed

Cecconello, M; Turnyanskiy, M; Conroy, S; Ericsson, G; Ronchi, E; Sangaroon, S; Akers, R; Fitzgerald, I; Cullen, A; Weiszflog, M

2010-10-01

A prototype neutron camera has been developed and installed at MAST as part of a feasibility study for a multichord neutron camera system with the aim to measure the spatial and time resolved 2.45 MeV neutron emissivity profile. Liquid scintillators coupled to a fast digitizer are used for neutron/gamma ray digital pulse shape discrimination. The preliminary results obtained clearly show the capability of this diagnostic to measure neutron emissivity profiles with sufficient time resolution to study the effect of fast ion loss and redistribution due to magnetohydrodynamic activity. A minimum time resolution of 2 ms has been achieved with a modest 1.5 MW of neutral beam injection heating with a measured neutron count rate of a few 100 kHz.

Cluster Tool for In Situ Processing and Comprehensive Characterization of Thin Films at High Temperatures.

PubMed

Wenisch, Robert; Lungwitz, Frank; Hanf, Daniel; Heller, René; Zscharschuch, Jens; Hübner, René; von Borany, Johannes; Abrasonis, Gintautas; Gemming, Sibylle; Escobar-Galindo, Ramon; Krause, Matthias

2018-06-13

A new cluster tool for in situ real-time processing and depth-resolved compositional, structural and optical characterization of thin films at temperatures from -100 to 800 °C is described. The implemented techniques comprise magnetron sputtering, ion irradiation, Rutherford backscattering spectrometry, Raman spectroscopy, and spectroscopic ellipsometry. The capability of the cluster tool is demonstrated for a layer stack MgO/amorphous Si (∼60 nm)/Ag (∼30 nm), deposited at room temperature and crystallized with partial layer exchange by heating up to 650 °C. Its initial and final composition, stacking order, and structure were monitored in situ in real time and a reaction progress was defined as a function of time and temperature.

Charged particle space weathering rates at the Moon derived from ARTEMIS observations

NASA Astrophysics Data System (ADS)

Poppe, A. R.; Farrell, W. M.; Halekas, J. S.

2017-12-01

The weathering of airless bodies exposed to space is a fundamental process in the formation and evolution of planetary surfaces. At the Moon, space weathering induces a variety of physical, chemical, and optical changes including the formation of nanometer sized amorphous rims on individual lunar grains. These rims are formed by vapor redeposition from micrometeoroid impacts and ion irradiation-induced amorphization of the crystalline matrix. For ion irradiation-induced rims, however, laboratory experiments of the depth and formation timescales of these rims stand in stark disagreement with observations of lunar soil grains. We use observations by the ARTEMIS spacecraft in orbit around the Moon to compute the mean ion flux to the lunar surface and convolve this flux with ion irradiation-induced vacancy production rates calculated using the Stopping Range of Ions in Matter (SRIM) model. From this, we calculate the formation timescales for amorphous rim production as a function of depth and compare to laboratory experiments and observations of lunar soil. Our analysis resolves two outstanding issues: (1) the provenance of >100 nm amorphous rims on lunar grains and (2) the nature of the depth-age relationship for amorphous rims on lunar grains. We also present the hypothesis that ion beam-induced epitaxial crystallization is responsible for the discrepancy between observational and experimental results of the formation time of <100 nm amorphous rims.

Langmuir probe measurements and mass spectrometry of plasma plumes generated by laser ablation of La0.4Ca0.6MnO3

NASA Astrophysics Data System (ADS)

Chen, Jikun; Lunney, James G.; Lippert, Thomas; Ojeda-G-P, Alejandro; Stender, Dieter; Schneider, Christof W.; Wokaun, Alexander

2014-08-01

The plasma formed in vacuum by UV nanosecond laser ablation of La0.4Ca0.6MnO3 in the fluence range of 0.8 to 1.9 J cm-2 using both Langmuir probe analysis and energy-resolved mass spectrometry has been studied. Mass spectrometry shows that the main positive ion species are Ca+, Mn+, La+, and LaO+. The Ca+ and Mn+ energy distributions are quite broad and lie in the 0-100 eV region, with the average energies increasing with laser fluence. In contrast, the La+ and LaO+ distributions are strongly peaked around 10 eV. The net time-of-arrival signal derived from the measured positive ion energy distributions is broadly consistent with the positive ion signal measured by the Langmuir probe. We also detected a significant number of O- ions with energies in the range of 0 to 10 eV. The Langmuir probe was also used to measure the temporal variation of the electron density and temperature at 6 cm from the ablation target. In the period when O- ions are found at this position, the plasma conditions are consistent with those required for significant negative oxygen ion formation, as revealed by studies on radio frequency excited oxygen plasma.

Submicrometer Emitter ESI Tips for Native Mass Spectrometry of Membrane Proteins in Ionic and Nonionic Detergents

NASA Astrophysics Data System (ADS)

Susa, Anna C.; Lippens, Jennifer L.; Xia, Zijie; Loo, Joseph A.; Campuzano, Iain D. G.; Williams, Evan R.

2018-01-01

Native mass spectrometry (native-MS) of membrane proteins typically requires a detergent screening protocol, protein solubilization in the preferred detergent, followed by protein liberation from the micelle by collisional activation. Here, submicrometer nano-ESI emitter tips are used for native-MS of membrane proteins solubilized in both nonionic and ionic detergent solutions. With the submicrometer nano-ESI emitter tips, resolved charge-state distributions of membrane protein ions are obtained from a 150 mM NaCl, 25 mM Tris-HCl with 1.1% octyl glucoside solution. The relative abundances of NaCl and detergent cluster ions at high m / z are significantly reduced with the submicrometer emitters compared with larger nano-ESI emitters that are commonly used. This technique is beneficial for significantly decreasing the abundances (by two to three orders of magnitude compared with the larger tip size: 1.6 μm) of detergent cluster ions formed from aqueous ammonium acetate solutions containing detergents that can overlap with the membrane protein ion signal. Resolved charge-state distributions of membrane protein ions from aqueous ammonium acetate solutions containing ionic detergents were obtained with the submicrometer nano-ESI emitters; this is the first report of native-MS of membrane proteins solubilized by ionic detergents. [Figure not available: see fulltext.

Submicrometer Emitter ESI Tips for Native Mass Spectrometry of Membrane Proteins in Ionic and Nonionic Detergents.

PubMed

Susa, Anna C; Lippens, Jennifer L; Xia, Zijie; Loo, Joseph A; Campuzano, Iain D G; Williams, Evan R

2018-01-01

Native mass spectrometry (native-MS) of membrane proteins typically requires a detergent screening protocol, protein solubilization in the preferred detergent, followed by protein liberation from the micelle by collisional activation. Here, submicrometer nano-ESI emitter tips are used for native-MS of membrane proteins solubilized in both nonionic and ionic detergent solutions. With the submicrometer nano-ESI emitter tips, resolved charge-state distributions of membrane protein ions are obtained from a 150 mM NaCl, 25 mM Tris-HCl with 1.1% octyl glucoside solution. The relative abundances of NaCl and detergent cluster ions at high m /z are significantly reduced with the submicrometer emitters compared with larger nano-ESI emitters that are commonly used. This technique is beneficial for significantly decreasing the abundances (by two to three orders of magnitude compared with the larger tip size: 1.6 μm) of detergent cluster ions formed from aqueous ammonium acetate solutions containing detergents that can overlap with the membrane protein ion signal. Resolved charge-state distributions of membrane protein ions from aqueous ammonium acetate solutions containing ionic detergents were obtained with the submicrometer nano-ESI emitters; this is the first report of native-MS of membrane proteins solubilized by ionic detergents. Graphical Abstract.

Time-resolved X-ray Absorption Spectroscopy for Electron Transport Study in Warm Dense Gold

NASA Astrophysics Data System (ADS)

Lee, Jong-Won; Bae, Leejin; Engelhorn, Kyle; Heimann, Philip; Ping, Yuan; Barbrel, Ben; Fernandez, Amalia; Beckwith, Martha Anne; Cho, Byoung-Ick; GIST Team; IBS Team; LBNL Collaboration; SLAC Collaboration; LLNL Collaboration

2015-11-01

The warm dense Matter represents states of which the temperature is comparable to Fermi energy and ions are strongly coupled. One of the experimental techniques to create such state in the laboratory condition is the isochoric heating of thin metal foil with femtosecond laser pulses. This concept largely relies on the ballistic transport of electrons near the Fermi-level, which were mainly studied for the metals in ambient conditions. However, they were barely investigated in warm dense conditions. We present a time-resolved x-ray absorption spectroscopy measured for the Au/Cu dual layered sample. The front Au layer was isochorically heated with a femtosecond laser pulse, and the x-ray absorption changes around L-edge of Cu, which was attached on the backside of Au, was measured with a picosecond resolution. Time delays between the heating of the `front surface' of Au layer and the alternation of x-ray spectrum of Cu attached on the `rear surface' of Au indicate the energetic electron transport mechanism through Au in the warm dense conditions. IBS (IBS-R012-D1) and the NRF (No. 2013R1A1A1007084) of Korea.

Ion heating and flows in a high power helicon source

NASA Astrophysics Data System (ADS)

Thompson, Derek S.; Agnello, Riccardo; Furno, Ivo; Howling, Alan; Jacquier, Rémy; Plyushchev, Gennady; Scime, Earl E.

2017-06-01

We report experimental measurements of ion temperatures and flows in a high power, linear, magnetized, helicon plasma device, the Resonant Antenna Ion Device (RAID). Parallel and perpendicular ion temperatures on the order of 0.6 eV are observed for an rf power of 4 kW, suggesting that higher power helicon sources should attain ion temperatures in excess of 1 eV. The unique RAID antenna design produces broad, uniform plasma density and perpendicular ion temperature radial profiles. Measurements of the azimuthal flow indicate rigid body rotation of the plasma column of a few kHz. When configured with an expanding magnetic field, modest parallel ion flows are observed in the expansion region. The ion flows and temperatures are derived from laser induced fluorescence measurements of the Doppler resolved velocity distribution functions of argon ions.

Electron-impact-ionization dynamics of S F6

NASA Astrophysics Data System (ADS)

Bull, James N.; Lee, Jason W. L.; Vallance, Claire

2017-10-01

A detailed understanding of the dissociative electron ionization dynamics of S F6 is important in the modeling and tuning of dry-etching plasmas used in the semiconductor manufacture industry. This paper reports a crossed-beam electron ionization velocity-map imaging study on the dissociative ionization of cold S F6 molecules, providing complete, unbiased kinetic energy distributions for all significant product ions. Analysis of these distributions suggests that fragmentation following single ionization proceeds via formation of S F5 + or S F3 + ions that then dissociate in a statistical manner through loss of F atoms or F2, until most internal energy has been liberated. Similarly, formation of stable dications is consistent with initial formation of S F4 2 + ions, which then dissociate on a longer time scale. These data allow a comparison between electron ionization and photoionization dynamics, revealing similar dynamical behavior. In parallel with the ion kinetic energy distributions, the velocity-map imaging approach provides a set of partial ionization cross sections for all detected ionic fragments over an electron energy range of 50-100 eV, providing partial cross sections for S2 +, and enables the cross sections for S F4 2 + from S F+ to be resolved.

Material quality frontiers of MOVPE grown AlGaAs for minority carrier devices

NASA Astrophysics Data System (ADS)

Heckelmann, S.; Lackner, D.; Dimroth, F.; Bett, A. W.

2017-04-01

In this study, secondary ion mass spectroscopy of oxygen, deep level transient spectroscopy and power dependent relative photoluminescence are compared regarding their ability to resolve differences in AlxGa1-xAs material quality. AlxGa1-xAs samples grown with two different trimethylaluminum sources showing low and high levels of oxygen contamination are compared. As tested in the growth of minority carrier devices, i.e. AlxGa1-xAs solar cells, the two precursors clearly lead to different device characteristics. It is shown that secondary ion mass spectroscopy could not resolve the difference in oxygen concentration, whereas deep level transient spectroscopy and photoluminescence based measurements indicate the influence of the precursor oxygen level on the material quality.

Jet-resolved vibronic structure in the higher excited states of N2O - Ultraviolet three-photon absorption spectroscopy from 80,000 to 90,000/cm

NASA Technical Reports Server (NTRS)

Patsilinakou, E.; Wiedmann, R. T.; Fotakis, C.; Grant, E. R.

1989-01-01

Ionization-detected UV multiphoton absorption spectroscopy of the excited states of N2O is presented, showing Rydberg structure within 20,000/cm of the first ionization threshold. Despite evidence for strong Rydberg-continuum coupling in the form of broadened bands and Fano line-shapes, the Rydberg structure persists, with atomic-like quantum defects and vibration structure well-matched with that of the ion. In the most clearly resolved spectrum, corresponding to the 3p(delta)1Pi state, Renner-Teller and Herzberg-Teller coupling of electronic and vibrational angular momentum are revealed. It is suggested that these mixings are properties of the N2O(+)Pi ion core.

High-Definition Differential Ion Mobility Spectrometry with Resolving Power up to 500

PubMed Central

Shvartsburg, Alexandre A.; Seim, Tom A.; Danielson, William F.; Norheim, Randy; Moore, Ronald J.; Anderson, Gordon A.; Smith, Richard D.

2013-01-01

As the resolution of analytical methods improves, further progress tends to be increasingly limited by instrumental parameter instabilities that could be ignored before. This is now the case with differential ion mobility spectrometry (FAIMS), where fluctuations of the voltages and gas pressure have become critical. A new high-definition generator for FAIMS compensation voltage reported here provides a stable and accurate output than can be scanned with negligible steps. This reduces the spectral drift and peak width, thus improving the resolving power (R) and resolution. The gain for multiply-charged peptides that have narrowest peaks is up to ~40%, and R ~ 400 – 500 is achievable using He/N2 or H2/N2 gas mixtures. PMID:23345059

High-Definition Differential Ion Mobility Spectrometry with Resolving Power up to 500

DOE Office of Scientific and Technical Information (OSTI.GOV)

Shvartsburg, Alexandre A.; Seim, Thomas A.; Danielson, William F.

2013-01-20

As the resolution of analytical methods improve, further progress tends to be increasingly limited by instrumental parameter instabilities that could be ignored before. This is now the case with differential ion mobility spectrometry (FAIMS), where fluctuations of the voltages and gas pressure have become critical. A new high-definition generator for FAIMS compensation voltage reported here provides a stable and accurate output than can be scanned with negligible steps. This reduces the spectral drift and peak width, thus improving the resolving power (R) and resolution. The gain for multiply-charged peptides that have narrowest peaks is up to ~40%, and R ~more » 400 - 500 is achievable using He/N2 or H2/N2 gas mixtures.« less

Time-resolved optical emission spectroscopic studies of picosecond laser produced Cr plasma

NASA Astrophysics Data System (ADS)

Rao, Kavya H.; Smijesh, N.; Klemke, N.; Philip, R.; Litvinyuk, I. V.; Sang, R. T.

2018-06-01

Time-resolved optical emission spectroscopic measurements of a plasma generated by irradiating a Cr target using 60 picosecond (ps) and 300 ps laser pulses are carried out to investigate the variation in the line width (δλ) of emission from neutrals and ions for increasing ambient pressures. Measurements ranging from 10-6 Torr to 102 Torr show a distinctly different variation in the δλ of neutrals (Cr I) compared to that of singly ionized Cr (Cr II), for both irradiations. δλ increases monotonously with pressure for Cr II, but an oscillation is evident at intermediate pressures for Cr I. This oscillation does not depend on the laser pulse widths used. In spite of the differences in the plasma formation mechanisms, it is experimentally found that there is an optimum intermediate background pressure for which δλ of neutrals drops to a minimum. Importantly, these results underline the fact that for intermediate pressures, the usual practice of calculating the plasma number density from the δλ of neutrals needs to be judiciously done, to avoid reaching inaccurate conclusions.

Capturing Structural Snapshots during Photochemical Reactions with Ultrafast Raman Spectroscopy: From Materials Transformation to Biosensor Responses.

PubMed

Fang, Chong; Tang, Longteng; Oscar, Breland G; Chen, Cheng

2018-06-21

Chemistry studies the composition, structure, properties, and transformation of matter. A mechanistic understanding of the pertinent processes is required to translate fundamental knowledge into practical applications. The current development of ultrafast Raman as a powerful time-resolved vibrational technique, particularly femtosecond stimulated Raman spectroscopy (FSRS), has shed light on the structure-energy-function relationships of various photosensitive systems. This Perspective reviews recent work incorporating optical innovations, including the broad-band up-converted multicolor array (BUMA) into a tunable FSRS setup, and demonstrates its resolving power to watch metal speciation and photolysis, leading to high-quality thin films, and fluorescence modulation of chimeric protein biosensors for calcium ion imaging. We discuss advantages of performing FSRS in the mixed time-frequency domain and present strategies to delineate mechanisms by tracking low-frequency modes and systematically modifying chemical structures with specific functional groups. These unique insights at the chemical-bond level have started to enable the rational design and precise control of functional molecular machines in optical, materials, energy, and life sciences.

Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy.

PubMed

Chatterley, Adam S; Lackner, Florian; Neumark, Daniel M; Leone, Stephen R; Gessner, Oliver

2016-06-07

Using femtosecond time-resolved extreme ultraviolet absorption spectroscopy, the dissociation dynamics of the haloalkane 1,2-dibromoethane (DBE) have been explored following strong field ionization by femtosecond near infrared pulses at intensities between 7.5 × 10(13) and 2.2 × 10(14) W cm(-2). The major elimination products are bromine atoms in charge states of 0, +1, and +2. The charge state distribution is strongly dependent on the incident NIR intensity. While the yield of neutral fragments is essentially constant for all measurements, charged fragment yields grow rapidly with increasing NIR intensities with the most pronounced effect observed for Br(++). However, the appearance times of all bromine fragments are independent of the incident field strength; these are found to be 320 fs, 70 fs, and 30 fs for Br˙, Br(+), and Br(++), respectively. Transient molecular ion features assigned to DBE(+) and DBE(++) are observed, with dynamics linked to the production of Br(+) products. Neutral Br˙ atoms are produced on a timescale consistent with dissociation of DBE(+) ions on a shallow potential energy surface. The appearance of Br(+) ions by dissociative ionization is also seen, as evidenced by the simultaneous decay of a DBE(+) ionic species. Dicationic Br(++) products emerge within the instrument response time, presumably from Coulomb explosion of triply charged DBE.

Tracking dissociation dynamics of strong-field ionized 1,2-dibromoethane with femtosecond XUV transient absorption spectroscopy

DOE PAGES

Chatterley, Adam S.; Lackner, Florian; Neumark, Daniel M.; ...

2016-05-11

Using femtosecond time-resolved extreme ultraviolet absorption spectroscopy, the dissociation dynamics of the haloalkane 1,2-dibromoethane (DBE) have been explored following strong field ionization by femtosecond near infrared pulses at intensities between 7.5 × 10 13 and 2.2 × 10 14 W cm -2. The major elimination products are bromine atoms in charge states of 0, +1, and +2. The charge state distribution is strongly dependent on the incident NIR intensity. While the yield of neutral fragments is essentially constant for all measurements, charged fragment yields grow rapidly with increasing NIR intensities with the most pronounced effect observed for Br ++. However,more » the appearance times of all bromine fragments are independent of the incident field strength; these are found to be 320 fs, 70 fs, and 30 fs for Br˙, Br +, and Br ++, respectively. Transient molecular ion features assigned to DBE + and DBE ++ are observed, with dynamics linked to the production of Br + products. Neutral Br˙ atoms are produced on a timescale consistent with dissociation of DBE + ions on a shallow potential energy surface. The appearance of Br + ions by dissociative ionization is also seen, as evidenced by the simultaneous decay of a DBE + ionic species. Dicationic Br ++ products emerge within the instrument response time, presumably from Coulomb explosion of triply charged DBE.« less

ExoCube INMS with Neutral Hydrogen Mode

NASA Astrophysics Data System (ADS)

Jones, S.; Paschalidis, N.; Rodriguez, M.; Sittler, E. C., Jr.; Chornay, D. J.; Cameron, T.; Uribe, P.; Nanan, G.; Noto, J.; Waldrop, L.; Mierkiewicz, E. J.; Gardner, D.; Nossal, S. M.; Puig-Suari, J.; Bellardo, J.

2015-12-01

The ExoCube mission launched on Jan 31 2015 into a polar orbit to acquire global knowledge of in situ densities of neutral and ionized H, He, and O in the upper ionosphere and lower exosphere. The CubeSat platform is used in combination with incoherent scatter radar and optical ground stations distributed throughout the Americas. ExoCube seeks to obtain the first in situ measurement of neutral exospheric hydrogen and will measure in situ atomic oxygen for the first time in decades. The compact Ion and Neutral Mass Spectrometer (INMS) developed by GSFC uses the gated Time of Flight technique for in situ measurements of ions and neutrals (H, He, N, O, N2, O2) with M/dM of approximately 10. The compact sensor has a dual symmetric configuration with ion and neutral sensor heads. Neutral particles are ionized by electron impact using a thermionic emitter. In situ measurements of neutral hydrogen are notoriously difficult as historically the signal has been contaminated by hydrogen outgassing which persists even years after commissioning. In order to obtain neutral atmospheric hydrogen fluxes, either the atmospheric peak and outgassing peak must be well resolved, or the outgassing component subtracted off. The ExoCube INMS employs a separate mode, specifically for measuring neutral Hydrogen. The details of this mode and lessons learned will be presented as well as in flight instrument validation data for the neutral channel and preliminary flight ion spectra. At the time of abstract submission, the ExoCube spacecraft is currently undergoing attitude control maneuvers to orient INMS in the ram direction for science operations.

Secondary Structures of Ubiquitin Ions Soft-Landed onto Self-Assembled Monolayer Surfaces

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hu, Qichi; Laskin, Julia

2016-06-09

The secondary structures of multiply charged ubiquitin ions soft-landed onto self-assembled monolayer (SAM) surfaces were studied using in situ infrared reflection-absorption spectroscopy (IRRAS). Two charge states of ubiquitin, 5+ and 13+, were mass selected separately from a mixture of different charge states produced by electrospray ionization (ESI). The low 5+ charge state represents a native-like folded state of ubiquitin, while the high 13+ charge state assumes an extended, almost linear conformation. Each of the two charge states was soft-landed onto a CH 3- and COOH-terminated SAM of alkylthiols on gold (HSAM and COOH-SAM). HSAM is a hydrophobic surface known tomore » stabilize helical conformations of soft-landed protonated peptides, whereas COOH-SAM is a hydrophilic surface that preferentially stabilizes β-sheet conformations. IRRAS spectra of the soft-landed ubiquitin ions were acquired as a function of time during and after ion soft-landing. Similar to smaller peptide ions, helical conformations of ubiquitin are found to be more abundant on HSAM, while the relative abundance of β-sheet conformations increases on COOH-SAM. The initial charge state of ubiquitin also has a pronounced effect on its conformation on the surface. Specifically, on both surfaces, a higher relative abundance of helical conformations and lower relative abundance of β-sheet conformations is observed for the 13+ charge state compared to the 5+ charge state. Time-resolved experiments indicate that the α-helical band in the spectrum of the 13+ charge state slowly increases with time on the HSAM surface and decreases in the spectrum of the 13+ charge state on COOH-SAM. These results further support the preference of the hydrophobic HSAM surface toward helical conformations and demonstrate that soft-landed protein ions may undergo slow conformational changes during and after deposition.« less

Spin Polarization Transfer from a Photogenerated Radical Ion Pair to a Stable Radical Controlled by Charge Recombination.

PubMed

Horwitz, Noah E; Phelan, Brian T; Nelson, Jordan N; Mauck, Catherine M; Krzyaniak, Matthew D; Wasielewski, Michael R

2017-06-15

Photoexcitation of electron donor-acceptor molecules frequently produces radical ion pairs with well-defined initial spin-polarized states that have attracted significant interest for spintronics. Transfer of this initial spin polarization to a stable radical is predicted to depend on the rates of the radical ion pair recombination reactions, but this prediction has not been tested experimentally. In this study, a stable radical/electron donor/chromophore/electron acceptor molecule, BDPA • -mPD-ANI-NDI, where BDPA • is α,γ-bisdiphenylene-β-phenylallyl, mPD is m-phenylenediamine, ANI is 4-aminonaphthalene-1,8-dicarboximide, and NDI is naphthalene-1,4:5,8-bis(dicarboximide), was synthesized. Photoexcitation of ANI produces the triradical BDPA • -mPD +• -ANI-NDI -• in which the mPD +• -ANI-NDI -• radical ion pair is spin coupled to the BDPA • stable radical. BDPA • -mPD +• -ANI-NDI -• and its counterpart lacking the stable radical are found to exhibit spin-selective charge recombination in which the triplet radical ion pair 3 (mPD +• -ANI-NDI -• ) is in equilibrium with the 3 *NDI charge recombination product. Time-resolved EPR measurements show that this process is associated with an inversion of the sign of the polarization transferred to BDPA • over time. The polarization transfer rates are found to be strongly solvent dependent, as shifts in this equilibrium affect the spin dynamics. These results demonstrate that even small changes in electron transfer dynamics can have a large effect on the spin dynamics of photogenerated multispin systems.

Gas Chromatography/Atmospheric Pressure Chemical Ionization-Fourier Transform Ion Cyclotron Resonance Mass Spectrometry of Pyrolysis Oil from German Brown Coal

PubMed Central

Zuber, Jan; Kroll, Marius M.; Rathsack, Philipp; Otto, Matthias

2016-01-01

Pyrolysis oil from the slow pyrolysis of German brown coal from Schöningen, obtained at a temperature of 500°C, was separated and analyzed using hyphenation of gas chromatography with an atmospheric pressure chemical ionization source operated in negative ion mode and Fourier transform ion cyclotron resonance mass spectrometry (GC-APCI-FT-ICR-MS). Development of this ultrahigh-resolving analysis method is described, that is, optimization of specific GC and APCI parameters and performed data processing. The advantages of GC-APCI-FT-ICR-MS hyphenation, for example, soft ionization, ultrahigh-resolving detection, and most important isomer separation, were demonstrated for the sample liquid. For instance, it was possible to separate and identify nine different propylphenol, ethylmethylphenol, and trimethylphenol isomers. Furthermore, homologous series of different acids, for example, alkyl and alkylene carboxylic acids, were verified, as well as homologous series of alkyl phenols, alkyl dihydroxy benzenes, and alkoxy alkyl phenols. PMID:27066076

Resolving the Small-Scale Structure of the Circumgalactic Medium in Cosmological Simulations

NASA Astrophysics Data System (ADS)

Corlies, Lauren

2017-08-01

We propose to resolve the circumgalactic medium (CGM) of L* galaxies down to 100 Msun (250 pc) in a full cosmological simulation to examine how mixing and cooling shape the physical nature of this gas on the scales expected from observations. COS has provided the best characterization of the low-z CGM to date, revealing the extent and amount of low- and high-ions and hinting at the kinematic relations between them. Yet cosmological galaxy simulations that can reproduce the stellar properties of galaxies have all struggled to reproduce these results even qualitatively. However, while the COS data imply that the low-ion absorption is occurring on sub-kpc scales, such scales can not be traced by simulations with resolution between 1-5 kpc in the CGM. Our proposed simulations will, for the first time, reach the resolution required to resolve these structures in the outer halo of L* galaxies. Using the adaptive mesh refinement code enzo, we will experiment with the size, shape, and resolution of an enforced high refinement region extending from the disk into the CGM to identify the best configuration for probing the flows of gas throughout the CGM. Our test case has found that increasing the resolution alone can have dramatic consequences for the density, temperature, and kinematics along a line of sight. Coupling this technique with an independent feedback study already underway will help disentangle the roles of global and small scale physics in setting the physical state of the CGM. Finally, we will use the MISTY pipeline to generate realistic mock spectra for direct comparison with COS data which will be made available through MAST.

Continuous-flow liquid microjunction surface sampling probe connected on-line with high-performance liquid chromatography/mass spectrometry for spatially resolved analysis of small molecules and proteins.

PubMed

Van Berkel, Gary J; Kertesz, Vilmos

2013-06-30

A continuous-flow liquid microjunction surface sampling probe extracts soluble material from surfaces for direct ionization and detection by mass spectrometry. Demonstrated here is the on-line coupling of such a probe with high-performance liquid chromatography/mass spectrometry (HPLC/MS) enabling extraction, separation and detection of small molecules and proteins from surfaces in a spatially resolved (~0.5 mm diameter spots) manner. A continuous-flow liquid microjunction surface sampling probe was connected to a six-port, two-position valve for extract collection and injection to an HPLC column. A QTRAP® 5500 hybrid triple quadrupole linear ion trap equipped with a Turbo V™ ion source operated in positive electrospray ionization (ESI) mode was used for all experiments. The system operation was tested with the extraction, separation and detection of propranolol and associated metabolites from drug dosed tissues, caffeine from a coffee bean, cocaine from paper currency, and proteins from dried sheep blood spots on paper. Confirmed in the tissue were the parent drug and two different hydroxypropranolol glucuronides. The mass spectrometric response for these compounds from different locations in the liver showed an increase with increasing extraction time (5, 20 and 40 s). For on-line separation and detection/identification of extracted proteins from dried sheep blood spots, two major protein peaks dominated the chromatogram and could be correlated with the expected masses for the hemoglobin α and β chains. Spatially resolved sampling, separation, and detection of small molecules and proteins from surfaces can be accomplished using a continuous-flow liquid microjunction surface sampling probe coupled on-line with HPLC/MS detection. Published in 2013. This article is a U.S. Government work and is in the public domain in the USA.

Blackbody infrared radiative dissociation of protonated oligosaccharides.

PubMed

Fentabil, Messele A; Daneshfar, Rambod; Kitova, Elena N; Klassen, John S

2011-12-01

The dissociation pathways, kinetics, and energetics of protonated oligosaccharides in the gas phase were investigated using blackbody infrared radiative dissociation (BIRD). Time-resolved BIRD measurements were performed on singly protonated ions of cellohexaose (Cel(6)), which is composed of β-(1→4)-linked glucopyranose rings, and five malto-oligosaccharides (Mal(x), where x=4-8), which are composed of α-(1→4)-linked glucopyranose units. At the temperatures investigated (85-160 °C), the oligosaccharides dissociate at the glycosidic linkages or by the loss of a water molecule to produce B- or Y-type ions. The Y ions dissociate to smaller Y or B ions, while the B ions yield exclusively smaller B ions. The sequential loss of water molecules from the smallest B ions (B(1) and B(2)) also occurs. Rate constants for dissociation of the protonated oligosaccharides and the corresponding Arrhenius activation parameters (E(a) and A) were determined. The E(a) and A-factors measured for protonated Mal(x) (x>4) are indistinguishable within error (~19 kcal mol(-1), 10(10) s(-1)), which is consistent with the ions being in the rapid energy exchange limit. In contrast, the Arrhenius parameters for protonated Cel(6) (24 kcal mol(-1), 10(12) s(-1)) are significantly larger. These results indicate that both the energy and entropy changes associated with the glycosidic bond cleavage are sensitive to the anomeric configuration. Based on the results of this study, it is proposed that formation of B and Y ions occurs through a common dissociation mechanism, with the position of the proton establishing whether a B or Y ion is formed upon glycosidic bond cleavage. © American Society for Mass Spectrometry, 2011

Structural investigation of new vanadium-bismuth-phosphate glasses by IR and ESR spectroscopy

NASA Astrophysics Data System (ADS)

Vedeanu, N.; Cozar, O.; Stanescu, R.; Cozar, I. B.; Ardelean, I.

2013-07-01

IR spectra changes of the xV2O5(1 - x)[0.8P2O5ṡ0.2Bi2O3] glass system with 0 ⩽ x ⩽ 50 mol% show that vanadium oxide acts as a network modifier at low concentration (x ⩽ 5 mol%), affecting especially the Bi2O3 network. In the same time the phosphate groups (structures) impose their presence by themselves, fact which is illustrated by the increasing of the intensity of characteristic 910, 1040, 1230 cm-1 bands. The IR bands belonging to the phosphate groups are strongly reduced for x ⩾ 10 mol% due to the phosphate network depolymerization and to the appearance of new vibrations characteristic for POV and VOV linkages, showing the network former role of V2O5. In the same time the changes observed in the ESR spectra of these glasses are explained supposing the superposition of two signals, one with a well-resolved hyperfine structure typical for isolated V4+ ions and a broad line characteristic for clustered ions. The line width dependence versus V2O5 content shows that dipole-dipole interactions exist between vanadium ions until x = 5 mol% and the superexchange interactions prevail at high content (x ⩾ 10 mol%).

Latitudinal distribution of the Jovian plasma sheet ions observed by Juno JADE-I

NASA Astrophysics Data System (ADS)

Kim, T. K. H.; Valek, P. W.; McComas, D. J.; Allegrini, F.; Bagenal, F.; Bolton, S. J.; Connerney, J. E. P.; Ebert, R. W.; Levin, S.; Louarn, P.; Pollock, C. J.; Ranquist, D. A.; Szalay, J.; Thomsen, M. F.; Wilson, R. J.

2017-12-01

The Jovian plasma sheet is a region where the centrifugal force dominates the heavy ion plasma. Properties of the plasma sheet ions near the equatorial plane have been studied with in-situ measurements from the Pioneer, Voyager, and Galileo spacecraft. However, the ion properties for the off-equator regions are not well known due to the limited measurements. Juno is the first polar orbiting spacecraft that can investigate the high latitude region of the Jovian magnetosphere. With Juno's unique trajectory, we will investigate the latitudinal distribution of the Jovian plasma sheet ions using measurements from the Jovian Auroral Distributions Experiment Ion sensor (JADE-I). JADE-I measures an ion's energy-per-charge (E/Q) from 0.01 keV/q to 46.2 keV/q with an electrostatic analyzer (ESA) and a mass-per-charge (M/Q) up to 64 amu/q with a carbon-foil-based time-of-flight (TOF) mass spectrometer. We have shown that the ambiguity between and (both have M/Q of 16) can be resolved in JADE-I using a semi-empirical simulation tool based on carbon foil effects (i.e., charge state modification, angular scattering, and energy loss) from incident ions passing through the TOF mass spectrometer. Based on the simulation results, we have developed an Ion Composition Analysis Tool (ICAT) that determines ion composition at each energy step of JADE-I (total of 64 steps). The velocity distribution for each ion species can be obtained from the ion composition as a function of each energy step. Since there is an ambipolar electric field due to mobile electrons and equatorially confined heavy ions, we expect to see acceleration along the field line. This study will show the species separated velocity distribution at various latitudes to investigate how the plasma sheet ions evolve along the field line.

Counting individual sulfur atoms in a protein by ultrahighresolution Fourier transform ion cyclotron resonance mass spectrometry: Experimental resolution of isotopic fine structure in proteins

PubMed Central

Shi, Stone D.-H.; Hendrickson, Christopher L.; Marshall, Alan G.

1998-01-01

A typical molecular ion mass spectrum consists of a sum of signals from species of various possible isotopic compositions. Only the monoisotopic peak (e.g., all carbons are 12C; all nitrogens are 14N, etc.) has a unique elemental composition. Every other isotope peak at approximately integer multiples of ∼1 Da higher in nominal mass represents a sum of contributions from isotope combinations differing by a few mDa (e.g., two 13C vs. two 15N vs. one 13C and one 15N vs. 34S, vs. 18O, etc., at ∼2 Da higher in mass than the monoisotopic mass). At sufficiently high mass resolving power, each of these nominal-mass peaks resolves into its isotopic fine structure. Here, we report resolution of the isotopic fine structure of proteins up to 15.8 kDa (isotopic 13C,15N doubly depleted tumor suppressor protein, p16), made possible by electrospray ionization followed by ultrahigh-resolution Fourier transform ion cyclotron resonance mass analysis at 9.4 tesla. Further, a resolving power of m/Δm50% ≈8,000,000 has been achieved on bovine ubiquitin (8.6 kDa). These results represent a 10-fold increase in the highest mass at which isotopic fine structure previously had been observed. Finally, because isotopic fine structure reveals elemental composition directly, it can be used to confirm or determine molecular formula. For p16, for example, we were able to determine (5.1 ± 0.3) the correct number (five) of sulfur atoms solely from the abundance ratio of the resolved 34S peak to the monoisotopic peak. PMID:9751700

Shutterless ion mobility spectrometer with fast pulsed electron source

NASA Astrophysics Data System (ADS)

Bunert, E.; Heptner, A.; Reinecke, T.; Kirk, A. T.; Zimmermann, S.

2017-02-01

Ion mobility spectrometers (IMS) are devices for fast and very sensitive trace gas analysis. The measuring principle is based on an initial ionization process of the target analyte. Most IMS employ radioactive electron sources, such as 63Ni or 3H. These radioactive materials have the disadvantage of legal restrictions and the electron emission has a predetermined intensity and cannot be controlled or disabled. In this work, we replaced the 3H source of our IMS with 100 mm drift tube length with our nonradioactive electron source, which generates comparable spectra to the 3H source. An advantage of our emission current controlled nonradioactive electron source is that it can operate in a fast pulsed mode with high electron intensities. By optimizing the geometric parameters and developing fast control electronics, we can achieve very short electron emission pulses for ionization with high intensities and an adjustable pulse width of down to a few nanoseconds. This results in small ion packets at simultaneously high ion densities, which are subsequently separated in the drift tube. Normally, the required small ion packet is generated by a complex ion shutter mechanism. By omitting the additional reaction chamber, the ion packet can be generated directly at the beginning of the drift tube by our pulsed nonradioactive electron source with only slight reduction in resolving power. Thus, the complex and costly shutter mechanism and its electronics can also be omitted, which leads to a simple low-cost IMS-system with a pulsed nonradioactive electron source and a resolving power of 90.

High pressure effects in high-field asymmetric waveform ion mobility spectrometry.

PubMed

Wang, Yonghuan; Wang, Xiaozhi; Li, Lingfen; Chen, Chilai; Xu, Tianbai; Wang, Tao; Luo, Jikui

2016-08-30

High-Field Asymmetric Waveform Ion Mobility Spectrometry (FAIMS) is an analytical technique based on the principle of non-linear electric field dependence of coefficient of mobility of ions for separation that was originally conceived in the Soviet Union in the early 1980s. Being well developed over the past decades, FAIMS has become an efficient method for the separation and characterization of gas-phase ions at ambient pressure, often in air, to detect trace amounts of chemical species including explosives, toxic chemicals, chemical warfare agents and other compounds. However the resolution of FAIMS and ion separation capability need to be improved for more applications of the technique. The effects of above-ambient pressure varying from 1 to 3 atm on peak position, resolving power, peak width, and peak intensity are investigated theoretically and experimentally using micro-fabricated planar FAIMS in purified air. Peak positions, varying with pressure in a way as a function of dispersion voltage, could be simplified by expressing both compensation and dispersion fields in Townsend units for E/N, the ratio of electric field intensity (E) to the gas number density (N). It is demonstrated that ion Townsend-scale peak positions remain unchanged for a range of pressures investigated, implying that the higher the pressure is, stronger compensation and separation fields are needed within limits of air breakdown field. Increase in pressure is found to separate ions that could not be distinguished in ambient pressure, which could be interpreted as the differentials of ions' peak compensation voltage expanded wider than the dilation of peak widths leading to resolving power enhancement with pressure. Increase in pressure can also result in an increase in peak intensity. Copyright © 2016 John Wiley & Sons, Ltd.

State-resolved Photodissociation and Radiative Association Data for the Molecular Hydrogen Ion

NASA Astrophysics Data System (ADS)

Zammit, Mark C.; Savage, Jeremy S.; Colgan, James; Fursa, Dmitry V.; Kilcrease, David P.; Bray, Igor; Fontes, Christopher J.; Hakel, Peter; Timmermans, Eddy

2017-12-01

We present state-resolved (electronic, vibrational, and rotational) cross sections and rate coefficients for the photodissociation (PD) of {{{H}}}2+ and radiative association (RA) of H–H+. We developed a fully quantum mechanical approach within the nonrelativistic Born–Oppenheimer approximation to describe {{{H}}}2+ and calculate the data for transitions between the ground electronic state 1s{σ }g and the 2p{σ }u, 2p{π }u, 3p{σ }u, 3p{π }u, 4p{σ }u, 4f{σ }u, 4f{π }u, and 4p{π }u electronic states (i.e., up to {{{H}}}2+ n = 4). Tables of the dipole-matrix elements and energies needed to calculate state-resolved cross sections and rate coefficients will be made publicly available. These data could be important in astrophysical models when dealing with photon wavelengths (or radiation temperature distributions that are weighted toward such wavelengths) around 100 nm. For example, at these wavelengths and a material temperature of 8400 K, the LTE-averaged PD cross section via the (second electronically excited) 2p{π }u state is over three times larger than the PD cross section via the (first electronically excited) 2p{σ }u state.

Applications and limitations of constrained high-resolution peak fitting on low resolving power mass spectra from the ToF-ACSM

DOE PAGES

Timonen, Hilkka; Cubison, Mike; Aurela, Minna; ...

2016-07-25

The applicability, methods and limitations of constrained peak fitting on mass spectra of low mass resolving power ( m/Δ m 50~500) recorded with a time-of-flight aerosol chemical speciation monitor (ToF-ACSM) are explored. Calibration measurements as well as ambient data are used to exemplify the methods that should be applied to maximise data quality and assess confidence in peak-fitting results. Sensitivity analyses and basic peak fit metrics such as normalised ion separation are employed to demonstrate which peak-fitting analyses commonly performed in high-resolution aerosol mass spectrometry are appropriate to perform on spectra of this resolving power. Information on aerosol sulfate, nitrate,more » sodium chloride, methanesulfonic acid as well as semi-volatile metal species retrieved from these methods is evaluated. The constants in a commonly used formula for the estimation of the mass concentration of hydrocarbon-like organic aerosol may be refined based on peak-fitting results. Lastly, application of a recently published parameterisation for the estimation of carbon oxidation state to ToF-ACSM spectra is validated for a range of organic standards and its use demonstrated for ambient urban data.« less

Fast neutral beam ion source coupled to a Fourier transform ion cyclotron resonance mass spectrometer

NASA Astrophysics Data System (ADS)

Hill, Nicholas C.; Limbach, Patrick A.; Shomo, Ronald E., II; Marshall, Alan G.; Appelhans, Anthony D.; Delmore, James E.

1991-11-01

The coupling of an autoneutralizing SF-6 fast ion-beam gun to a Fourier transform ion cyclotron resonance (FT/ICR) mass spectrometer is described. The fast neutral beam provides for secondary-ion-type FT/ICR mass analysis [e.g., production of abundant pseudomolecular (M+H)+ ions] of involatile samples without the need for external ion injection, since ions are formed at the entrance to the ICR ion trap. The design, construction, and testing of the hybrid instrument are described. The feasibility of the experiment (for both broadband and high-resolution FT/ICR positive-ion mass spectra) is demonstrated with tetra-butylammonium bromide and a Tylenol■ sample. The ability to analyze high molecular weight polymers with high mass resolution is demonstrated for Teflon■. All of the advantages of the fast neutral beam ion source previously demonstrated with quadrupole mass analysis are preserved, and the additional advantages of FT/ICR mass analysis (e.g., high mass resolving power, ion trapping) are retained.

Exciplexes versus Loose Ion Pairs: How Does the Driving Force Impact the Initial Product Ratio of Photoinduced Charge Separation Reactions?

PubMed Central

2014-01-01

Many donor–acceptor systems can undergo a photoinduced charge separation reaction, yielding loose ion pairs (LIPs). LIPs can be formed either directly via (distant) electron transfer (ET) or indirectly via the dissociation of an initially formed exciplex or tight ion pair. Establishing the prevalence of one of the reaction pathways is challenging because differentiating initially formed exciplexes from LIPs is difficult due to similar spectroscopic footprints. Hence, no comprehensive reaction model has been established for moderately polar solvents. Here, we employ an approach based on the time-resolved magnetic field effect (MFE) of the delayed exciplex luminescence to distinguish the two reaction channels. We focus on the effects of the driving force of ET and the solvent permittivity. We show that, surprisingly, the exciplex channel is significant even for an exergonic ET system with a free energy of ET of −0.58 eV and for the most polar solutions studied (butyronitrile). Our findings demonstrate that exciplexes play a crucial role even in polar solvents and at moderate driving forces, contrary to what is usually assumed. PMID:25243054

A new window towards multidimensional sensing of transition metal cations through dual mode sensing ability of N-benzyl-(3-hydoxy-2-naphthalene): Emission enhancement coupled remarkable spectral shift

NASA Astrophysics Data System (ADS)

Paul, Bijan Kumar; Mahanta, Subrata; Singh, Rupashree Balia; Guchhait, Nikhil

2011-06-01

A structurally simple Schiff base N-benzyl-(3-hydroxy-2-naphthalene) (NBHN32) has been synthesized and characterized by 1H NMR, 13C NMR, and DEPT spectroscopy. The photophysical behaviour of NBHN32 in response to the presence of various transition metal cations has been explored by means of steady-state absorption, emission and time-resolved emission spectroscopy techniques. Efficient through space intramolecular photoinduced electron transfer (PET) between the naphthalene fluorophore and the imine group has been argued for extremely low fluorescence yield of NBHN32 compared to the parent molecule 3-hydroxy-2-naphthaldehyde (HN32) containing the same fluorophore but lacking the receptor moiety. Transition metal ion-induced emission enhancement is thus addressed on the lexicon of perturbation of the PET by the metal ions. Apart from fluorescence enhancement, transition metal ion imparts remarkable shift of the emission maxima of NBHN32, which is another unique aspect on the proposed ability of NBHN32 to function as a fluorescence chemosensor.

Calculation of low-Z impurity pellet induced fluxes of charge exchange neutral particles escaping from magnetically confined toroidal plasmas.

PubMed

Goncharov, P R; Ozaki, T; Sudo, S; Tamura, N; Tolstikhina, I Yu; Sergeev, V Yu

2008-10-01

Measurements of energy- and time-resolved neutral hydrogen and helium fluxes from an impurity pellet ablation cloud, referred to as pellet charge exchange or PCX experiments, can be used to study local fast ion energy distributions in fusion plasmas. The estimation of the local distribution function f(i)(E) of fast ions entering the cloud requires knowledge of both the fraction F(0)(E) of incident ions exiting the cloud as neutral atoms and the attenuation factor A(E,rho) describing the loss of fast atoms in the plasma. Determination of A(E,rho), in turn, requires the total stopping cross section sigma(loss) of neutral atoms in the plasma and the Jacobian reflecting the measurement geometry and the magnetic surface shape. The obtained functions F(0)(E) and A(E,rho) enter multiplicatively into the probability density for escaping neutral particle kinetic energy. A general calculation scheme has been developed and realized as a FORTRAN code, which is to be applied for the calculation of f(i)(E) from PCX experimental results obtained with low-Z impurity pellets.

Characterizing the Performance of the Princeton Advanced Test Stand Ion Source

NASA Astrophysics Data System (ADS)

Stepanov, A.; Gilson, E. P.; Grisham, L.; Kaganovich, I.; Davidson, R. C.

2012-10-01

The Princeton Advanced Test Stand (PATS) is a compact experimental facility for studying the physics of intense beam-plasma interactions relevant to the Neutralized Drift Compression Experiment - II (NDCX-II). The PATS facility consists of a multicusp RF ion source mounted on a 2 m-long vacuum chamber with numerous ports for diagnostic access. Ar+ beams are extracted from the source plasma with three-electrode (accel-decel) extraction optics. The RF power and extraction voltage (30 - 100 kV) are pulsed to produce 100 μsec duration beams at 0.5 Hz with excellent shot-to-shot repeatability. Diagnostics include Faraday cups, a double-slit emittance scanner, and scintillator imaging. This work reports measurements of beam parameters for a range of beam energies (30 - 50 keV) and currents to characterize the behavior of the ion source and extraction optics. Emittance scanner data is used to calculate the beam trace-space distribution and corresponding transverse emittance. If the plasma density is changing during a beam pulse, time-resolved emittance scanner data has been taken to study the corresponding evolution of the beam trace-space distribution.

Nano suboxide layer generated in Ta{sub 2}O{sub 5} by Ar{sup +} ion irradiation

DOE Office of Scientific and Technical Information (OSTI.GOV)

Song, W. D., E-mail: song-wendong@dsi.a-star.edu.sg, E-mail: ying-ji-feng@dsi.a-star.edu.sg; Ying, J. F., E-mail: song-wendong@dsi.a-star.edu.sg, E-mail: ying-ji-feng@dsi.a-star.edu.sg; He, W.

2015-01-19

Ta{sub 2}O{sub 5}/TaO{sub x} heterostructure has become a leading oxide layer in memory cells and/or a bidirectional selector for resistive random access memory (RRAM). Although atomic layer deposition (ALD) was found to be uniquely suitable for depositing uniform and conformal films on complex topographies, it is hard to use ALD to grow suboxide TaO{sub x} layer. In this study, tantalum oxide films with a composition of Ta{sub 2}O{sub 5} were grown by ALD. Using Ar{sup +} ion irradiation, the suboxide was formed in the top layer of Ta{sub 2}O{sub 5} films by observing the Ta core level shift toward lowermore » binding energy with angle-resolved X-ray photoelectron spectroscopy. By controlling the energy and irradiation time of an Ar{sup +} ion beam, Ta{sub 2}O{sub 5}/TaO{sub x} heterostructure can be reliably produced on ALD films, which provides a way to fabricate the critical switching layers of RRAM.« less

Europium-doped mesoporous titania thin films: rare-earth locations and emission fluctuations under illumination.

PubMed

Leroy, Celine Marie; Cardinal, Thierry; Jubera, Veronique; Treguer-Delapierre, Mona; Majimel, Jerome; Manaud, Jean Pierre; Backov, Renal; Boissière, Cedric; Grosso, David; Sanchez, Clement; Viana, Bruno; Pellé, Fabienne

2008-10-06

Herein, Eu(III)-doped 3D mesoscopically ordered arrays of mesoporous and nanocrystalline titania are prepared and studied. The rare-earth-doped titania thin films-synthesized via evaporation-induced self-assembly (EISA)-are characterized by using environmental ellipsoporosimetry, electronic microscopy (i.e. high-resolution scanning electron microscopy, HR-SEM, and transmission electron microscopy, HR-TEM), X-ray diffraction, and luminescence spectroscopy. Structural characterizations show that high europium-ion loadings can be incorporated into the titanium-dioxide walls without destroying the mesoporous arrangement. The luminescence properties of Eu(III) are investigated by using steady-state and time-resolved spectroscopy via excitation of the Eu(III) ions through the titania host. Using Eu(III) luminescence as a probe, the europium-ion sites can be addressed with at least two different environments within the mesoporous framework, namely, a nanocrystalline environment and a glasslike one. Emission fluctuations ((5)D(0)-->(7)F(2)) are observed upon continuous UV excitation in the host matrix. These fluctuations are attributed to charge trapping and appear to be strongly dependent on the amount of europium and the level of crystallinity.

Towards the development of new phosphors with reduced content of rare earth elements: Structural and optical characterization of Ce:Tb: Al{sub 2}SiO{sub 5}

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chiriu, D.; Stagi, L.; Carbonaro, C.M.

2016-05-15

Highlights: • A new promising inert matrix as host of luminescent ions is proposed. • Al2SiO5 matrix is free from Rare earths (critical raw materials). • Doping the matrix with Ce and Tb we obtain an efficient green emitter. • Cerium acts as sensitizer for Terbium emission. - Abstract: A new promising inert matrix as host of luminescent ions is proposed. Al2SiO5 samples, doped with rare earths (Ce, Tb single doped and co-doped) are proposed as good prospect for the development of new UV–vis converter with reduced content of rare earths elements. Structural characterization by Raman, XRD spectroscopy and TEMmore » imaging reveals the sillimanite phase and nano sized dimension of the investigated powders. Optical characterization by steady time and time resolved emission spectroscopy for the single doped and co-doped samples allows to identify an efficient energy transfer from Ce to Tb ions under near UV excitation wavelength. The intense green emission observed in the Ce:Tb co-doped Al2SiO5 system suggests its potential application as efficient blue pumped green emitter phosphor to be exploited for white LED: to this purpose we tested the compound in combination with a red emitting doping ion recording for Ce:Tb:Cr:ASO system a correlated color temperature of 6720 K.« less

The 2004 NASA Aerospace Battery Workshop

NASA Technical Reports Server (NTRS)

2006-01-01

Topics covered include: Super NiCd(TradeMark) Energy Storage for Gravity Probe-B Relativity Mission; Hubble Space Telescope 2004 Battery Update; The Development of Hermetically Sealed Aerospace Nickel-Metal Hydride Cell; Serial Charging Test on High Capacity Li-Ion Cells for the Orbiter Advanced Hydraulic Power System; Cell Equalization of Lithium-Ion Cells; The Long-Term Performance of Small-Cell Batteries Without Cell-Balancing Electronics; Identification and Treatment of Lithium Battery Cell Imbalance under Flight Conditions; Battery Control Boards for Li-Ion Batteries on Mars Exploration Rovers; Cell Over Voltage Protection and Balancing Circuit of the Lithium-Ion Battery; Lithium-Ion Battery Electronics for Aerospace Applications; Lithium-Ion Cell Charge Control Unit; Lithium Ion Battery Cell Bypass Circuit Test Results at the U.S. Naval Research Laboratory; High Capacity Battery Cell By-Pass Switches: High Current Pulse Testing of Lithium-Ion; Battery By-Pass Switches to Verify Their Ability to Withstand Short-Circuits; Incorporation of Physics-Based, Spatially-Resolved Battery Models into System Simulations; A Monte Carlo Model for Li-Ion Battery Life Projections; Thermal Behavior of Large Lithium-Ion Cells; Thermal Imaging of Aerospace Battery Cells; High Rate Designed 50 Ah Li-Ion Cell for LEO Applications; Evaluation of Corrosion Behavior in Aerospace Lithium-Ion Cells; Performance of AEA 80 Ah Battery Under GEO Profile; LEO Li-Ion Battery Testing; A Review of the Feasibility Investigation of Commercial Laminated Lithium-Ion Polymer Cells for Space Applications; Lithium-Ion Verification Test Program; Panasonic Small Cell Testing for AHPS; Lithium-Ion Small Cell Battery Shorting Study; Low-Earth-Orbit and Geosynchronous-Earth-Orbit Testing of 80 Ah Batteries under Real-Time Profiles; Update on Development of Lithium-Ion Cells for Space Applications at JAXA; Foreign Comparative Technology: Launch Vehicle Battery Cell Testing; 20V, 40 Ah Lithium Ion Polymer Battery for the Spacesuit; Low Temperature Life-Cycle Testing of a Lithium-Ion Battery for Low-Earth-Orbiting Spacecraft; and Evaluation of the Effects of DoD and Charge Rate on a LEO Optimized 50 Ah Li-Ion Aerospace Cell.

K-shell photoabsorption edge of strongly coupled aluminum driven by laser-converted radiation

NASA Astrophysics Data System (ADS)

Zhao, Yang; Zhang, Zhiyu; Qing, Bo; Yang, Jiamin; Zhang, Jiyan; Wei, Minxi; Yang, Guohong; Song, Tianming; Xiong, Gang; Lv, Min; Hu, Zhimin; Deng, Bo; Hu, Xin; Zhang, Wenhai; Shang, Wanli; Hou, Lifei; Du, Huabing; Zhan, Xiayu; Yu, Ruizhen

2017-03-01

The first observation of the K-shell photoabsorption edge of strongly coupled aluminum generated by intense x-ray radiation-driven shocks is reported. By using a “dog bone” gold hohlraum as an x-ray converter, colliding shocks compression and preheating shielding are achieved to generate an unexplored state with a density of 5.5 g/cm3 and temperature of 0.43 eV (the ion-ion coupling parameter Γii is around 240). The time-resolved K-shell photoabsorption edges are measured with a crystal spectrometer using a short x-ray backlighter. The broadenings and redshifts of the edges are studied by using the slope fitting of the edge and quantum molecular dynamics calculations. This work shows that the K-edge of aluminum driven by laser-converted radiation provides a novel capability to probe WDM at extended conditions.

DEATH-STAR: Silicon and photovoltaic fission fragment detector arrays for light-ion induced fission correlation studies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Koglin, J. D.; Burke, J. T.; Fisher, S. E.

Here, the Direct Excitation Angular Tracking pHotovoltaic-Silicon Telescope ARray (DEATH-STAR) combines a series of 12 silicon detectors in a ΔE–E configuration for charged particle identification with a large-area array of 56 photovoltaic (solar) cells for detection of fission fragments. The combination of many scattering angles and fission fragment detectors allows for an angular-resolved tool to study reaction cross sections using the surrogate method, anisotropic fission distributions, and angular momentum transfers through stripping, transfer, inelastic scattering, and other direct nuclear reactions. The unique photovoltaic detectors efficiently detect fission fragments while being insensitive to light ions and have a timing resolution ofmore » 15.63±0.37 ns. Alpha particles are detected with a resolution of 35.5 keV 1σ at 7.9 MeV. Measured fission fragment angular distributions are also presented.« less

DEATH-STAR: Silicon and Photovoltaic Fission Fragment Detector Arrays for Light-Ion Induced Fission Correlation Studies

NASA Astrophysics Data System (ADS)

Koglin, J. D.; Burke, J. T.; Fisher, S. E.; Jovanovic, I.

2017-05-01

The Direct Excitation Angular Tracking pHotovoltaic-Silicon Telescope ARray (DEATH-STAR) combines a series of 12 silicon detectors in a ΔE - E configuration for charged particle identification with a large-area array of 56 photovoltaic (solar) cells for detection of fission fragments. The combination of many scattering angles and fission fragment detectors allows for an angular-resolved tool to study reaction cross sections using the surrogate method, anisotropic fission distributions, and angular momentum transfers through stripping, transfer, inelastic scattering, and other direct nuclear reactions. The unique photovoltaic detectors efficiently detect fission fragments while being insensitive to light ions and have a timing resolution of 15.63±0.37 ns. Alpha particles are detected with a resolution of 35.5 keV 1σ at 7.9 MeV. Measured fission fragment angular distributions are also presented.

DEATH-STAR: Silicon and photovoltaic fission fragment detector arrays for light-ion induced fission correlation studies

DOE PAGES

Koglin, J. D.; Burke, J. T.; Fisher, S. E.; ...

2017-02-20

Here, the Direct Excitation Angular Tracking pHotovoltaic-Silicon Telescope ARray (DEATH-STAR) combines a series of 12 silicon detectors in a ΔE–E configuration for charged particle identification with a large-area array of 56 photovoltaic (solar) cells for detection of fission fragments. The combination of many scattering angles and fission fragment detectors allows for an angular-resolved tool to study reaction cross sections using the surrogate method, anisotropic fission distributions, and angular momentum transfers through stripping, transfer, inelastic scattering, and other direct nuclear reactions. The unique photovoltaic detectors efficiently detect fission fragments while being insensitive to light ions and have a timing resolution ofmore » 15.63±0.37 ns. Alpha particles are detected with a resolution of 35.5 keV 1σ at 7.9 MeV. Measured fission fragment angular distributions are also presented.« less

Enhancing the luminescence efficiency of silicon-nanocrystals by interaction with H+ ions.

PubMed

Cannas, Marco; Camarda, Pietro; Vaccaro, Lavinia; Amato, Francesco; Messina, Fabrizio; Fiore, Tiziana; Li Vigni, Maria

2018-04-18

The emission of silicon nanocrystals (Si-NCs), synthesized by pulsed laser ablation in water, was investigated on varying the pH of the solution. These samples emit μs decaying orange photoluminescence (PL) associated with radiative recombination of quantum-confined excitons. Time-resolved spectra reveal that both the PL intensity and the lifetime increase by a factor of ∼20 when the pH decreases from 10 to 1 thus indicating that the emission quantum efficiency increases by inhibiting nonradiative decay rates. Infrared (IR) absorption and electron paramagnetic resonance (EPR) experiments allow addressing the origin of defects on which the excitons nonradiatively recombine. The linear correlation between the PL and the growth of SiH groups demonstrates that H+ ions passivate the nonradiative defects that are located in the interlayer between the Si-NC core and the amorphous SiO2 shell.

Spontaneous and stimulated emission spectroscopy of a Nd(3+)-doped phosphate glass under wavelength selective pumping.

PubMed

Iparraguirre, I; Azkargorta, J; Balda, R; Venkata Krishnaiah, K; Jayasankar, C K; Al-Saleh, M; Fernández, J

2011-09-26

The influence of the host matrix on the spectroscopic and laser properties of Nd(3+) in a K-Ba-Al phosphate glass has been investigated as a function of rare-earth concentration. Site-selective time resolved laser spectroscopy and stimulated emission experiments under selective wavelength laser pumping show the existence of a very complex crystal field site distribution of Nd(3+) ions in this glass. The peak of the broad stimulated (4)F(3/2)→(4)I(11/2) emission shifts in a non monotonous way up to 3 nm as a function of the excitation wavelength. This behavior can be explained by the relatively moderate inter-site energy transfer among Nd(3+) ions found in this system and measured by using fluorescence line narrowing spectroscopy. The best slope efficiency obtained for the laser emission was 40%. © 2011 Optical Society of America

Instrument for spatially resolved simultaneous measurements of forces and currents in particle beams

DOE Office of Scientific and Technical Information (OSTI.GOV)

Spethmann, A., E-mail: spethmann@physik.uni-kiel.de; Trottenberg, T., E-mail: trottenberg@physik.uni-kiel.de; Kersten, H., E-mail: kersten@physik.uni-kiel.de

The article presents a device for spatially resolved and simultaneous measurements of forces and currents in particle beams, especially in beams composed of ions and neutral atoms. The forces are exerted by the impinging beam particles on a plane circular conductive target plate of 20 mm diameter mounted on a pendulum with electromagnetic force compensation. The force measurement in the micronewton range is achieved by electromagnetic compensation by means of static Helmholtz coils and permanent magnets attached to the pendulum. Exemplary measurements are performed in the 1.2 keV beam of a broad beam ion source. The simultaneous measurements of forcesmore » and currents onto the same target are compared with each other and with Faraday cup measurements.« less

A spatially resolving x-ray crystal spectrometer for measurement of ion-temperature and rotation-velocity profiles on the Alcator C-Mod tokamak.

PubMed

Hill, K W; Bitter, M L; Scott, S D; Ince-Cushman, A; Reinke, M; Rice, J E; Beiersdorfer, P; Gu, M-F; Lee, S G; Broennimann, Ch; Eikenberry, E F

2008-10-01

A new spatially resolving x-ray crystal spectrometer capable of measuring continuous spatial profiles of high resolution spectra (lambda/d lambda>6000) of He-like and H-like Ar K alpha lines with good spatial (approximately 1 cm) and temporal (approximately 10 ms) resolutions has been installed on the Alcator C-Mod tokamak. Two spherically bent crystals image the spectra onto four two-dimensional Pilatus II pixel detectors. Tomographic inversion enables inference of local line emissivity, ion temperature (T(i)), and toroidal plasma rotation velocity (upsilon(phi)) from the line Doppler widths and shifts. The data analysis techniques, T(i) and upsilon(phi) profiles, analysis of fusion-neutron background, and predictions of performance on other tokamaks, including ITER, will be presented.

Surface-Induced Dissociation of Protein Complexes in a Hybrid Fourier Transform Ion Cyclotron Resonance Mass Spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yan, Jing; Zhou, Mowei; Gilbert, Joshua D.

Mass spectrometry continues to develop as a valuable tool in the analysis of proteins and protein complexes. In protein complex mass spectrometry studies, surface-induced dissociation (SID) has been successfully applied in quadrupole time-of-flight (Q-TOF) instruments. SID provides structural information on noncovalent protein complexes that is complementary to other techniques. However, the mass resolution of Q-TOF instruments can limit the information that can be obtained for protein complexes by SID. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) provides ultrahigh resolution and ultrahigh mass accuracy measurements. Here in this study, an SID device was designed and successfully installed in amore » hybrid FT-ICR instrument in place of the standard gas collision cell. The SID-FT-ICR platform has been tested with several protein complex systems (homooligomers, a heterooligomer, and a protein-ligand complex, ranging from 53 to 85 kDa), and the results are consistent with data previously acquired on Q-TOF platforms, matching predictions from known protein interface information. Lastly, SID fragments with the same m/z but different charge states are well-resolved based on distinct spacing between adjacent isotope peaks, and the addition of metal cations and ligands can also be isotopically resolved with the ultrahigh mass resolution available in FT-ICR.« less

Surface-Induced Dissociation of Protein Complexes in a Hybrid Fourier Transform Ion Cyclotron Resonance Mass Spectrometer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yan, Jing; Zhou, Mowei; Gilbert, Joshua D.

Mass spectrometry continues to develop as a valuable tool in the analysis of proteins and protein complexes. In protein complex mass spectrometry studies, surface-induced dissociation (SID) has been successfully applied in quadrupole time-of-flight (Q-TOF) instruments. SID provides structural information on non-covalent protein complexes that is complementary to other techniques. However, the mass resolution of Q-TOF instruments can limit the information that can be obtained for protein complexes by SID. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) provides ultrahigh resolution and ultrahigh mass accuracy measurements. In this study, an SID device was designed and successfully installed in a hybridmore » FT-ICR instrument in place of the standard gas collision cell. The SID-FT-ICR platform has been tested with several protein complex systems (homooligomers, a heterooligomer, and a protein-ligand complex, ranging from 53 kDa to 85 kDa), and the results are consistent with data previously acquired on Q-TOF platforms, matching predictions from known protein interface information. SID fragments with the same m/z but different charge states are well-resolved based on distinct spacing between adjacent isotope peaks, and the addition of metal cations and ligands can also be isotopically resolved with the ultrahigh mass resolution available in FT-ICR.« less

Surface-Induced Dissociation of Protein Complexes in a Hybrid Fourier Transform Ion Cyclotron Resonance Mass Spectrometer

DOE PAGES

Yan, Jing; Zhou, Mowei; Gilbert, Joshua D.; ...

2016-12-02

Mass spectrometry continues to develop as a valuable tool in the analysis of proteins and protein complexes. In protein complex mass spectrometry studies, surface-induced dissociation (SID) has been successfully applied in quadrupole time-of-flight (Q-TOF) instruments. SID provides structural information on noncovalent protein complexes that is complementary to other techniques. However, the mass resolution of Q-TOF instruments can limit the information that can be obtained for protein complexes by SID. Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) provides ultrahigh resolution and ultrahigh mass accuracy measurements. Here in this study, an SID device was designed and successfully installed in amore » hybrid FT-ICR instrument in place of the standard gas collision cell. The SID-FT-ICR platform has been tested with several protein complex systems (homooligomers, a heterooligomer, and a protein-ligand complex, ranging from 53 to 85 kDa), and the results are consistent with data previously acquired on Q-TOF platforms, matching predictions from known protein interface information. Lastly, SID fragments with the same m/z but different charge states are well-resolved based on distinct spacing between adjacent isotope peaks, and the addition of metal cations and ligands can also be isotopically resolved with the ultrahigh mass resolution available in FT-ICR.« less

X-ray emission from high temperature plasmas

NASA Technical Reports Server (NTRS)

Harries, W. L.

1977-01-01

The physical processes occurring in plasma focus devices were investigated with particular emphasis on X-ray emission. Topics discussed include: trajectories of high energy electrons; detection of ion trajectories; spatial distribution of neutron emission; space and time resolved emission of hard X-rays from a plasma focus; the staged plasma focus as a variation of the hypocloidal pinch; formation of current sheets in a staged plasma focus; and X-ray and neutron emission from a staged plasma focus. The possibility of operating dense plasma-focus type devices in multiple arrays beyond the scaling law for a single gun is discussed.

O-shell emission of heavy atoms in an optically thin tokamak plasma

NASA Astrophysics Data System (ADS)

Finkenthal, M.; Lippmann, S.; Huang, L. K.; Zwicker, A.; Moos, H. W.; Goldstein, W. H.; Osterheld, A. L.

1992-04-01

Heavy atoms Au (Z=79), Pb (Z=82), Bi (Z=83), and U (Z=92) have been introduced in the low-density (ne~1013 cm-3) high-temperature (Te>=1 keV) TEXT tokamak (Fusion Research Center, University of Texas at Austin) plasma. The emission has been measured in the 50-200-Å range using a photometrically calibrated, time-resolving grazing-incidence spectrometer. The O-shell ion emission has been identified by comparison with ab initio energy-level calculations and line-intensity predictions of collisional radiative models for various charge states with 5p65dk ground-state configurations.

Time resolved 3D momentum imaging of ultrafast dynamics by coherent VUV-XUV radiation

DOE PAGES

Sturm, F. P.; Wright, T. W.; Ray, D.; ...

2016-06-14

Have we present a new experimental setup for measuring ultrafast nuclear and electron dynamics of molecules after photo-excitation and ionization. We combine a high flux femtosecond vacuum ultraviolet (VUV) and extreme ultraviolet (XUV) source with an internally cold molecular beam and a 3D momentum imaging particle spectrometer to measure electrons and ions in coincidence. We describe a variety of tools developed to perform pump-probe studies in the VUV-XUV spectrum and to modify and characterize the photon beam. First benchmark experiments are presented to demonstrate the capabilities of the system.

Novel algorithm for simultaneous component detection and pseudo-molecular ion characterization in liquid chromatography-mass spectrometry.

PubMed

Zhang, Yufeng; Wang, Xiaoan; Wo, Siukwan; Ho, Hingman; Han, Quanbin; Fan, Xiaohui; Zuo, Zhong

2015-01-01

Resolving components and determining their pseudo-molecular ions (PMIs) are crucial steps in identifying complex herbal mixtures by liquid chromatography-mass spectrometry. To tackle such labor-intensive steps, we present here a novel algorithm for simultaneous detection of components and their PMIs. Our method consists of three steps: (1) obtaining a simplified dataset containing only mono-isotopic masses by removal of background noise and isotopic cluster ions based on the isotopic distribution model derived from all the reported natural compounds in dictionary of natural products; (2) stepwise resolving and removing all features of the highest abundant component from current simplified dataset and calculating PMI of each component according to an adduct-ion model, in which all non-fragment ions in a mass spectrum are considered as PMI plus one or several neutral species; (3) visual classification of detected components by principal component analysis (PCA) to exclude possible non-natural compounds (such as pharmaceutical excipients). This algorithm has been successfully applied to a standard mixture and three herbal extract/preparations. It indicated that our algorithm could detect components' features as a whole and report their PMI with an accuracy of more than 98%. Furthermore, components originated from excipients/contaminants could be easily separated from those natural components in the bi-plots of PCA. Copyright © 2014 Elsevier B.V. All rights reserved.

A radially accessible tubular in situ X-ray cell for spatially resolved operando scattering and spectroscopic studies of electrochemical energy storage devices

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Hao; Allan, Phoebe K.; Borkiewicz, Olaf J.

2016-09-16

A tubularoperandoelectrochemical cell has been developed to allow spatially resolved X-ray scattering and spectroscopic measurements of individual cell components, or regions thereof, during device operation. These measurements are enabled by the tubular cell geometry, wherein the X-ray-transparent tube walls allow radial access for the incident and scattered/transmitted X-ray beam; by probing different depths within the electrode stack, the transformation of different components or regions can be resolved. The cell is compatible with a variety of synchrotron-based scattering, absorption and imaging methodologies. The reliability of the electrochemical cell and the quality of the resulting X-ray scattering and spectroscopic data are demonstratedmore » for two types of energy storage: the evolution of the distribution of the state of charge of an Li-ion battery electrode during cycling is documented using X-ray powder diffraction, and the redistribution of ions between two porous carbon electrodes in an electrochemical double-layer capacitor is documented using X-ray absorption near-edge spectroscopy.« less

The complex ion structure of warm dense carbon measured by spectrally resolved x-ray scattering

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kraus, D.; Barbrel, B.; Falcone, R. W.

2015-05-15

We present measurements of the complex ion structure of warm dense carbon close to the melting line at pressures around 100 GPa. High-pressure samples were created by laser-driven shock compression of graphite and probed by intense laser-generated x-ray sources with photon energies of 4.75 keV and 4.95 keV. High-efficiency crystal spectrometers allow for spectrally resolving the scattered radiation. Comparing the ratio of elastically and inelastically scattered radiation, we find evidence for a complex bonded liquid that is predicted by ab-initio quantum simulations showing the influence of chemical bonds under these conditions. Using graphite samples of different initial densities we demonstrate the capability ofmore » spectrally resolved x-ray scattering to monitor the carbon solid-liquid transition at relatively constant pressure of 150 GPa. Showing first single-pulse scattering spectra from cold graphite of unprecedented quality recorded at the Linac Coherent Light Source, we demonstrate the outstanding possibilities for future high-precision measurements at 4th Generation Light Sources.« less

Self-consistent simulation of high-frequency driven plasma sheaths

NASA Astrophysics Data System (ADS)

Shihab, Mohammed; Eremin, Denis; Mussenbrock, Thomas; Brinkmann, Ralf

2011-10-01

Low pressure capacitively coupled plasmas are widely used in plasma processing and microelectronics industry. Understanding the dynamics of the boundary sheath is a fundamental problem. It controls the energy and angular distribution of ions bombarding the electrode, which in turn affects the surface reaction rate and the profile of microscopic features. In this contribution, we investigate the dynamics of plasma boundary sheaths by means of a kinetic self-consistent model, which is able to resolve the ion dynamics. Asymmetric sheath dynamics is observed for the intermediate RF regime, i.e., in the regime where the ion plasma frequency is equal to the driving frequency. The ion inertia causes an additional phase difference between the expansion and the contraction phase of the plasma sheath and an asymmetry for the ion energy distribution bimodal shape. A comparison with experimental results and particle in cell simulations is performed. Low pressure capacitively coupled plasmas are widely used in plasma processing and microelectronics industry. Understanding the dynamics of the boundary sheath is a fundamental problem. It controls the energy and angular distribution of ions bombarding the electrode, which in turn affects the surface reaction rate and the profile of microscopic features. In this contribution, we investigate the dynamics of plasma boundary sheaths by means of a kinetic self-consistent model, which is able to resolve the ion dynamics. Asymmetric sheath dynamics is observed for the intermediate RF regime, i.e., in the regime where the ion plasma frequency is equal to the driving frequency. The ion inertia causes an additional phase difference between the expansion and the contraction phase of the plasma sheath and an asymmetry for the ion energy distribution bimodal shape. A comparison with experimental results and particle in cell simulations is performed. The financial support from the Federal Ministry of Education and Research within the frame of the project ``Plasma-Technology-Grid'' and the support of the DFG via the collaborative research center SFB-TR87 is gratefully acknowledged.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Godfrey, T. J.; Yu, Hui; Ullrich, Susanne, E-mail: ullrich@physast.uga.edu

The studies herein investigate the involvement of the low-lying {sup 1}L{sub a} and {sup 1}L{sub b} states with {sup 1}ππ{sup *} character and the {sup 1}πσ{sup *} state in the deactivation process of indole following photoexcitation at 201 nm. Three gas-phase, pump-probe spectroscopic techniques are employed: (1) Time-resolved photoelectron spectroscopy (TR-PES), (2) hydrogen atom (H-atom) time-resolved kinetic energy release (TR-KER), and (3) time-resolved ion yield (TR-IY). Each technique provides complementary information specific to the photophysical processes in the indole molecule. In conjunction, a thorough examination of the electronically excited states in the relaxation process, with particular focus on the involvement ofmore » the {sup 1}πσ{sup *} state, is afforded. Through an extensive analysis of the TR-PES data presented here, it is deduced that the initial excitation of the {sup 1}B{sub b} state decays to the {sup 1}L{sub a} state on a timescale beyond the resolution of the current experimental setup. Relaxation proceeds on the {sup 1}L{sub a} state with an ultrafast decay constant (<100 femtoseconds (fs)) to the lower-lying {sup 1}L{sub b} state, which is found to possess a relatively long lifetime of 23 ± 5 picoseconds (ps) before regressing to the ground state. These studies also manifest an additional component with a relaxation time of 405 ± 76 fs, which is correlated with activity along the {sup 1}πσ{sup *} state. TR-KER and TR-IY experiments, both specifically probing {sup 1}πσ{sup *} dynamics, exhibit similar decay constants, further validating these observations.« less

Time-of-flight atom-probe field-ion microscope for the study of defects in metals. Report No. 2357. [W--25 at. % Re

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hall, T.M.; Wagner, A.; Berger, A.S.

1975-06-01

An ultra-high vacuum time-of-flight (TOF) atom-probe field ion microscope (FIM) specifically designed for the study of defects in metals is described. The variable magnification FIM image is viewed with the aid of an internal image intensification system based on a channel electron-multiplier array. The specimen is held in a liquid-helium-cooled goniometer stage, and the specimen is exchanged by means of a high-vacuum (less than 10/sup -6/ torr) specimen exchange device. This stage allows the specimen to be maintained at a tip temperature anywhere in the range from 13 to 450/sup 0/K. Specimens can also be irradiated in-situ with any low-energymore » (less than 1 keV) gas ion employing a specially constructed ion gun. The pulse-field evaporated ions are detected by a Chevron ion-detector located 2.22 m from the FIM specimen. The TOF of the ions are measured by a specially constructed eight-channel digital timer with a resolution of +-10 ns. The entire process of applying the evaporation pulse to the specimen, measuring the dc and pulse voltages, and analyzing the TOF data is controlled by a NOVA 1220 computer. The computer is also interfaced to a Tektronix graphics terminal which displays the data in the form of a histogram of the number of events versus the mass-to-charge ratio. An extensive set of computer programs to test and operate the atom-probe FIM have been developed. With this automated system we can presently record and analyze 10 TOF s/sup -1/. In the performance tests reported here the instrument has resolved the seven stable isotopes of molybdenum, the five stable isotopes of tungsten, and the two stable isotopes of rhenium in a tungsten--25 at. percent rhenium alloy. (auth)« less

Energy-transfer processes in neon-hydrogen mixtures excited by electron beams

DOE Office of Scientific and Technical Information (OSTI.GOV)

Morozov, A.; Kruecken, R.; Ulrich, A.

2005-12-15

Energy- and charge-transfer processes in neon-hydrogen mixtures (500-1400 hPa neon and 0.001-3 hPa hydrogen partial pressures) excited by a pulsed low-energy ({approx}10 keV) electron beam were investigated using time-resolved spectroscopy. Time spectra of the hydrogen Lyman-{alpha} line, neon excimer emission (second continuum), and neon atomic lines (3p-3s transitions) were recorded. The time-integrated intensity of the Lyman-{alpha} emission was measured for the same range of gas mixtures. It is shown that direct energy transfer from Ne{sub 2}* excimers and neon atoms in the four lowest excited states as well as recombination of H{sub 3}{sup +} ions are the main channels populatingmore » atomic hydrogen in the n=2 state. A rate constant of (4.2{+-}1.4)x10{sup -11} cm{sup 3} s{sup -1} was obtained for the charge transfer from Ne{sub 2}{sup +} ions to molecular hydrogen. A lower limit for the depopulation rate constant of Ne{sub 2}* excimers by molecular hydrogen (combination of energy transfer and ionization) was found to be 1.0x10{sup -10} cm{sup 3} s{sup -1}.« less

Light output function and assembly of the time-of-flight enhanced diagnostics neutron spectrometer plastic scintillators for background reduction by double kinematic selection at EAST

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peng, X. Y.; Chen, Z. J.; Zhang, X.

The 2.5 MeV neutron spectrometer TOFED (Time-Of-Flight Enhanced Diagnostics) has been constructed to perform advanced neutron emission spectroscopy diagnosis of deuterium plasmas on EAST. The instrument has a double-ring structure which, in combination with pulse shape digitization, allows for a dual kinematic selection in the time-of-flight/recoil proton energy (tof/E{sub p}) space, thus improving the spectrometer capability to resolve fast ion signatures in the neutron spectrum, in principle up to a factor ≈100. The identification and separation of features from the energetic ions in the neutron spectrum depends on the detailed knowledge of the instrument response function, both in terms ofmore » the light output function of the scintillators and the effect of undesired multiple neutron scatterings in the instrument. This work presents the determination of the light output function of the TOFED plastic scintillator detectors and their geometrical assembly. Results from dedicated experiments with γ-ray sources and quasi-monoenergetic neutron beams are presented. Implications on the instrument capability to perform background suppression based on double kinematic selection are discussed.« less

Extreme ultraviolet probing of nonequilibrium dynamics in high energy density germanium

NASA Astrophysics Data System (ADS)

Principi, E.; Giangrisostomi, E.; Mincigrucci, R.; Beye, M.; Kurdi, G.; Cucini, R.; Gessini, A.; Bencivenga, F.; Masciovecchio, C.

2018-05-01

Intense femtosecond infrared laser pulses induce a nonequilibrium between thousands of Kelvin hot valence electrons and room-temperature ions in a germanium sample foil. The evolution of this exotic state of matter is monitored with time-resolved extreme ultraviolet absorption spectroscopy across the Ge M2 ,3 edge (≃30 eV ) using the FERMI free-electron laser. We analyze two distinct regimes in the ultrafast dynamics in laser-excited Ge: First, on a subpicosecond time scale, the electron energy distribution thermalizes to an extreme temperature unreachable in equilibrium solid germanium; then, during the following picoseconds, the lattice reacts strongly altering the electronic structure and resulting in melting to a metallic state alongside a breakdown of the local atomic order. Data analysis, based on a hybrid approach including both numerical and analytical calculations, provides an estimation of the electron and ion temperatures, the electron density of states, the carrier-phonon relaxation time, as well as the carrier density and lattice heat capacity under those extreme nonequilibrium conditions. Related structural anomalies, such as the occurrence of a transient low-density liquid phase and the possible drop in lattice heat capacity are discussed.

Decay dynamics of nascent acetonitrile and nitromethane dipole-bound anions produced by intracluster charge-transfer

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yandell, Margaret A.; King, Sarah B.; Neumark, Daniel M., E-mail: dneumark@berkeley.edu

2014-05-14

Decay dynamics of nascent dipole bound states of acetonitrile and nitromethane are examined using time-resolved photoelectron imaging of iodide-acetonitrile (I{sup −}·CH{sub 3}CN) and iodide-nitromethane (I{sup −}·CH{sub 3}NO{sub 2}) complexes. Dipole-bound anions are created by UV-initiated electron transfer to the molecule of interest from the associated iodide ion at energies just below the vertical detachment energy of the halide-molecule complex. The acetonitrile anion is observed to decay biexponentially with time constants in the range of 4–900 ps. In contrast, the dipole bound state of nitromethane decays rapidly over 400 fs to form the valence bound anion. The nitromethane valence anion speciesmore » then decays biexponentially with time constants of 2 ps and 1200 ps. The biexponential decay dynamics in acetonitrile are interpreted as iodine atom loss and autodetachment from the excited dipole-bound anion, followed by slower autodetachment of the relaxed metastable ion, while the dynamics of the nitromethane system suggest that a dipole-bound anion to valence anion transition proceeds via intramolecular vibrational energy redistribution to nitro group modes in the vicinity of the iodine atom.« less

Decay dynamics of nascent acetonitrile and nitromethane dipole-bound anions produced by intracluster charge-transfer.

PubMed

Yandell, Margaret A; King, Sarah B; Neumark, Daniel M

2014-05-14

Decay dynamics of nascent dipole bound states of acetonitrile and nitromethane are examined using time-resolved photoelectron imaging of iodide-acetonitrile (I(-)·CH3CN) and iodide-nitromethane (I(-)·CH3NO2) complexes. Dipole-bound anions are created by UV-initiated electron transfer to the molecule of interest from the associated iodide ion at energies just below the vertical detachment energy of the halide-molecule complex. The acetonitrile anion is observed to decay biexponentially with time constants in the range of 4-900 ps. In contrast, the dipole bound state of nitromethane decays rapidly over 400 fs to form the valence bound anion. The nitromethane valence anion species then decays biexponentially with time constants of 2 ps and 1200 ps. The biexponential decay dynamics in acetonitrile are interpreted as iodine atom loss and autodetachment from the excited dipole-bound anion, followed by slower autodetachment of the relaxed metastable ion, while the dynamics of the nitromethane system suggest that a dipole-bound anion to valence anion transition proceeds via intramolecular vibrational energy redistribution to nitro group modes in the vicinity of the iodine atom.

Numerical study of the magnetized friction force

NASA Astrophysics Data System (ADS)

Fedotov, A. V.; Bruhwiler, D. L.; Sidorin, A. O.; Abell, D. T.; Ben-Zvi, I.; Busby, R.; Cary, J. R.; Litvinenko, V. N.

2006-07-01

Fundamental advances in experimental nuclear physics will require ion beams with orders of magnitude luminosity increase and temperature reduction. One of the most promising particle accelerator techniques for achieving these goals is electron cooling, where the ion beam repeatedly transfers thermal energy to a copropagating electron beam. The dynamical friction force on a fully ionized gold ion moving through magnetized and unmagnetized electron distributions has been simulated, using molecular dynamics techniques that resolve close binary collisions. We present a comprehensive examination of theoretical models in use by the electron cooling community. Differences in these models are clarified, enabling the accurate design of future electron cooling systems for relativistic ion accelerators.

Communication: Identification of daughter ions through their electronic spectroscopy at low temperature

NASA Astrophysics Data System (ADS)

Dedonder, Claude; Féraud, Géraldine; Jouvet, Christophe

2014-10-01

We present experimental results on photofragmentation of cooled fragments issued from the photofragmentation of cold parent ions. The cooling of the daughter ions at a few K allows its characterization not only through its fragmentation pattern but also through its well resolved electronic spectroscopy. The proof of principle of the method is demonstrated on the photofragment resulting from Cα-Cβ bond rupture in protonated tyrosine (TyrH+). The analysis of the daughter ion (m/z 108) photofragmentation spectrum is in agreement with the proposed mechanism implying a proton transfer to the phenyl ring as the first step of the fragmentation mechanism of TyrH+.

Ion Structure Near a Core-Shell Dielectric Nanoparticle

NASA Astrophysics Data System (ADS)

Ma, Manman; Gan, Zecheng; Xu, Zhenli

2017-02-01

A generalized image charge formulation is proposed for the Green's function of a core-shell dielectric nanoparticle for which theoretical and simulation investigations are rarely reported due to the difficulty of resolving the dielectric heterogeneity. Based on the formulation, an efficient and accurate algorithm is developed for calculating electrostatic polarization charges of mobile ions, allowing us to study related physical systems using the Monte Carlo algorithm. The computer simulations show that a fine-tuning of the shell thickness or the ion-interface correlation strength can greatly alter electric double-layer structures and capacitances, owing to the complicated interplay between dielectric boundary effects and ion-interface correlations.

Electron Currents and Heating in the Ion Diffusion Region of Asymmetric Reconnection

NASA Technical Reports Server (NTRS)

Graham, D. B.; Khotyaintsev, Yu. V.; Norgren, C.; Vaivads, A.; Andre, M.; Lindqvist, P. A.; Marklund, G. T.; Ergun, R. E.; Paterson, W. R.; Gershman, D. J.;

Broadband ion mobility deconvolution for rapid analysis of complex mixtures.

PubMed

Pettit, Michael E; Brantley, Matthew R; Donnarumma, Fabrizio; Murray, Kermit K; Solouki, Touradj

2018-05-04

High resolving power ion mobility (IM) allows for accurate characterization of complex mixtures in high-throughput IM mass spectrometry (IM-MS) experiments. We previously demonstrated that pure component IM-MS data can be extracted from IM unresolved post-IM/collision-induced dissociation (CID) MS data using automated ion mobility deconvolution (AIMD) software [Matthew Brantley, Behrooz Zekavat, Brett Harper, Rachel Mason, and Touradj Solouki, J. Am. Soc. Mass Spectrom., 2014, 25, 1810-1819]. In our previous reports, we utilized a quadrupole ion filter for m/z-isolation of IM unresolved monoisotopic species prior to post-IM/CID MS. Here, we utilize a broadband IM-MS deconvolution strategy to remove the m/z-isolation requirement for successful deconvolution of IM unresolved peaks. Broadband data collection has throughput and multiplexing advantages; hence, elimination of the ion isolation step reduces experimental run times and thus expands the applicability of AIMD to high-throughput bottom-up proteomics. We demonstrate broadband IM-MS deconvolution of two separate and unrelated pairs of IM unresolved isomers (viz., a pair of isomeric hexapeptides and a pair of isomeric trisaccharides) in a simulated complex mixture. Moreover, we show that broadband IM-MS deconvolution improves high-throughput bottom-up characterization of a proteolytic digest of rat brain tissue. To our knowledge, this manuscript is the first to report successful deconvolution of pure component IM and MS data from an IM-assisted data-independent analysis (DIA) or HDMSE dataset.

Photoionization dynamics of ammonia (B(1)E''): dependence on ionizing photon energy and initial vibrational level.

PubMed

Hockett, Paul; Staniforth, Michael; Reid, Katharine L

2010-10-28

In this article we present photoelectron spectra and angular distributions in which ion rotational states are resolved. This data enables the comparison of direct and threshold photoionization techniques. We also present angle-resolved photoelectron signals at different total energies, providing a method to scan the structure of the continuum in the near-threshold region. Finally, we have studied the influence of vibrational excitation on the photoionization dynamics.

High-resolution Bent-crystal Spectrometer for the Ultra-soft X-ray Region

DOE R&D Accomplishments Database

Beiersdorfer, P.; von Goeler, S.; Bitter, M.; Hill, K. W.; Hulse, R. A.; Walling, R. S.

1988-10-01

A multichannel vacuum Brag-crystal spectrometer has been developed for high-resolution measurements of the line emission from tokamak plasmas in the wavelength region between 4 and 25 angstrom. The spectrometer employs a bent crystal in Johann geometry and a microchannel-plate intensified photodiode array. The instrument is capable of measuring high-resolution spectra (lambda/..delta..lambda approx. 3000) with fast time resolution (4 msec per spectrum) and good spatial resolution (3 cm). The spectral bandwidth is ..delta..lambda/lambda{sub 0} = 8 angstrom. A simple tilt mechanism allows access to different wavelength intervals. In order to illustrate the utility of the new spectrometer, time- and space-resolved measurements of the n = 3 to n = 2 spectrum of selenium from the Princeton Large Torus tokamak plasmas are presented. The data are used to determine the plasma transport parameters and to infer the radial distribution of fluorinelike, neonlike, and sodiumlike ions of selenium in the plasma. The new ultra-soft x-ray spectrometer has thus enabled us to demonstrate the utility of high-resolution L-shell spectroscopy of neonlike ions as a fusion diagnostic.

Location and ion-binding of membrane-associated valinomycin, a proton nuclear magnetic resonance study.

PubMed

Meers, P; Feigenson, G W

1988-03-03

Valinomycin, incorporated in small unilamellar vesicles of perdeuterated dimyristoylphosphatidylcholine, reveals several well-resolved 1H-NMR resonances. These resonances were used to examine the location, orientation and ion-binding of membrane-bound valinomycin. The order of affinity of membrane-bound valinomycin for cations is Rb+ greater than K+ greater than Cs+ greater than Ba2+, and binding is sensitive to surface change. The exchange between bound and free forms is fast on the NMR time scale. The intrinsic binding constants, extrapolated to zero anion concentration, are similar to those determined in aqueous solution. Rb+ and K+ show 1:1 binding to valinomycin, whereas the stoichiometry of Cs+ and Ba2+ is not certain. Paramagnetic chemical shift reagents and nitroxide spin label relaxation probes were used to study the location and orientation of valinomycin in the membrane. Despite relatively fast exchange of bound cations, the time average location of the cation-free form of valinomycin is deep within the bilayer under the conditions of these experiments. Upon complexation to K+, valinomycin moves closer to the interfacial region.