| 1. |
- Abelev, Betty, et al.
(författare)
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Long-range angular correlations on the near and away side in p-Pb collisions at root S-NN=5.02 TeV
- 2013
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Ingår i: Physics Letters. Section B: Nuclear, Elementary Particle and High-Energy Physics. - : Elsevier BV. - 0370-2693. ; 719:1-3, s. 29-41
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Tidskriftsartikel (refereegranskat)abstract
- Angular correlations between charged trigger and associated particles are measured by the ALICE detector in p-Pb collisions at a nucleon-nucleon centre-of-mass energy of 5.02 TeV for transverse momentum ranges within 0.5 < P-T,P-assoc < P-T,P-trig < 4 GeV/c. The correlations are measured over two units of pseudorapidity and full azimuthal angle in different intervals of event multiplicity, and expressed as associated yield per trigger particle. Two long-range ridge-like structures, one on the near side and one on the away side, are observed when the per-trigger yield obtained in low-multiplicity events is subtracted from the one in high-multiplicity events. The excess on the near-side is qualitatively similar to that recently reported by the CMS Collaboration, while the excess on the away-side is reported for the first time. The two-ridge structure projected onto azimuthal angle is quantified with the second and third Fourier coefficients as well as by near-side and away-side yields and widths. The yields on the near side and on the away side are equal within the uncertainties for all studied event multiplicity and p(T) bins, and the widths show no significant evolution with event multiplicity or p(T). These findings suggest that the near-side ridge is accompanied by an essentially identical away-side ridge. (c) 2013 CERN. Published by Elsevier B.V. All rights reserved.
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| 2. |
- Abelev, Betty, et al.
(författare)
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Measurement of prompt J/psi and beauty hadron production cross sections at mid-rapidity in pp collisions at root s=7 TeV
- 2012
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Ingår i: Journal of High Energy Physics. - 1029-8479. ; :11
-
Tidskriftsartikel (refereegranskat)abstract
- The ALICE experiment at the LHC has studied J/psi production at mid-rapidity in pp collisions at root s = 7 TeV through its electron pair decay on a data sample corresponding to an integrated luminosity L-int = 5.6 nb(-1). The fraction of J/psi from the decay of long-lived beauty hadrons was determined for J/psi candidates with transverse momentum p(t) > 1,3 GeV/c and rapidity vertical bar y vertical bar < 0.9. The cross section for prompt J/psi mesons, i.e. directly produced J/psi and prompt decays of heavier charmonium states such as the psi(2S) and chi(c) resonances, is sigma(prompt J/psi) (p(t) > 1.3 GeV/c, vertical bar y vertical bar < 0.9) = 8.3 +/- 0.8(stat.) +/- 1.1 (syst.)(-1.4)(+1.5) (syst. pol.) mu b. The cross section for the production of b-hadrons decaying to J/psi with p(t) > 1.3 GeV/c and vertical bar y vertical bar < 0.9 is a sigma(J/psi <- hB) (p(t) > 1.3 GeV/c, vertical bar y vertical bar < 0.9) = 1.46 +/- 0.38 (stat.)(-0.32)(+0.26) (syst.) mu b. The results are compared to QCD model predictions. The shape of the p(t) and y distributions of b-quarks predicted by perturbative QCD model calculations are used to extrapolate the measured cross section to derive the b (b) over bar pair total cross section and d sigma/dy at mid-rapidity.
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| 3. |
- Abelev, Betty, et al.
(författare)
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Underlying Event measurements in pp collisions at root s=0.9 and 7 TeV with the ALICE experiment at the LHC
- 2012
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Ingår i: Journal of High Energy Physics. - 1029-8479. ; :7
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Tidskriftsartikel (refereegranskat)abstract
- We present measurements of Underlying Event observables in pp collisions at root s = 0 : 9 and 7 TeV. The analysis is performed as a function of the highest charged-particle transverse momentum p(T),L-T in the event. Different regions are defined with respect to the azimuthal direction of the leading (highest transverse momentum) track: Toward, Transverse and Away. The Toward and Away regions collect the fragmentation products of the hardest partonic interaction. The Transverse region is expected to be most sensitive to the Underlying Event activity. The study is performed with charged particles above three different p(T) thresholds: 0.15, 0.5 and 1.0 GeV/c. In the Transverse region we observe an increase in the multiplicity of a factor 2-3 between the lower and higher collision energies, depending on the track p(T) threshold considered. Data are compared to PYTHIA 6.4, PYTHIA 8.1 and PHOJET. On average, all models considered underestimate the multiplicity and summed p(T) in the Transverse region by about 10-30%.
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| 4. |
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| 5. |
- Anderson, Emma K., 1986-, et al.
(författare)
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Fragmentation of and electron detachment from hot copper and silver dimer anions : A comparison
- 2023
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 107:6
-
Tidskriftsartikel (refereegranskat)abstract
- We measured the spontaneous decays of internally hot copper and silver dimer anions, and , stored in one of the two ion-beam storage rings of the Double Electrostatic Ion Ring Experiment (DESIREE) at Stockholm University. A coincidence detection technique was utilized enabling essentially background-free measurements of -> Cu + Cu- and -> Ag + Ag- fragmentation rates. Furthermore, the total rates of neutral decay products (monomers and dimers) were measured and the relative contributions of fragmentation and electron emission ( -> Cu2 + e- and -> Ag2 + e-) were deduced as functions of storage time. Fragmentation is completely dominant at early times. However, after about 20 ms of storage, electron emission is observed and becomes the leading decay path after 100 ms for both dimer anions. The branching ratios between fragmentation and electron emission (vibrationally assisted autodetachment processes) are very nearly the same for and Ag-2 throughout the present storage cycle of 10 seconds. This is surprising considering the difference between the electron affinities of the neutral dimers, Cu2 and Ag2, and the difference between the and the dissociation energies.
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| 6. |
- Anderson, Emma K., et al.
(författare)
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Spontaneous electron emission from hot silver dimer anions: Breakdown of the Born-Oppenheimer approximation
- 2020
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 124
-
Tidskriftsartikel (refereegranskat)abstract
- We report the first experimental evidence of spontaneous electron emission from a homonuclear dimer anion through direct measurements of Ag−2 → Ag2 + e− decays on milliseconds and seconds timescales. This observation is very surprising as there is no avoided crossing between adiabatic energy curves to mediate such a process. The process is weak, yet dominates the decay signal after 100 ms when ensembles of internally hot Ag−2 ions are stored in the cryogenic ion-beam storage ring, DESIREE, for 10 s. The electron emission process is associated with an instantaneous, very large reduction of the vibrational energy of the dimer system. This represents a dramatic deviation from a Born-Oppenheimer description of dimer dynamics.
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| 7. |
- Breznau, Nate, et al.
(författare)
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Observing many researchers using the same data and hypothesis reveals a hidden universe of uncertainty
- 2022
-
Ingår i: Proceedings of the National Academy of Sciences of the United States of America. - : National Academy of Sciences. - 0027-8424 .- 1091-6490. ; 119:44
-
Tidskriftsartikel (refereegranskat)abstract
- This study explores how researchers analytical choices affect the reliability of scientific findings. Most discussions of reliability problems in science focus on systematic biases. We broaden the lens to emphasize the idiosyncrasy of conscious and unconscious decisions that researchers make during data analysis. We coordinated 161 researchers in 73 research teams and observed their research decisions as they used the same data to independently test the same prominent social science hypothesis: that greater immigration reduces support for social policies among the public. In this typical case of social science research, research teams reported both widely diverging numerical findings and substantive conclusions despite identical start conditions. Researchers expertise, prior beliefs, and expectations barely predict the wide variation in research outcomes. More than 95% of the total variance in numerical results remains unexplained even after qualitative coding of all identifiable decisions in each teams workflow. This reveals a universe of uncertainty that remains hidden when considering a single study in isolation. The idiosyncratic nature of how researchers results and conclusions varied is a previously underappreciated explanation for why many scientific hypotheses remain contested. These results call for greater epistemic humility and clarity in reporting scientific findings.
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| 8. |
- Frazier-Wood, Alexis C., et al.
(författare)
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Genetic variants associated with subjective well-being, depressive symptoms, and neuroticism identified through genome-wide analyses
- 2016
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Ingår i: Nature Genetics. - : Nature Research (part of Springer Nature). - 1061-4036 .- 1546-1718. ; 48, s. 624-
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Tidskriftsartikel (refereegranskat)abstract
- Very few genetic variants have been associated with depression and neuroticism, likely because of limitations on sample size in previous studies. Subjective well-being, a phenotype that is genetically correlated with both of these traits, has not yet been studied with genome-wide data. We conducted genome-wide association studies of three phenotypes: subjective well-being (n = 298,420), depressive symptoms (n = 161,460), and neuroticism (n = 170,911). We identify 3 variants associated with subjective well-being, 2 variants associated with depressive symptoms, and 11 variants associated with neuroticism, including 2 inversion polymorphisms. The two loci associated with depressive symptoms replicate in an independent depression sample. Joint analyses that exploit the high genetic correlations between the phenotypes (vertical bar(p) over cap vertical bar approximate to 0.8) strengthen the overall credibility of the findings and allow us to identify additional variants. Across our phenotypes, loci regulating expression in central nervous system and adrenal or pancreas tissues are strongly enriched for association.
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| 9. |
- Schmidt-May, Alice F., 1988-, et al.
(författare)
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Observation of an isotope effect in state-selective mutual neutralization of lithium with hydrogen
- 2023
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 108:4
-
Tidskriftsartikel (refereegranskat)abstract
- We report on mutual neutralization measurements between 7Li+ and 1H- at effective center-of-mass collision energies in the range of 100 to 350 meV. We find that final states of lithium with principal quantum number n = 3 dominate with 3s separated from the unresolved 3p and 3d states. We measure the 3s branching fraction to be 0.665(12) at 100(16) meV and no significant dependence on collision energy is observed in the studied range. Comparing to previous results on mutual neutralization between 7Li+ and 2H- [G. Eklund et al., Phys. Rev. A 102, 012823 (2020)], we find that 7Li+ collisions with 1H- result in a significantly higher 3s branching fraction than collisions with 2H-. The difference is 0.087(14). The 3s branching fraction of 7Li+ + 1H- and the determined isotope difference are in agreement with results from extended full quantum calculations based on the same input data and numerical method as in Croft et al. [H. Croft, A. S. Dickinson, and F. X. Gadea, J. Phys. B 32, 81 (1999)]. These calculations reveal strong Stueckelberg oscillations of the 3s branching fraction for both isotopes.
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| 10. |
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| 11. |
- Schmidt-May, Alice F., 1988-, et al.
(författare)
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State-resolved mutual neutralization of 16O+ with 1H− and 2H− at collision energies below 100 meV
- 2024
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 109:5
-
Tidskriftsartikel (refereegranskat)abstract
- We measured the product-state distribution and its dependence on the hydrogen isotope for the mutual neutralization between 16O+ and 1,2H− at the double electrostatic ion-beam storage ring DESIREE for center-of-mass collision energies below 100 meV. We find at least six product channels into ground-state hydrogen and oxygen in different excited states. The majority of oxygen products populate terms corresponding to 2?22?3(4?∘)4? with 5S∘ as the main reaction product. We also observe product channels into terms corresponding to 2?22?3(4?)3?. Collisions with the heavier hydrogen isotope yield a branching into these lower excited states smaller than collisions with 1H−. The observed reaction products agree with the theoretical predictions. The detailed branching fractions, however, differ between the theoretical results, and none of them fully agree with the experiment.
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| 12. |
- Smith, Jennifer A, et al.
(författare)
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Genome-wide association study identifies 74 loci associated with educational attainment
- 2016
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Ingår i: Nature (London). - : Springer Science and Business Media LLC. - 1476-4687 .- 0028-0836. ; 533:7604, s. 539-542
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Tidskriftsartikel (refereegranskat)abstract
- Educational attainment is strongly influenced by social and other environmental factors, but genetic factors are estimated to account for at least 20% of the variation across individuals. Here we report the results of a genome-wide association study (GWAS) for educational attainment that extends our earlier discovery sample of 101,069 individuals to 293,723 individuals, and a replication study in an independent sample of 111,349 individuals from the UK Biobank. We identify 74 genome-wide significant loci associated with the number of years of schooling completed. Single-nucleotide polymorphisms associated with educational attainment are disproportionately found in genomic regions regulating gene expression in the fetal brain. Candidate genes are preferentially expressed in neural tissue, especially during the prenatal period, and enriched for biological pathways involved in neural development. Our findings demonstrate that, even for a behavioural phenotype that is mostly environmentally determined, a well-powered GWAS identifies replicable associated genetic variants that suggest biologically relevant pathways. Because educational attainment is measured in large numbers of individuals, it will continue to be useful as a proxy phenotype in efforts to characterize the genetic influences of related phenotypes, including cognition and neuropsychiatric diseases.
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| 13. |
- Thomas, Richard D., et al.
(författare)
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The double electrostatic ion ring experiment : A unique cryogenic electrostatic storage ring for merged ion-beams studies
- 2011
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Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 82:6, s. 065112-
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Tidskriftsartikel (refereegranskat)abstract
- We describe the design of a novel type of storage device currently under construction at Stockholm University, Sweden, using purely electrostatic focussing and deflection elements, in which ion beams of opposite charges are confined under extreme high vacuum cryogenic conditions in separate rings and merged over a common straight section. The construction of this double electrostatic ion ring experiment uniquely allows for studies of interactions between cations and anions at low and well-defined internal temperatures and centre-of-mass collision energies down to about 10 K and 10 meV, respectively. Position sensitive multi-hit detector systems have been extensively tested and proven to work in cryogenic environments and these will be used to measure correlations between reaction products in, for example, electron-transfer processes. The technical advantages of using purely electrostatic ion storage devices over magnetic ones are many, but the most relevant are: electrostatic elements which are more compact and easier to construct; remanent fields, hysteresis, and eddy-currents, which are of concern in magnetic devices, are no longer relevant; and electrical fields required to control the orbit of the ions are not only much easier to create and control than the corresponding magnetic fields, they also set no upper mass limit on the ions that can be stored. These technical differences are a boon to new areas of fundamental experimental research, not only in atomic and molecular physics but also in the boundaries of these fields with chemistry and biology. For examples, studies of interactions with internally cold molecular ions will be particular useful for applications in astrophysics, while studies of solvated ionic clusters will be of relevance to aeronomy and biology.
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| 14. |
- Zettergren, Henning, et al.
(författare)
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Roadmap on dynamics of molecules and clusters in the gas phase
- 2021
-
Ingår i: European Physical Journal D. - : Springer Science and Business Media LLC. - 1434-6060 .- 1434-6079. ; 75:5
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Tidskriftsartikel (refereegranskat)abstract
- This roadmap article highlights recent advances, challenges and future prospects in studies of the dynamics of molecules and clusters in the gas phase. It comprises nineteen contributions by scientists with leading expertise in complementary experimental and theoretical techniques to probe the dynamics on timescales spanning twenty order of magnitudes, from attoseconds to minutes and beyond, and for systems ranging in complexity from the smallest (diatomic) molecules to clusters and nanoparticles. Combining some of these techniques opens up new avenues to unravel hitherto unexplored reaction pathways and mechanisms, and to establish their significance in, e.g. radiotherapy and radiation damage on the nanoscale, astrophysics, astrochemistry and atmospheric science.
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| 15. |
- Zhu, Boxing, et al.
(författare)
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Radiative cooling of polyyne anions : C4H- and C6H-
- 2022
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 157:17
-
Tidskriftsartikel (refereegranskat)abstract
- Time-dependent photodetachment action spectra for the linear hydrocarbon anions C4H− and C6H− are investigated using the cryogenic Double ElectroStatic Ion Ring ExpEriment. The radiative cooling characteristics of these ions on the millisecond to seconds timescale are characterized by monitoring changes in their spectra as the ions cool by spontaneous infrared (IR) emission. The average cooling rates, extracted using Non-negative Matrix Factorization, are fit with 1/e lifetimes of 19 ± 2 and 3.0 ± 0.2 s for C4H− and C6H−, respectively. The cooling rates are successfully reproduced using a simple harmonic cascade model of IR emission. The ultraslow radiative cooling dynamics determined in this work provide important data for understanding the thermal cooling properties of linear hydrocarbon anions and for refining models of the formation and destruction mechanisms of these anions in astrochemical environments.
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| 16. |
- Anderson, Emma K., et al.
(författare)
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Decays of excited silver-cluster anions Agn, n=4 to 7, in the Double ElectroStatic Ion Ring ExpEriment
- 2018
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 98:2
-
Tidskriftsartikel (refereegranskat)abstract
- Spontaneous decays of small, hot silver-cluster anions Ag-n(-), n = 4-7, have been studied using one of the rings of the Double ElectroStatic Ion Ring ExpEriment (DESIREE). Observation of these decays over very long time scales is possible due to the very low residual gas pressure (similar to 10(-14)) and cryogenic (13 K) operation of DESIREE. The yield of neutral particles from stored beams of Ag-6(-) and Ag-2(-) anions were measured for 100 milliseconds and were found to follow single power-law behavior with millisecond time-scale exponential cutoffs. The Ag-4(-) and Ag-5(-) anions were stored for 60 s and the observed decays show two-component power-law behaviors. We present calculations of the rate constants for electron detachment from and fragmentation of Ag-4(-) and Ag-5(-). In these calculations, we assume that the internal energy distribution of the clusters are flat and with this we reproduce the early steep parts of the experimentally measured decay curves for Ag-4(-) and Ag-5(-) which extends to tens and hundreds of milliseconds, respectively. The fact that the calculations reproduce the early slopes of Ag-4(-) and Ag-5(-), which differ for the two cases, suggests that it is the changes in fragmentation rates with internal cluster energies of Ag-4(-) and Ag-5(-) rather than conditions in the ion source that determine this behavior. Comparisons with the measurements strongly suggest that the neutral particles detected in these time domains originate from Ag-4(-) -> Ag-3(-) + Ag and Ag-5(-) -> Ag-3(-) +Ag-2 fragmentation processes.
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| 17. |
- Anderson, Emma K., 1986-
(författare)
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DESIREE: Instrumentation Developments and Hot Metal Cluster Decays
- 2019
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This thesis presents instrumentation developments and measurements performed at the Double ElectroStatic Ion Ring ExpEriment, DESIREE, at Stockholm University. DESIREE operates at cryogenic temperatures ~13 K, with very low background pressures of ~10-14mbar, allowing the observation of stored ions to long times of tens of seconds and longer.Investigations into improving the count rate capability of the DESIREE detectors are presented. Microchannel plate (MCP) detectors are used for position sensitive particle counting in the DESIREE detector assemblies. In a cryogenic environment the operational resistance of MCPs is orders of magnitude higher than at room temperature and this limits the possible count rates. Novel low-resistance MCP detectors were investigated and resulted in the replacement of the MCPs in the DESIREE detector assemblies.DESIREE was used to measure spontaneous decays of hot, small cluster anions. The decays of small silver, copper and gold cluster anions are presented and compared to statistical model calculations. An experiment that is able to measure the proportion of spontaneous decay due to fragmentation or electron detachment in dimer anions of silver and copper is presented and significant, previously overlooked, contributions from electron detachment to the decay is identified. Furthermore, measurements of the stability and decay of small carbon cluster dianions are presented. These experiments utilised the aforementioned low-resistance MCPs.
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| 18. |
- Aumayr, Friedrich, et al.
(författare)
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Roadmap on photonic, electronic and atomic collision physics : III. Heavy particles
- 2019
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Ingår i: Journal of Physics B. - : IOP Publishing. - 0953-4075 .- 1361-6455. ; 52:17
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Tidskriftsartikel (refereegranskat)abstract
- We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. Roadmap III focusses on heavy particles: with zero to relativistic speeds. Modern theoretical and experimental approaches provide detailed insight into the wide range of many-body interactions involving projectiles and targets of varying complexity ranging from simple atoms, through molecules and clusters, complex biomolecules and nanoparticles to surfaces and crystals. These developments have been driven by technological progress and future developments will expand the horizon of the systems that can be studied. This Roadmap aims at looking back along the road, explaining the evolution of the field, and looking forward, collecting nineteen contributions from leading scientists in the field.
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| 19. |
- Barklem, Paul, et al.
(författare)
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Mutual Neutralization in Li++H−/D− and Na++H−/D− Collisions : Implications of Experimental Results for Non-LTE Modeling of Stellar Spectra
- 2021
-
Ingår i: Astrophysical Journal. - : American Astronomical Society. - 0004-637X .- 1538-4357. ; 908:2
-
Tidskriftsartikel (refereegranskat)abstract
- Advances in merged-beams instruments have allowed experimental studies of the mutual neutralization (MN) processes in collisions of both Li+ and Na+ ions with D− at energies below 1 eV. These experimental results place constraints on theoretical predictions of MN processes of Li+ and Na+ with H−, important for non-LTE modeling of Li and Na spectra in late-type stars. We compare experimental results with calculations for methods typically used to calculate MN processes, namely the full quantum (FQ) approach, and asymptotic model approaches based on the linear combination of atomic orbitals (LCAO) and semiempirical (SE) methods for deriving couplings. It is found that FQ calculations compare best overall with the experiments, followed by the LCAO, and the SE approaches. The experimental results together with the theoretical calculations, allow us to investigate the effects on modeled spectra and derived abundances and their uncertainties arising from uncertainties in the MN rates. Numerical experiments in a large grid of 1D model atmospheres, and a smaller set of 3D models, indicate that neglect of MN can lead to abundance errors of up to 0.1 dex (26%) for Li at low metallicity, and 0.2 dex (58%) for Na at high metallicity, while the uncertainties in the relevant MN rates as constrained by experiments correspond to uncertainties in abundances of much less than 0.01 dex (2%). This agreement for simple atoms gives confidence in the FQ, LCAO, and SE model approaches to be able to predict MN with the accuracy required for non-LTE modeling in stellar atmospheres.
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| 20. |
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| 21. |
- Bernard, Jérôme, et al.
(författare)
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Efficient radiative cooling of tetracene cations C18H12+ : absolute recurrent fluorescence rates as a function of internal energy
- 2023
-
Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 25:15, s. 10726-10740
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Tidskriftsartikel (refereegranskat)abstract
- We have measured recurrent fluorescence (RF) cooling rates of internally hot tetracene cations, C18H12+, as functions of their storage times and internal energies in two different electrostatic ion-beam storage rings – the cryogenic ring DESIREE with a circumference of 8.6 meters in Stockholm and the much smaller room temperature ring Mini-Ring in Lyon, which has a circumference of 0.71 meters. The RF rates were measured to be as high as 150 to 1000 s−1 for internal energies in the 7 to 9.4 eV energy range, where we have probed the time evolution of the internal energy distribution with nanosecond laser pulses with a 1 kHz repetition rate. These RF rates are found to be significantly higher than those of previously investigated smaller PAHs such as e.g. anthracene and naphthalene, for which the lowest non-forbidden electronic excited state, the D2 state, is populated with a smaller probability by inverse internal conversion. Furthermore, the D2–D0 transition rate is smaller for these smaller molecules than for tetracene. The complementary features of the two storage rings allow for RF rate measurements in a broader internal energy range than has been possible before. The smaller sampling period of about 6 μs in Mini-Ring is ideal to study the cooling dynamics of the hotter ions that decay fast, whereas DESIREE with a sampling period of about 60 μs is better suited to study the colder ions that decay on longer timescales ranging up to hundreds of milliseconds. The excellent agreement between the two series of measurements in the region where they overlap demonstrates the complementarity of the two electrostatic ion-beam storage rings.
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| 22. |
- Bernigaud, Virgile, et al.
(författare)
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Electron capture-induced dissociation of AK dipeptide dications : Influence of ion velocity, crown-ether complexation and collision gas
- 2008
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Ingår i: International Journal of Mass Spectrometry. - : Elsevier BV. - 1387-3806 .- 1873-2798. ; 276:2-3, s. 77-81
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Tidskriftsartikel (refereegranskat)abstract
- The fragmentation of doubly protonated AK dipeptide ions has been investigated after collisional electron transfer. Electron capture leads to three dominant channels, H loss, NH3 loss, and N–Cα bond breakage to give either c+ or z+ fragment ions. The relative importance of these channels has been explored as a function of ion velocity, the degree of complexation with crown ether, and collision gas. Our results indicate that H loss and NH3 loss are competing channels whereas the probability of N–Cα bond breakage is more or less constant.
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| 23. |
- Bogot, Alon, et al.
(författare)
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The mutual neutralization of hydronium and hydroxide
- 2024
-
Ingår i: Science. - 0036-8075 .- 1095-9203. ; 383:6680, s. 285-289
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Tidskriftsartikel (refereegranskat)abstract
- Mutual neutralization of hydronium (H3O+) and hydroxide (OH−) ions is a very fundamental chemical reaction. Yet, there is only limited experimental evidence about the underlying reaction mechanisms. Here, we report three-dimensional imaging of coincident neutral products of mutual-neutralization reactions at low collision energies of cold and isolated ions in the cryogenic double electrostatic ion-beam storage ring (DESIREE). We identified predominant H2O + OH + H and 2OH + H2 product channels and attributed them to an electron-transfer mechanism, whereas a minor contribution of H2O + H2O with high internal excitation was attributed to proton transfer. The reported mechanism-resolved internal product excitation, as well as collision-energy and initial ion-temperature dependence, provide a benchmark for modeling charge-transfer mechanisms.
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| 24. |
- Bull, James N., et al.
(författare)
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Ultraslow radiative cooling of Cn- (n=3-5)
- 2019
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 151:11
-
Tidskriftsartikel (refereegranskat)abstract
- Ultraslow radiative cooling lifetimes and adiabatic detachment energies for three astrochemically relevant anions, Cn- (n = 3-5), are measured using the Double ElectroStatic Ion Ring ExpEriment (DESIREE) infrastructure at Stockholm University. DESIREE maintains a background pressure of approximate to 10(-14) mbar and temperature of approximate to 13 K, allowing storage of mass-selected ions for hours and providing conditions coined a molecular cloud in a box. Here, we construct two-dimensional (2D) photodetachment spectra for the target anions by recording photodetachment signal as a function of irradiation wavelength and ion storage time (seconds to minute time scale). Ion cooling lifetimes, which are associated with infrared radiative emission, are extracted from the 2D photodetachment spectrum for each ion by tracking the disappearance of vibrational hot-band signal with ion storage time, giving 1e cooling lifetimes of 3.1 +/- 0.1 s (C3-), 6.8 +/- 0.5 s (C4-), and 24 +/- 5 s (C5-). Fits of the photodetachment spectra for cold ions, i.e., those stored for at least 30 s, provide adiabatic detachment energies in good agreement with values from laser photoelectron spectroscopy on jet-cooled anions, confirming that radiative cooling has occurred in DESIREE. Ion cooling lifetimes are simulated using a simple harmonic cascade model, finding good agreement with experiment and providing a mode-by-mode understanding of the radiative cooling properties. The 2D photodetachment strategy and radiative cooling modeling developed in this study could be applied to investigate the ultraslow cooling dynamics of a wide range of molecular anions.
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| 25. |
- Chartkunchand, Kiattichart C., et al.
(författare)
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Dianion diagnostics in DESIREE : High-sensitivity detection of C-n(2-) from a sputter ion source
- 2018
-
Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 89:3
-
Tidskriftsartikel (refereegranskat)abstract
- A sputter ion source with a solid graphite target has been used to produce dianions with a focus on carbon cluster dianions, C-n(2-), with n = 7-24. Singly and doubly charged anions from the source were accelerated together to kinetic energies of 10 keV per atomic unit of charge and injected into one of the cryogenic (13 K) ion-beam storage rings of the Double ElectroStatic Ion Ring Experiment facility at Stockholm University. Spontaneous decay of internally hot C-n(2-) dianions injected into the ring yielded C-n(2-) anions with kinetic energies of 20 keV, which were counted with a microchannel plate detector. Mass spectra produced by scanning the magnetic field of a 90 degrees analyzing magnet on the ion injection line reflect the production of internally hot C-7(2-) - C-24(2-) dianions with lifetimes in the range of tens of microseconds to milliseconds. In spite of the high sensitivity of this method, no conclusive evidence of C-6(2-) was found while there was a clear C-7(2-) signal with the expected isotopic distribution. This is consistent with earlier experimental studies and with theoretical predictions. An upper limit is deduced for a C-6(2-) signal that is two orders-of-magnitude smaller than that for C-7(2-). In addition, CnO2- and CnCu2- dianions were detected.
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| 26. |
- Chartkunchand, Kiattichart C., et al.
(författare)
-
Radiative lifetimes of the bound excited states of Pt-
- 2016
-
Ingår i: Physical Review A - Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 94:3
-
Tidskriftsartikel (refereegranskat)abstract
- © 2016 American Physical Society.The intrinsic radiative lifetimes of the 5d106sS1/22 and 5d96s2 D3/22 bound excited states in the platinum anion Pt- have been studied at cryogenic temperatures at the Double ElectroStatic Ion Ring Experiment (DESIREE) facility at Stockholm University. The intrinsic lifetime of the higher-lying 5d106s S1/22 state was measured to be 2.54±0.10s, while only a lifetime in the range of 50-200 ms could be estimated for the 5d96s2 D3/22 fine-structure level. The storage lifetime of the Pt- ion beam was measured to be a little over 15 min at a ring temperature of 13K. The present study reports the lifetime of an atomic negative ion in an excited bound state with an electron configuration different from that of the ground state.
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| 27. |
- Chen, Tao, et al.
(författare)
-
Absolute fragmentation cross sections in atom-molecule collisions : Scaling laws for non-statistical fragmentation of polycyclic aromatic hydrocarbon molecules
- 2014
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 140:22
-
Tidskriftsartikel (refereegranskat)abstract
- We present scaling laws for absolute cross sections for non-statistical fragmentation in collisions between Polycyclic Aromatic Hydrocarbons (PAH/PAH(+)) and hydrogen or helium atoms with kinetic energies ranging from 50 eV to 10 keV. Further, we calculate the total fragmentation cross sections (including statistical fragmentation) for 110 eV PAH/PAH(+) + He collisions, and show that they compare well with experimental results. We demonstrate that non-statistical fragmentation becomes dominant for large PAHs and that it yields highly reactive fragments forming strong covalent bonds with atoms (H and N) and molecules (C6H5). Thus nonstatistical fragmentation may be an effective initial step in the formation of, e. g., Polycyclic Aromatic Nitrogen Heterocycles (PANHs). This relates to recent discussions on the evolution of PAHNs in space and the reactivities of defect graphene structures.
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| 28. |
- Chen, Tao, et al.
(författare)
-
Formation of H2 from internally heated polycyclic aromatic hydrocarbons : Excitation energy dependence
- 2015
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 142:14
-
Tidskriftsartikel (refereegranskat)abstract
- We have investigated the effectiveness of molecular hydrogen (H-2) formation from Polycyclic Aromatic Hydrocarbons (PAHs) which are internally heated by collisions with keV ions. The present and earlier experimental results are analyzed in view of molecular structure calculations and a simple collision model. We estimate that H-2 formation becomes important for internal PAH temperatures exceeding about 2200 K, regardless of the PAH size and the excitation agent. This suggests that keV ions may effectively induce such reactions, while they are unlikely due to, e.g., absorption of single photons with energies below the Lyman limit. The present analysis also suggests that H-2 emission is correlated with multi-fragmentation processes, which means that the [PAH-2H](+) peak intensities in the mass spectra may not be used for estimating H-2-formation rates.
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| 29. |
- de Ruette, Nathalie, et al.
(författare)
-
DESIREE electrospray ion source test bench and setup for collision induced dissociation experiments
- 2018
-
Ingår i: Review of Scientific Instruments. - : AIP Publishing. - 0034-6748 .- 1089-7623. ; 89:7
-
Tidskriftsartikel (refereegranskat)abstract
- In this paper, we give a detailed description of an electrospray ion source test bench and a single-pass setup for ion fragmentation studies at the Double ElectroStatic Ion Ring ExpEriment infrastructure at Stockholm University. This arrangement allows for collision-induced dissociation experiments at the center-of-mass energies between 10 eV and 1 keV. Charged fragments are analyzed with respect to their kinetic energies (masses) by means of an electrostatic energy analyzer with a wide angular acceptance and adjustable energy resolution.
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| 30. |
- Eklund, Gustav, et al.
(författare)
-
Cryogenic merged-ion-beam experiments in DESIREE : Final-state-resolved mutual neutralization of Li+ and D-
- 2020
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society (APS). - 2469-9926 .- 2469-9934. ; 102:1
-
Tidskriftsartikel (refereegranskat)abstract
- We have developed an experimental technique to study charge-and energy-flow processes in sub-eV collisions between oppositely charged, internally cold, ions of atoms, molecules, and clusters. Two ion beams are stored in separate rings of the cryogenic ion-beam storage facility DESIREE, and merged in a common straight section where a set of biased drift tubes is used to control the center-of-mass collision energy locally in fine steps. Here, we present measurements on mutual neutralization between Li+ and D- where a time-sensitive imaging-detector system is used to measure the three-dimensional distance between the neutral Li and D atoms as they reach the detector. This scheme allows for direct measurements of kinetic-energy releases, and here it reveals separate populations of the 3s state and the (3p + 3d) states in neutral Li while the D atom is left in its ground state 1s. The branching fraction of the 3s final state is measured to be 57.8 +/- 0.7% at a center-of-mass collision energy of 78 +/- 13 meV. The technique paves the way for studies of charge-, energy-, and mass-transfer reactions in single collisions involving molecular and cluster ions in well-defined quantum states.
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| 31. |
- Eklund, Gustav, 1990-, et al.
(författare)
-
Experimental lifetime of the a1Δ electronically excited state of CH−
- 2022
-
Ingår i: Physical Review Research. - : American Physical Society (APS). - 2643-1564. ; 4:1
-
Tidskriftsartikel (refereegranskat)abstract
- By repeatedly probing the a1Δ excited state and the X3Σ− ground-state populations in a beam of CH− ions stored in a cryogenic ion-beam storage ring for 100 s, we extract an intrinsic lifetime of 14.9±0.5 s for this excited state. This is far longer than all earlier experimental and theoretical results, exposing large difficulties in measuring and calculating slow decays and the need for benchmark quality experiments.
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| 32. |
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| 33. |
- Eklund, Gustav, et al.
(författare)
-
Final-state-resolved mutual neutralization of Na+ and D-
- 2021
-
Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 103:3
-
Tidskriftsartikel (refereegranskat)abstract
- The present paper reports on a merged-beam experiment on mutual neutralization between Na+ and D-. For this experiment, we have used the DESIREE ion-beams storage-ring facility. The reaction products are detected using a position- and time-sensitive detector, which ideally allows for determination of the population of each individual quantum state in the final atomic systems. Here, the 4s, 3d, and 4p final states in Na are observed and in all cases the D atom is in its ground state 1s S-2. The respective branching fractions of the states populated in Na are determined by fitting results from a Monte Carlo simulation of the experiment to the measured data. The center-of-mass collision energy is controlled using a set of biased drift tubes, and the branching fractions are measured for energies between 80 meV and 393 meV. The resulting branching fractions are found to agree qualitatively with the only available theoretical calculations for this particular system, which are based on a multichannel Landau-Zener approach using dynamic couplings determined with a linear combination of atomic orbitals model.
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| 34. |
- Gatchell, Michael, 1988-
(författare)
-
Collision Induced Fragmentation of Molecules and Molecular Clusters : Knockout Driven Reactions in Fullerenes and PAHs
- 2014
-
Licentiatavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This licentiate thesis covers experimental and theoretical studies of the fragmentation and sub- sequent reactions of fullerenes or Polycyclic Aromatic Hydrocarbons (PAHs). I present results from experiments where atoms or ions collide with fullerenes, PAHs, or clusters of these mole- cules at energies from 100 eV up to tens of keV.The results of these experiments are interpreted using quantum chemical calculations, mol- ecular dynamics simulations, and a stopping model that we have developed. With these models I show that different energy transfer processes dominate at different collision energies, from nuclear stopping in low energy (~ 100 eV) collisions to electronic stopping at higher energies (~ 10 keV). I particularly focus on non-statistical fragmentation induced by nuclear stopping which can lead to the formation of exotic new species such as the odd-numbered C119 fullerene- like molecule.
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| 35. |
- Gatchell, Michael, et al.
(författare)
-
Commissioning of the DESIREE storage rings - a new facility for cold ion-ion collisions
- 2014
-
Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488:1
-
Konferensbidrag (refereegranskat)abstract
- We report on the ongoing commissioning of the Double ElectroStatic Ion Ring ExpEriment, DESIREE, at Stockholm University. Beams of atomic carbon anions (C-) and smaller carbon anion molecules (C-2(-), C-3(-), C-4(-) etc.) have been produced in a sputter ion source, accelerated to 10 keV or 20 keV, and stored successfully in the two electrostatic rings. The rings are enclosed in a common vacuum chamber cooled to below 13 Kelvin. The DESIREE facility allows for studies of internally relaxed single isolated atomic, molecular and cluster ions and for collision experiments between cat-and anions down to very low center-of-mass collision energies (meV scale). The total thermal load of the vacuum chamber at this temperature is measured to be 32 W. The decay rates of stored ion beams have two components: a non-exponential component caused by the space charge of the beam itself which dominates at early times and an exponential term from the neutralization of the beam in collisions with residual gas at later times. The residual gas limited storage lifetime of carbon anions in the symmetric ring is over seven minutes while the 1/e lifetime in the asymmetric ring is measured to be about 30 seconds. Although we aim to improve the storage in the second ring, the number of stored ions are now sufficient for many merged beams experiments with positive and negative ions requiring milliseconds to seconds ion storage.
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| 36. |
- Gatchell, Michael, et al.
(författare)
-
Failure of hydrogenation in protecting polycyclic aromatic hydrocarbons from fragmentation
- 2015
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 92:5
-
Tidskriftsartikel (refereegranskat)abstract
- A recent study of soft x-ray absorption in native and hydrogenated coronene cations, C24H12+m + m = 0-7, led to the conclusion that additional hydrogen atoms protect (interstellar) polycyclic aromatic hydrocarbon (PAH) molecules from fragmentation [Reitsma et al., Phys. Rev. Lett. 113, 053002 (2014)]. The present experiment with collisions between fast (30-200 eV) He atoms and pyrene (C16H10+m +, m = 0, 6, and 16) and simulations without reference to the excitation method suggests the opposite. We find that the absolute carbon-backbone fragmentation cross section does not decrease but increases with the degree of hydrogenation for pyrene molecules.
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| 37. |
- Gatchell, Michael, et al.
(författare)
-
First results from the Double ElectroStatic Ion-Ring ExpEriment, DESIREE
- 2014
-
Ingår i: XXVIII International Conference on Photonic, Electronic and Atomic Collisions (ICPEAC 2013). - : Institute of Physics (IOP). ; 488
-
Konferensbidrag (refereegranskat)abstract
- We have stored the first beams in one of the rings of the double electrostatic ion-storage ring, DESIREE at cryogenic and at room temperature conditions. At cryogenic operations the following parameters are found. Temperature; T= 13K, pressure; p <10(-13) mbar, initial number of stored ions; N > 10(7) and storage lifetime of a C-2(-) beam; tau = 450 S.
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| 38. |
- Gatchell, Michael, et al.
(författare)
-
Ions colliding with mixed clusters of C-60 and coronene : Fragmentation and bond formation
- 2014
-
Ingår i: Physical Review A. Atomic, Molecular, and Optical Physics. - 1050-2947 .- 1094-1622. ; 90:2
-
Tidskriftsartikel (refereegranskat)abstract
- We have studied collisions between 22.5 keV He2+ ions and mixed clusters [(C-60)(m)(C24H12)(n)] of m C-60 and n coronene molecules where m and n range up to about ten. Surprisingly, the cluster fragmentation behavior in distant collisions is dramatically different for pure coronene clusters (m = 0) and clusters containing a single C-60 molecule (m = 1). In the latter case, the clusters may be ionized without also being fragmented on the experimental time scale of tens of microseconds. This does not occur for pure coronene clusters, but is a main characteristic of pure fullerene clusters. For ion trajectories penetrating the mixed cluster, we observe covalent bond formations between C-59 or C-58 and C-60, but not between coronene fragments and C-60, or between C-60 fragments and coronene. These results are explained by means of classical molecular dynamics simulations of collisions inside the fragmenting mixed clusters.
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| 39. |
- Gatchell, Michael, et al.
(författare)
-
Ions colliding with polycyclic aromatic hydrocarbon clusters
- 2013
-
Ingår i: Physica Scripta. - 0031-8949 .- 1402-4896. ; T156, s. 014062-
-
Tidskriftsartikel (refereegranskat)abstract
- We have measured the ionization and fragmentation of polycyclic aromatic hydrocarbon (PAH) molecules and their clusters. We find that PAH clusters containing up to roughly 100 individual molecules fragment strongly following collisions with keV ions in low or high charge states (q). For both types of collisions, singly charged PAH molecules are found to be the dominant products but for very different reasons. A high-q ion projectile charge leads to strong multiple ionization of the PAH clusters and subsequent Coulomb explosions. A low-q ion projectile charge often leads to single ionization but stronger internal heating and long evaporation sequences with a singly charged PAH monomer as the end product. We have developed a Monte Carlo method for collision-induced heating of PAH clusters and present an evaporation model where the clusters cool slowly as most of the internal energies are stored in intramolecular vibrations and not in molecule-molecule vibrations.
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| 40. |
- Gatchell, Michael, 1988-
(författare)
-
Molecular Hole Punching : Impulse Driven Reactions in Molecules and Molecular Clusters
- 2016
-
Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- When molecules are excited by photons or energetic particles, they will cool through the emission of photons, electrons, or by fragmenting. Such processes are often thermal as they occur after the excitation energy has been redistributed across all degrees-of-freedom in the system. Collisions with atoms or ions may also lead to ultrafast fragmentation in Rutherford-like scattering processes, where one or several atoms can literally be knocked out of the molecule by the incoming projectile before the energy can be completely redistributed. The resulting fragmentation pathways can in such knockout processes be very different from those in thermal processes.This thesis covers extensive studies of collisions between ions/atoms and isolated Polycyclic Aromatic Hydrocarbon (PAH) molecules, isolated fullerene molecules, or clusters of these. The high stabilities and distinct fragmentation channels make these types of molecules excellent test cases for characterizing knockout-driven fragmentation and the reactions that these processes can lead to. I will present experimental measurements for a wide range of energies and compare them with my own molecular dynamics simulations and quantum chemical calculations. In this thesis, I present an in-depth study of the role of knockout in the energetic processing of molecules and clusters. The competition between knockout and thermally driven fragmentation is discussed in detail.Knockout-driven fragmentation is shown to result in exotic fragments that are far more reactive than the intact parent molecules or fragments from thermal processes. When such reactive species are formed within molecular clusters efficient molecular growth can take place on sub-picosecond timescales. The cluster environments are crucial here because they protect the newly formed molecules by absorbing excess energy. This is a possible pathway for the growth of large PAHs, fullerenes, and similar carbonaceous complexes found in, for instance, the interstellar medium.
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| 41. |
- Gatchell, Michael, et al.
(författare)
-
Non-statistical fragmentation of PAHs and fullerenes in collisions with atoms
- 2014
-
Ingår i: International Journal of Mass Spectrometry. - : Elsevier BV. - 1387-3806 .- 1873-2798. ; 365, s. 260-265
-
Tidskriftsartikel (refereegranskat)abstract
- Non-statistical fragmentation processes may be important when Polycyclic Aromatic Hydrocarbon molecules (PAHs), fullerenes, or other large complex molecules collide with atoms and atomic ions. For collisions with hydrogen or helium this occurs for center-of-mass energies between a few tens to a few hundreds of electron volts and typically results in losses of single atoms. In such processes one forms much more reactive fragments than in statistical fragmentation, which instead are dominated by losses of C2- or C2H2-molecules (H-atoms) from fullerenes and PAHs, respectively. An enhanced reactivity has recently been demonstrated for van der Waals clusters of C60 molecules where prompt knockouts of single C-atoms from one of the fullerenes yield highly reactive C59+ fragments, which easily form covalent bonds with a C60 molecule inside the clusters
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| 42. |
- Gatchell, Michael, 1988-, et al.
(författare)
-
Stability of C59 Knockout Fragments from Femtoseconds to Infinity
-
Annan publikation (övrigt vetenskapligt/konstnärligt)abstract
- We have studied the stability of C59 anions as a function of time, from their formation on femtosecond timescales to their stabilization on second timescales and beyond, using a combination of theory and experiments. The C59 fragments were produced in collisions between C60 fullerene anions and neutral helium gas at a velocity of 90 km/s (corresponding to a collision energy of 166 eV in the center-of-mass frame). The fragments were then stored in a cryogenic ion-beam storage ring at the DESIREE facility where they were followed for up to one minute. Classical molecular dynamics simulations were used to determine the reaction cross section and the excitation energy distributions of the products formed in these collisions. We found that about 15 percent of the C59 ions initially stored in the ring are intact after about 100 ms, and that this population then remains intact indefinitely. This means that C60 fullerenes exposed to energetic atoms and ions, such as stellar winds and shock waves, will produce stable, highly reactive products, like C59, that are fed into interstellar chemical reaction networks.
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| 43. |
- Gatchell, Michael, 1988-, et al.
(författare)
-
Stability of C59 Knockout Fragments from Femtoseconds to Infinity
- 2024
-
Ingår i: Astrophysical Journal. - 0004-637X .- 1538-4357. ; 966:2
-
Tidskriftsartikel (refereegranskat)abstract
- We have studied the stability of C59 anions as a function of time, from their formation on femtosecond timescales to their stabilization on second timescales and beyond, using a combination of theory and experiments. The C-59 fragments were produced in collisions between C60 fullerene anions and neutral helium gas at a velocity of 90 km s−1 (corresponding to a collision energy of 166 eV in the center-of-mass frame). The fragments were then stored in a cryogenic ion beam storage ring at the DESIREE facility, where they were followed for up to 1 minute. Classical molecular dynamics simulations were used to determine the reaction cross section and the excitation energy distributions of the products formed in these collisions. We find that about 15% of the C-59 ions initially stored in the ring are intact after about 100 ms and that this population then remains intact indefinitely. This means that C60 fullerenes exposed to energetic atoms and ions, such as stellar winds and shock waves, will produce stable, highly reactive products, like C59, that are fed into interstellar chemical reaction networks.
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| 44. |
- Gatchell, Michael, et al.
(författare)
-
Survival of polycyclic aromatic hydrocarbon knockout fragments in the interstellar medium
- 2021
-
Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 12:1
-
Tidskriftsartikel (refereegranskat)abstract
- Laboratory studies play a crucial role in understanding the chemical nature of the interstellar medium (ISM), but the disconnect between experimental timescales and the timescales of reactions in space can make a direct comparison between observations, laboratory, and model results difficult. Here we study the survival of reactive fragments of the polycyclic aromatic hydrocarbon (PAH) coronene, where individual C atoms have been knocked out of the molecules in hard collisions with He atoms at stellar wind and supernova shockwave velocities. Ionic fragments are stored in the DESIREE cryogenic ion-beam storage ring where we investigate their decay for up to one second. After 10 ms the initially hot stored ions have cooled enough so that spontaneous dissociation no longer takes place at a measurable rate; a majority of the fragments remain intact and will continue to do so indefinitely in isolation. Our findings show that defective PAHs formed in energetic collisions with heavy particles may survive at thermal equilibrium in the interstellar medium indefinitely, and could play an important role in the chemistry in there, due to their increased reactivity compared to intact or photo-fragmented PAHs. Ion storage rings allow reactions to be studied over orders of magnitude in time, bridging the gap between typical experimental and astronomical timescales. Here the authors observe that polycyclic aromatic hydrocarbon fragments produced upon collision with He atoms at velocities typical of stellar winds and supernova shockwaves remain intact up to second timescales, thus may play an important role in interstellar chemistry.
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| 45. |
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| 46. |
- Giacomozzi, Linda, et al.
(författare)
-
Decay pathways for protonated and deprotonated adenine molecules
- 2019
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 151:4
-
Tidskriftsartikel (refereegranskat)abstract
- We have measured fragment mass spectra and total destruction cross sections for protonated and deprotonated adenine following collisions with He at center-of-mass energies in the 20-240 eV range. Classical and ab initio molecular dynamics simulations are used to provide detailed information on the fragmentation pathways and suggest a range of alternative routes compared to those reported in earlier studies. These new pathways involve, for instance, losses of HNC molecules from protonated adenine and losses of NH2 or C3H2N2 from deprotonated adenine. The present results may be important to advance the understanding of how biomolecules may be formed and processed in various astrophysical environments.
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| 47. |
- Giacomozzi, Linda, et al.
(författare)
-
Knockout driven fragmentation of porphyrins
- 2017
-
Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry (RSC). - 1463-9076 .- 1463-9084. ; 19:30, s. 19750-19755
-
Tidskriftsartikel (refereegranskat)abstract
- We have studied collisions between tetraphenylporphyrin cations and He or Ne at center-of-mass energies in the range 50-110 eV. The experimental results were interpreted in view of density functional theory calculations of dissociation energies and classical molecular dynamics simulations of how the molecules respond to the He/Ne impact. We demonstrate that prompt atom knockout strongly contributes to the total destruction cross sections. Such impulse driven processes typically yield highly reactive fragments and are expected to be important for collisions with any molecular system in this collision energy range, but have earlier been very difficult to isolate for biomolecules.
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| 48. |
- Gnaser, H., et al.
(författare)
-
Spontaneous and photo-induced decay processes of WF5- and HfF5- molecular anions in a cryogenic storage ring
- 2022
-
Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 157:4
-
Tidskriftsartikel (refereegranskat)abstract
- Spontaneous and photo-induced decay processes of HfF5- and WF5- molecular anions were investigated in the Double ElectroStatic Ion Ring ExpEriment (DESIREE). The observation of these reactions over long time scales (several tens of ms) was possible due to the cryogenic temperatures (13 K) and the extremely low residual gas pressure (similar to 10(-14) mbar) of DESIREE. For photo-induced reactions, laser wavelengths in the range 240 to 450 nm were employed. Both anion species were found to undergo spontaneous decay via electron detachment or fragmentation. After some ms, radiative cooling processes were observed to lower the probability for further decay through these processes. Photo-induced reactions indicate the existence of an energy threshold for WF5- anions at about 3.5 eV, above which the neutralization yield increases strongly. By contrast, HfF5- ions exhibit essentially no enhanced production of neutrals upon photon interaction, even for the highest photon energy used in this experiment (similar to 5.2 eV). This suppression will be highly beneficial for the efficient detection, in accelerator mass spectrometry, of the extremely rare isotope Hf-182 using the Hf-182-F-5(-) anion while effectively reducing the interfering stable isobar W-182 in the analyte ion (WF5-)-W-182. The radionuclide Hf-182 is of great relevance in astrophysical environments as it constitutes a potential candidate to study the events of nucleosynthesis that may have taken place in the vicinity of the solar system several million years Published under an exclusive license by AIP Publishing.
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| 49. |
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| 50. |
- Grumer, Jon, et al.
(författare)
-
State-Resolved Mutual Neutralization of Mg+ and D-
- 2022
-
Ingår i: Physical Review Letters. - : American Physical Society. - 0031-9007 .- 1079-7114. ; 128:3
-
Tidskriftsartikel (refereegranskat)abstract
- We present experimental final-state distributions for Mg atoms formed in Mg+ + D- mutual neutralization reactions at center-of-mass collision energies of 59 +/- 12 meV by using the merged-beams method. Comparisons with available full-quantum results reveal large discrepancies and a previously underestimated total rate coefficient by up to a factor of 2 in the 0-1 eV (< 10(4) K) regime. Asymptotic model calculations arc shown to describe the process much better and we recommend applying this method to more complex iron group systems; data that is of urgent need in stellar spectral modeling.
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