| 1. |
- Bogot, Alon, et al.
(författare)
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The mutual neutralization of hydronium and hydroxide
- 2024
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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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| 2. |
- Eklund, Gustav, et al.
(författare)
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Cryogenic merged-ion-beam experiments in DESIREE : Final-state-resolved mutual neutralization of Li+ and D-
- 2020
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society (APS). - 2469-9926 .- 2469-9934. ; 102:1
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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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| 3. |
- Eklund, Gustav, 1990-
(författare)
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Experiments on mutual neutralization using storage rings with merged ion beams
- 2020
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- This thesis presents work on merged-beams experiments using the DESIREE facility, which consists of two electrostatic ion-storage rings operated at cryogenic temperatures of about 13 K. The two storage rings have a common straight section, where oppositely charged ions can interact at sub-eV collision energies. The work consists of development of the experimental method, tools for data analysis, and simulations for interpretation of the experimental results. This development has led to the first results from merged-beams experiments at DESIREE. The experiments are performed on mutual neutralization, a collision process where an electron is transferred from a negatively charged ion to a positively charged ion, resulting in two neutral products. This reaction is investigated for three systems: Li+ with D−, Na+ with D−, and Mg+ with D−. The reactions studied are of astrophysical interest, in particular for modeling of stellar atmospheres. The detection of the reaction products is done by using a position- and time-sensitive detector, and from this information it is possible to determine the quantum states involved in the reaction. The branching fractions of the reaction channels are measured and compared to theoretical modeling.
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| 4. |
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| 5. |
- Eklund, Gustav, et al.
(författare)
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Final-state-resolved mutual neutralization of Na+ and D-
- 2021
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - : American Physical Society. - 2469-9926 .- 2469-9934. ; 103:3
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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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| 6. |
- Gatchell, Michael, 1988-, et al.
(författare)
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Stability of C59 Knockout Fragments from Femtoseconds to Infinity
- 2024
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Ingår i: Astrophysical Journal. - 0004-637X .- 1538-4357. ; 966:2
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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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| 7. |
- Gatchell, Michael, et al.
(författare)
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Survival of polycyclic aromatic hydrocarbon knockout fragments in the interstellar medium
- 2021
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Ingår i: Nature Communications. - : Springer Science and Business Media LLC. - 2041-1723. ; 12:1
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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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| 8. |
- Gnaser, H., et al.
(författare)
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Spontaneous and photo-induced decay processes of WF5- and HfF5- molecular anions in a cryogenic storage ring
- 2022
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Ingår i: Journal of Chemical Physics. - : AIP Publishing. - 0021-9606 .- 1089-7690. ; 157:4
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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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| 9. |
- Grumer, Jon, et al.
(författare)
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State-Resolved Mutual Neutralization of Mg+ and D-
- 2022
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Ingår i: Physical Review Letters. - : American Physical Society. - 0031-9007 .- 1079-7114. ; 128:3
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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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| 10. |
- Grumer, Jon, et al.
(författare)
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State-Resolved Mutual Neutralization of Mg+ and D−
- 2022
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 128:3
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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 (<104 K) regime. Asymptotic model calculations are 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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