| 1. |
- 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
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 107:6
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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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| 2. |
- 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
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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. ; 108:4
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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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| 3. |
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| 4. |
- 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
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Ingår i: Physical Review A: covering atomic, molecular, and optical physics and quantum information. - 2469-9926 .- 2469-9934. ; 109:5
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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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| 5. |
- 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
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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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| 6. |
- 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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| 7. |
- Gatchell, Michael, 1988-, et al.
(författare)
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Stability of C59 Knockout Fragments from Femtoseconds to Infinity
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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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| 8. |
- 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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| 9. |
- Lee, Jason W. L., et al.
(författare)
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Cooling dynamics of energized naphthalene and azulene radical cations
- 2023
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Ingår i: Journal of Chemical Physics. - 0021-9606 .- 1089-7690. ; 158:17
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Tidskriftsartikel (refereegranskat)abstract
- Naphthalene and azulene are isomeric polycyclic aromatic hydrocarbons (PAHs) and are topical in the context of astrochemistry due to the recent discovery of substituted naphthalenes in the Taurus Molecular Cloud-1 (TMC-1). Here, the thermal- and photo-induced isomerization, dissociation, and radiative cooling dynamics of energized (vibrationally hot) naphthalene (Np+) and azulene (Az(+)) radical cations, occurring over the microsecond to seconds timescale, are investigated using a cryogenic electrostatic ion storage ring, affording molecular cloud in a box conditions. Measurement of the cooling dynamics and kinetic energy release distributions for neutrals formed through dissociation, until several seconds after hot ion formation, are consistent with the establishment of a rapid (sub-microsecond) Np+ reversible arrow Az(+) quasi-equilibrium. Consequently, dissociation by C2H2-elimination proceeds predominantly through common Az(+) decomposition pathways. Simulation of the isomerization, dissociation, recurrent fluorescence, and infrared cooling dynamics using a coupled master equation combined with high-level potential energy surface calculations [CCSD(T)/cc-pVTZ], reproduce the trends in the measurements. The data show that radiative cooling via recurrent fluorescence, predominately through the Np+ D-0 <- D-2 transition, efficiently quenches dissociation for vibrational energies up to approximate to 1 eV above dissociation thresholds. Our measurements support the suggestion that small cations, such as naphthalene, may be more abundant in space than previously thought. The strategy presented in this work could be extended to fingerprint the cooling dynamics of other PAH ions for which isomerization is predicted to precede dissociation.
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| 10. |
- Najeeb, P. K., 1986-, et al.
(författare)
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Stability and Cooling of the C72- Dianion
- 2023
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Ingår i: Physical Review Letters. - 0031-9007 .- 1079-7114. ; 131:11
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Tidskriftsartikel (refereegranskat)abstract
- We have studied the stability of the smallest long-lived all carbon molecular dianion (C72-) in new time domains and with a single ion at a time using a cryogenic electrostatic ion-beam storage ring. We observe spontaneous electron emission from internally excited dianions on millisecond timescales and monitor the survival of single colder C72- molecules on much longer timescales. We find that their intrinsic lifetime exceeds several minutes - 6 orders of magnitude longer than established from earlier experiments on C72-. This is consistent with our calculations of vertical electron detachment energies predicting one inherently stable isomer and one isomer which is stable or effectively stable behind a large Coulomb barrier for C72-→C7-+e- separation.
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