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Cooling of gold cluster anions, Au𝑁 (𝑁=2–13,15), in a cryogenic ion-beam storage ring
Stockholm University, Faculty of Science, Department of Physics.ORCID iD: 0000-0002-0161-4560
Stockholm University, Faculty of Science, Department of Physics.
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Number of Authors: 122024 (English)In: Physical Review A: covering atomic, molecular, and optical physics and quantum information, ISSN 2469-9926, E-ISSN 2469-9934, Vol. 110, no 5, article id 052813Article in journal (Refereed) Published
Abstract [en]

We measured the spontaneous and photoinduced decays of anionic gold clusters, , with sizes ranging from 𝑁=2 to 13 and 15. After production in a sputter ion source, the size-selected clusters were stored in the cryogenic electrostatic ion-beam storage ring DESIREE, and their neutralization decays were measured for storage times between 0.1 and 100 s. The dimer was observed to decay by electron emission in parallel to neutral atom emission at long times, implying a breakdown of the Born-Oppenheimer approximation, analogous to the behavior of copper and silver dimers. Radiative cooling is observed for all other cluster sizes. The decays of clusters 𝑁=3,6,8–13,15 show only a single radiative cooling time. For 𝑁=6–13 the cooling times have a strong odd-even oscillation with an amplitude that decrease with cluster size and with the even 𝑁 having the faster cooling. We compare our results with previous measurements of radiative cooling rates of the corresponding cationic gold clusters, , which also show an odd-even effect with a similar oscillation amplitude but at orders of magnitude shorter timescales and out of phase with the anions. The tetramer and pentamer both show two cooling times, which we tentatively ascribe to different structural forms at different ranges of high angular momenta of the ions in the and beams. For , the shape of the decay curve suggests that the cluster cools by emission of low-energy photons. The calculated limit on photon energies strongly suggests that cooling is by vibrational transitions in this case. For , time-resolved studies of photoinduced decays were performed to track the evolution of the internal energy distribution. We conclude that the radiative cooling is dominated by sequences of vibrational transitions in the IR. The laser-enhanced neutralization rate of was exponential, in contrast to its spontaneous decay rate, indicating that the cluster had already been cooled to a very narrow internal energy distribution at 120 ms as the total (integrated) laser-enhanced intensity was independent of the laser firing time at later times. The unimolecular rate constants decreased from 500 s−1 when laser excited at 0.12 s to 40 s−1 when laser excited at 0.62 s.

Place, publisher, year, edition, pages
2024. Vol. 110, no 5, article id 052813
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Atom and Molecular Physics and Optics
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URN: urn:nbn:se:su:diva-240937DOI: 10.1103/PhysRevA.110.052813ISI: 001413369600008Scopus ID: 2-s2.0-85210323053OAI: oai:DiVA.org:su-240937DiVA, id: diva2:1946507
Available from: 2025-03-21 Created: 2025-03-21 Last updated: 2025-03-21Bibliographically approved

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Anderson, Emma K.Björkhage, MikaelCederquist, HenrikJi, MingChaoRosén, StefanSchmidt-May, AliceStockett, Mark H.Zettergren, HenningSchmidt, Henning T.

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Anderson, Emma K.Björkhage, MikaelCederquist, HenrikJi, MingChaoRosén, StefanSchmidt-May, AliceStockett, Mark H.Zettergren, HenningSchmidt, Henning T.
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Physical Review A: covering atomic, molecular, and optical physics and quantum information
Atom and Molecular Physics and Optics

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