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Unravelling the electronic nature of the radiative cooling of cobalt clusters

In this paper, we report on the experimental determination of photon emission rates of laser-excited cobalt clusters, Co_{n}^{+} (n=5–23), deduced from fragmentation mass spectrometry and metastable decay fractions. The rates are so high that they can only be ascribed to recurrent fluorescence (RF),...

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Bibliographic Details
Published in:Physical review research 2021-09, Vol.3 (3), p.033225, Article 033225
Main Authors: Peeters, Kristien, Janssens, Ewald, Hansen, Klavs, Lievens, Peter, Ferrari, Piero
Format: Article
Language:English
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Summary:In this paper, we report on the experimental determination of photon emission rates of laser-excited cobalt clusters, Co_{n}^{+} (n=5–23), deduced from fragmentation mass spectrometry and metastable decay fractions. The rates are so high that they can only be ascribed to recurrent fluorescence (RF), a process where emitting states are populated by inverse internal conversion, followed by photon emission. Cooling via electronic states is confirmed by quantitative agreement with calculated rates using the low-lying electronic transitions predicted by time-dependent density functional theory calculations for n=5–10, which are performed considering all electrons and including relativistic effects implicitly. The outstanding agreement between experiment and theory provides clear evidence that the clusters radiate via electronic states, being a consistent theoretical and experimental study invoking RF.
ISSN:2643-1564
2643-1564
DOI:10.1103/PhysRevResearch.3.033225