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Attosecond correlated electron dynamics at C$_{60}$ giant plasmon resonance

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Version 2 2023-06-08, 12:50
Version 1 2023-01-12, 14:33
posted on 2023-06-08, 12:50 authored by Shubhadeep Biswas, Andrea Trabattoni, Philipp Rupp, Maia Magrakvelidze, Mohamed El-Amine Madjet, Umberto De Giovannini, Mattea C. Castrovilli, Mara Galli, Qingcao Liu, Erik P. Månsson, Johannes Schötz, Vincent Wanie, François Légaré, Pawel Wnuk, Mauro Nisoli, Angel Rubio, Himadri S. Chakraborty, Matthias F. Kling, Francesca Calegari
Fullerenes have unique physical and chemical properties that are associated with their delocalized conjugated electronic structure. Among them, there is a giant ultra-broadband - and therefore ultrafast - plasmon resonance, which for C$_{60}$ is in the extreme-ultraviolet energy range. While this peculiar resonance has attracted considerable interest for the potential downscaling of nanoplasmonic applications such as sensing, drug delivery and photocatalysis at the atomic level, its electronic character has remained elusive. The ultrafast decay time of this collective excitation demands attosecond techniques for real-time access to the photoinduced dynamics. Here, we uncover the role of electron correlations in the giant plasmon resonance of C$_{60}$ by employing attosecond photoemission chronoscopy. We find a characteristic photoemission delay of up to 200 attoseconds pertaining to the plasmon that is purely induced by coherent large-scale correlations. This result provides novel insight into the quantum nature of plasmonic resonances, and sets a benchmark for advancing nanoplasmonic applications.



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