Timing the escape of a photoexcited electron from a molecular cage

Connor Fields, Aleksandra Foerster, Sadegh Ghaderzadeh, Ilya Popov, Bang Huynh, Filipe Junqueira, Tyler James, Sofia Alonso Perez, David A. Duncan, Tien-Lin Lee, Yitao Wang, Sally Bloodworth, Gabriela Hoffman, Mark Walkey, Richard J. Whitby, Malcolm H. Levitt, Brian Kiraly, James N. O’Shea, Elena Besley () and Philip Moriarty ()
Additional contact information
Connor Fields: University of Nottingham
Aleksandra Foerster: University of Nottingham
Sadegh Ghaderzadeh: University of Nottingham
Ilya Popov: University of Nottingham
Bang Huynh: University of Nottingham
Filipe Junqueira: University of Nottingham
Tyler James: University of Nottingham
Sofia Alonso Perez: University of Nottingham
David A. Duncan: University of Nottingham
Tien-Lin Lee: Harwell Science & Innovation Campus
Yitao Wang: University of Nottingham
Sally Bloodworth: University of Southampton
Gabriela Hoffman: University of Southampton
Mark Walkey: University of Southampton
Richard J. Whitby: University of Southampton
Malcolm H. Levitt: University of Southampton
Brian Kiraly: University of Nottingham
James N. O’Shea: University of Nottingham
Elena Besley: University of Nottingham
Philip Moriarty: University of Nottingham

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Charge transfer is fundamentally dependent on the overlap of the orbitals comprising the transport pathway. This has key implications for molecular, nanoscale, and quantum technologies, for which delocalization (and decoherence) rates are essential figures of merit. Here, we apply the core hole clock technique—an energy-domain variant of ultrafast spectroscopy—to probe the delocalization of a photoexcited electron inside a closed molecular cage, namely the Ar 2p54s1 state of Ar@C60. Despite marginal frontier orbital mixing in the ground configuration, almost 80% of the excited state density is found outside the buckyball due to the formation of a markedly diffuse hybrid orbital. Far from isolating the intracage excitation, the surrounding fullerene is instead a remarkably efficient conduit for electron transfer: we measure characteristic delocalization times of 6.6 ± 0.3 fs and ≲ 500 attoseconds, respectively, for a 3D Ar@C60 film and a 2D monolayer on Ag(111).

Date: 2025
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DOI: 10.1038/s41467-025-60260-z

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