Data for paper 'Timing the Escape of a Caged Electron'
Publication Date
September 5, 2024
Creators
Description
Core-Hole Clock Spectroscopy Data for Ar@C60:
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 2p5 4s1 state of Ar@C60. Despite the lack of 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 6.5 ± 0.1 fs and ≲ 0.6 fs, respectively, for a 3D Ar@C60 film and a 2D monolayer on Ag(111).
Subjects
Subjects (JACS)
Subjects (LC)
Divisions
University of Nottingham, UK Campus::Faculty of Science::School of Chemistry
University of Nottingham, UK Campus::Faculty of Science::School of Physics and Astronomy
Data type
X-ray Photoemission Spectroscopy, Near Edge X-ray Fine Structure, X-ray Standing Wave, Density functional Theory
Data collection method
X-ray Photoemission Spectroscopy, Near Edge X-ray Fine Structure, X-ray Standing Wave, Density functional Theory
Resource languages
English
Publisher
University of Nottingham
Date Issued
September 5, 2024
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Name
ground_ab209.csv
Size
39.08 KB
Format
Comma Separated Variable (CSV)
Checksum (MD5)
ac3410438da53a8c960d0f20026e3ca8
Name
i09-254694.nxs
Description
Resonant Auger decay - on resonance spectrum - Ar@C60 monolayer
Size
1.3 MB
Format
Unknown
Checksum (MD5)
9b987f00228d135a8aada9a7ffa435f1