Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 7, Issue 22, Pages 4677-4682Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.6b02139
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Funding
- Chemical Sciences, Geosciences, and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy [DE-FG02-86ER13491, DE-SC0012376, DE-SC0012628, DE-SC0008146]
- European Union via the ERC grant ATTOCO [307203]
- DFG via the Cluster of Excellence: Munich Center for Advanced Photonics (MAP)
- Fonds National de la Recherche Scientifique, Belgium
- Fonds de la Recherche Scientifique de Belgique (F.R.S.-FNRS) [2.5020.11]
- European Research Council (ERC) [307203] Funding Source: European Research Council (ERC)
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The transition between two distinct ionization mechanisms in femtosecond laser fields at 785 nm is observed for C-60 molecules. The transition occurs in the investigated intensity range from 3 to 20 TW/cm(2) and is visualized in electron kinetic energy spectra below the one-photon energy (1.5 eV) obtained via velocity map imaging. Assignment of several observed broad spectral peaks to ionization from superatom molecular orbitals (SAMOs) and Rydberg states is based on time-dependent density functional theory simulations. We find that ionization from SAMOs dominates the spectra for intensities below 5 TW/cm(2). As the intensity increases, Rydberg state ionization exceeds the prominence of SAMOs. Using short laser pulses (20 fs) allowed uncovering of distinct six-lobe photoelectron angular distributions with kinetic energies just above the threshold (below 0.2 eV), which we interpret as over-the-barrier ionization of shallow f-Rydberg states in C-60.
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