Progress towards a realistic theoretical description of C60 photoelectron-momentum imaging experiments using time-dependent density-functional theory

Wopperer P, Gao CZ, Barillot T, Cauchy C, Marciniak A, Despre V, Loriot V, Celep G, Bordas C, Lepine F, Dinh PM, Suraud E, Reinhard PG (2015)

Publication Type: Journal article

Publication year: 2015

Journal

Physical Review A - Atomic, Molecular, and Optical Physics American Physical Society

Book Volume: 91

Article Number: 042514

Journal Issue: 4

DOI: 10.1103/PhysRevA.91.042514

Abstract

We have studied theoretical photoelectron-momentum distributions of C60 using time-dependent density functional theory (TDDFT) in real time and including a self-interaction correction. Our calculations furthermore account for a proper orientation averaging allowing a direct comparison with experimental results. To illustrate the capabilities of this direct (microscopic and time-dependent) approach, two very different photo-excitation conditions are considered: excitation with a high-frequency XUV light at 20 eV and with a low-frequency IR femtosecond pulse at 1.55 eV. The interaction with the XUV light leads to one-photon transitions and a linear ionization regime. In that situation, the spectrum of occupied single-electron states in C60 is directly mapped to the photoelectron spectrum. On the contrary, the IR pulse leads to multiphoton ionization in which only the two least-bound states contribute to the process. In both dynamical regimes (mono- and multiphoton), calculated and experimental angle-resolved photoelectron spectra compare reasonably well. The observed discrepancies can be understood by the theoretical underestimation of higher-order many-body interaction processes such as electron-electron scattering and by the fact that experiments are performed at finite temperature. These results pave the way to a multiscale description of the C60 ionization mechanisms that is required to render justice to the variety of processes observed experimentally for fullerene molecules.

Authors with CRIS profile

Paul-Gerhard Reinhard Naturwissenschaftliche Fakultät

Additional Organisation(s)

Institut für Theoretische Physik

Involved external institutions

Université Claude Bernard Lyon 1 (UCB) FR France (FR) Université Fédérale de Toulouse Midi-Pyrénées FR France (FR)

How to cite

APA:

Wopperer, P., Gao, C.Z., Barillot, T., Cauchy, C., Marciniak, A., Despre, V.,... Reinhard, P.-G. (2015). Progress towards a realistic theoretical description of C60 photoelectron-momentum imaging experiments using time-dependent density-functional theory. Physical Review A - Atomic, Molecular, and Optical Physics, 91(4). https://doi.org/10.1103/PhysRevA.91.042514

MLA:

Wopperer, P., et al. "Progress towards a realistic theoretical description of C60 photoelectron-momentum imaging experiments using time-dependent density-functional theory." Physical Review A - Atomic, Molecular, and Optical Physics 91.4 (2015).

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