XUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment

A. Marciniak, V. Despré, T. Barillot, A. Rouzée, M.C.E. Galbraith, J. Klei, C.-H. Yang, C.T.L. Smeenk, V. Loriot, S. Nagaprasad Reddy, A.G.G.M. Tielens, S. Mahapatra, A. I. Kuleff, M.J.J. Vrakking and F. Lépine ()
Additional contact information
A. Marciniak: Institut Lumière Matière, Université Lyon 1, CNRS, UMR 5306
V. Despré: Institut Lumière Matière, Université Lyon 1, CNRS, UMR 5306
T. Barillot: Institut Lumière Matière, Université Lyon 1, CNRS, UMR 5306
A. Rouzée: Max-Born-Institut
M.C.E. Galbraith: Max-Born-Institut
J. Klei: Max-Born-Institut
C.-H. Yang: Max-Born-Institut
C.T.L. Smeenk: Max-Born-Institut
V. Loriot: Institut Lumière Matière, Université Lyon 1, CNRS, UMR 5306
S. Nagaprasad Reddy: School of Chemistry, University of Hyderabad
A.G.G.M. Tielens: Leiden Observatory, Leiden University
S. Mahapatra: School of Chemistry, University of Hyderabad
A. I. Kuleff: Theoretische Chemie, PCI, Universität Heidelberg
M.J.J. Vrakking: Max-Born-Institut
F. Lépine: Institut Lumière Matière, Université Lyon 1, CNRS, UMR 5306

Nature Communications, 2015, vol. 6, issue 1, 1-6

Abstract: Abstract Highly excited molecular species are at play in the chemistry of interstellar media and are involved in the creation of radiation damage in a biological tissue. Recently developed ultrashort extreme ultraviolet light sources offer the high excitation energies and ultrafast time-resolution required for probing the dynamics of highly excited molecular states on femtosecond (fs) (1 fs=10−15s) and even attosecond (as) (1 as=10−18 s) timescales. Here we show that polycyclic aromatic hydrocarbons (PAHs) undergo ultrafast relaxation on a few tens of femtoseconds timescales, involving an interplay between the electronic and vibrational degrees of freedom. Our work reveals a general property of excited radical PAHs that can help to elucidate the assignment of diffuse interstellar absorption bands in astrochemistry, and provides a benchmark for the manner in which coupled electronic and nuclear dynamics determines reaction pathways in large molecules following extreme ultraviolet excitation.

Date: 2015
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DOI: 10.1038/ncomms8909

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