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- ItemXUV excitation followed by ultrafast non-adiabatic relaxation in PAH molecules as a femto-astrochemistry experiment([London] : Nature Publishing Group UK, 2015) Marciniak, A.; Despré, V.; Barillot, T.; Rouzée, A.; Galbraith, M.C.E.; Klei, J.; Yang, C.-H.; Smeenk, C.T.L.; Loriot, V.; Nagaprasad Reddy, S.; Tielens, A.G.G.M.; Mahapatra, S.; Kuleff, A.I.; Vrakking, M.J.J.; Lépine, F.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.
- ItemAttosecond time delays in C60 valence photoemissions at the giant plasmon(Bristol : IOP Publ., 2015) Barillot, T.; Magrakvelidze, M.; Loriot, V.; Bordas, C.; Hervieux, P.-A.; Gisselbrecht, M.; Johnsson, P.; Laksman, J.; Mansson, E.P.; Sorensen, S.; Canton, S.E.; Dahlström, J.M.; Dixit, G.; Madjet, M.E.; Lépine, F.; Chakraborty, H.S.We perform time-dependent local density functional calculations of the time delay in C60 HOMO and HOMO-1 photoionization at giant plasmon energies. A semiclassical model is used to develop further insights.