Relaxation dynamics of helium nanodroplets after photodissociation of a dopant homonuclear diatomic molecule. The case of Cl@(He)

• Published in: Physical chemistry chemical physics : PCCP 2016-01, Vol.18 (4), p.249-2416
• Main Authors: Vilà, Arnau, González, Miguel, Mayol, Ricardo
• Format: Article
• ISSN: 1463-9076; 1463-9084
• DOI: 10.1039/c5cp02679b

To investigate the quantum dynamics of the relaxation process of excited helium nanodroplets, 4 He N , arising from the photodissociation of Cl 2 embedded molecules (B ← X electronic transition), here we have performed a time dependent density functional theory (TDDFT) study considering nanodroplets of different sizes ( N = 50, 100, 200, 300 and 500), extending a previous study which was centered on the photodissociation step. The relaxation process takes place in the timescale of several hundred picoseconds and a simple dependence of this process on time has been found. The results have been satisfactorily analyzed in terms of a phenomenological model proposed here and also by applying the Rice-Ramsperger-Kassel (RRK) statistical chemical kinetic model for unimolecular reactions. From what we know, this is the first time that the dynamics of these de-excitation processes has been studied, opening up a window for understanding them. We expect that this work will encourage further research on this little known but interesting phenomenon. The quantum (TDDFT) dynamics of the relaxation process (Δ t ∼ 500 ps) of excited helium nanodroplets was studied for the first time.