American Chemical Society
jz6b02598_si_004.avi (4.19 MB)

Imaging Excited-State Dynamics of Doped He Nanodroplets in Real-Time

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posted on 2016-12-20, 00:00 authored by Johannes von Vangerow, François Coppens, Antonio Leal, Martí Pi, Manuel Barranco, Nadine Halberstadt, Frank Stienkemeier, Marcel Mudrich
The real-time dynamics of excited alkali metal atoms (Rb) attached to quantum fluid He nanodroplets is investigated using femtosecond imaging spectroscopy and time-dependent density functional theory. We disentangle the competing dynamics of desorption of excited Rb atoms off the He droplet surface and solvation inside the droplet interior as the Rb atom is ionized. For Rb excited to the 5p and 6p states, desorption occurs on starkly differing time scales (∼100 versus ∼1 ps, respectively). The comparison between theory and experiment indicates that desorption proceeds either impulsively (6p) or in a transition regime between impulsive dissociation and complex desorption (5p).