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J Phys Chem Lett. 2017 Jan 05;8(1):307-312. doi: 10.1021/acs.jpclett.6b02598. Epub 2016 Dec 22.

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

The journal of physical chemistry letters

Johannes von Vangerow, François Coppens, Antonio Leal, Martí Pi, Manuel Barranco, Nadine Halberstadt, Frank Stienkemeier, Marcel Mudrich

Affiliations

  1. Physikalisches Institut, Universität Freiburg , Hermann-Herder-Str. 3, 79104 Freiburg, Germany.
  2. Laboratoire des Collisions, Agrégats, Réactivité, IRSAMC, UMR 5589, CNRS et Université Paul Sabatier-Toulouse 3, 118 route de Narbonne, F-31062 Toulouse Cedex 09, France.
  3. Departament FQA, Facultat de Física, and IN2UB, Universitat de Barcelona , Diagonal 645, 08028 Barcelona, Spain.

PMID: 27996261 DOI: 10.1021/acs.jpclett.6b02598

Abstract

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).

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