Anders Sondergaard, Robert Zillich, Henrik Stapelfeldt,
"Rotational dissociation of impulsively aligned van der Waals complexes"
, in The Journal of Chemical Physics, Vol. 147, Seite(n) 074304, 8-2017, ISSN: 0021-9606
Original Titel:
Rotational dissociation of impulsively aligned van der Waals complexes
Sprache des Titels:
Englisch
Original Kurzfassung:
The nonadiabatic alignment dynamics of weakly bound molecule-atom complexes, induced by a
moderately intense 300 fs nonresonant laser pulse, is calculated by direct numerical solution of the
time-dependent Schr ?odinger equation. Our method propagates the wave function according to the
coupled channel equations for the complex, which can be done in a very efficient and stable manner
out to large times. We present results for two van der Waal complexes, CS 2 ?He and HCCH?He,
as respective examples of linear molecules with large and small moments of inertia. Our main result
is that at intensities typical of nonadiabatic alignment experiments, these complexes rapidly dis-
sociate. In the case of the CS 2 ?He complex, the ensuing rotational dynamics resembles that of
isolated molecules, whereas for the HCCH?He complex, the detachment of the He atom severely
perturbs and essentially quenches the subsequent rotational motion. At intensities of the laser pulse
2.0 × 10 12 W/cm 2 , it is shown that the molecule-He complex can rotate and align without breaking
apart. We discuss the implications of our findings for recent experiments on iodine molecules solvated
in helium nanodroplets.
Forschungs-