Femtosecond two-photon photoassociation of hot magnesium atoms: A quantum dynamical study using thermal random phase wavefunctions

Saieswari Amaran, Ronnie Kosloff, Michał Tomza, Wojciech Skomorowski, Filip Pawłowski, Robert Moszynski, Leonid Rybak, Liat Levin, Zohar Amitay, J. Martin Berglund, Daniel M. Reich, Christiane P. Koch

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Abstract

Two-photon photoassociation of hot magnesium atoms by femtosecond laser pulses, creating electronically excited magnesium dimer molecules, is studied from first principles, combining ab initio quantum chemistry and molecular quantum dynamics. This theoretical framework allows for rationalizing the generation of molecular rovibrational coherence from thermally hot atoms [L. Rybak, S. Amaran, L. Levin, M. Tomza, R. Moszynski, R. Kosloff, C. P. Koch, and Z. Amitay, Phys. Rev. Lett. 107, 273001 (2011)]. Random phase thermal wavefunctions are employed to model the thermal ensemble of hot colliding atoms. Comparing two different choices of basis functions, random phase wavefunctions built from eigenstates are found to have the fastest convergence for the photoassociation yield. The interaction of the colliding atoms with a femtosecond laser pulse is modeled non-perturbatively to account for strong-field effects.

Original languageEnglish
Article number164124
JournalJournal of Chemical Physics
Volume139
Issue number16
DOIs
StatePublished - 28 Oct 2013

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