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

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.
Authors:
;  [1] ; ; ; ;  [2] ; ; ;  [3] ; ; ;  [4]
  1. Fritz Haber Research Centre and The Department of Physical Chemistry, Hebrew University, Jerusalem 91904 (Israel)
  2. Department of Chemistry, University of Warsaw, Pasteura 1, 02-093 Warsaw (Poland)
  3. The Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000 (Israel)
  4. Theoretische Physik, Universität Kassel, Heinrich-Plett-Straße 40, 34132 Kassel (Germany)
Publication Date:
OSTI Identifier:
22220369
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 139; Journal Issue: 16; Other Information: (c) 2013 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; 74 ATOMIC AND MOLECULAR PHYSICS; CONVERGENCE; EIGENSTATES; EIGENVALUES; INTERACTIONS; LASERS; MAGNESIUM; PULSES; REACTION KINETICS; VIBRATIONAL STATES; WAVE FUNCTIONS