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

Journal Article · Mon Oct 28 04:00:00 EDT 2013 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4826350· OSTI ID:22220369

Amaran, Saieswari; Kosloff, Ronnie ^[1]; Tomza, Michał; Skomorowski, Wojciech; Pawłowski, Filip; Moszynski, Robert ^[2]; Rybak, Leonid; Levin, Liat; Amitay, Zohar ^[3]; Berglund, J. Martin; Reich, Daniel M.; Koch, Christiane P. ^[4]

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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)

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.

• OSTI ID: 22220369
• Journal Information: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 16 Vol. 139; ISSN JCPSA6; ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

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