title: Femtosecond two-photon photoassociation of hot magnesium atoms: a quantum dynamical study using thermal random phase wavefunctions.
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.
authors.affiliation: Fritz Haber Research Centre and The Department of Physical Chemistry, Hebrew University, Jerusalem 91904, Israel.
authors.forename: Saieswari
authors.initials: S
authors.lastname: Amaran
authors.forename: Ronnie
authors.initials: R
authors.lastname: Kosloff
authors.forename: Michał
authors.initials: M
authors.lastname: Tomza
authors.forename: Wojciech
authors.initials: W
authors.lastname: Skomorowski
authors.forename: Filip
authors.initials: F
authors.lastname: Pawłowski
authors.forename: Robert
authors.initials: R
authors.lastname: Moszynski
authors.forename: Leonid
authors.initials: L
authors.lastname: Rybak
authors.forename: Liat
authors.initials: L
authors.lastname: Levin
authors.forename: Zohar
authors.initials: Z
authors.lastname: Amitay
authors.forename: J Martin
authors.initials: JM
authors.lastname: Berglund
authors.forename: Daniel M
authors.initials: DM
authors.lastname: Reich
authors.forename: Christiane P
authors.initials: CP
authors.lastname: Koch