TY - JOUR
T1 - Femtosecond two-photon photoassociation of hot magnesium atoms
T2 - A quantum dynamical study using thermal random phase wavefunctions
AU - Amaran, Saieswari
AU - Kosloff, Ronnie
AU - Tomza, Michał
AU - Skomorowski, Wojciech
AU - Pawłowski, Filip
AU - Moszynski, Robert
AU - Rybak, Leonid
AU - Levin, Liat
AU - Amitay, Zohar
AU - Berglund, J. Martin
AU - Reich, Daniel M.
AU - Koch, Christiane P.
PY - 2013/10/28
Y1 - 2013/10/28
N2 - 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.
AB - 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.
UR - http://www.scopus.com/inward/record.url?scp=84903367773&partnerID=8YFLogxK
U2 - 10.1063/1.4826350
DO - 10.1063/1.4826350
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AN - SCOPUS:84903367773
SN - 0021-9606
VL - 139
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 16
M1 - 164124
ER -