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

被引：32

作者：

Amaran, Saieswari ^{[1
,2
]}

Kosloff, Ronnie ^{[1
,2
]}

Tomza, Michal ^{[3
]}

Skomorowski, Wojciech ^{[3
]}

Pawlowski, Filip ^{[3
,6
]}

Moszynski, Robert ^{[3
]}

Rybak, Leonid ^{[4
]}

Levin, Liat ^{[4
]}

Amitay, Zohar ^{[4
]}

Berglund, J. Martin ^{[5
]}

Reich, Daniel M. ^{[5
]}

Koch, Christiane P. ^{[5
]}

机构：

[1] Hebrew Univ Jerusalem, Fritz Haber Res Ctr, IL-91904 Jerusalem, Israel

[2] Hebrew Univ Jerusalem, Dept Phys Chem, IL-91904 Jerusalem, Israel

[3] Univ Warsaw, Dept Chem, PL-02093 Warsaw, Poland

[4] Technion Israel Inst Technol, Shirlee Jacobs Femtosecond Laser Res Lab, Schulich Fac Chem, IL-32000 Haifa, Israel

[5] Univ Kassel, D-34132 Kassel, Germany

[6] Kazimierz Wielki Univ, Inst Phys, PL-85072 Bydgoszcz, Poland

来源：

JOURNAL OF CHEMICAL PHYSICS | 2013年 / 139卷 / 16期

基金：

美国国家科学基金会;

关键词：

FREQUENCY-DEPENDENT POLARIZABILITIES; COHERENT CONTROL; CROSS-SECTIONS; LASER CONTROL; SPECTROSCOPY; MOLECULES; RELAXATION; RESONANCES; ENERGIES; COMPLEX;

D O I：

10.1063/1.4826350

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

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. (C) 2013 AIP Publishing LLC.

引用

页数：14

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