Generating Molecular Rovibrational Coherence by Two-Photon Femtosecond Photoassociation of Thermally Hot Atoms

Journal Article · Fri Dec 30 04:00:00 EST 2011 · Physical Review Letters

DOI:https://doi.org/10.1103/PHYSREVLETT.107.273001· OSTI ID:21612587

Rybak, Leonid; Levin, Liat; Amitay, Zohar ^[1]; Amaran, Saieswari; Kosloff, Ronnie ^[2]; Tomza, Michal; Moszynski, Robert ^[3]; Koch, Christiane P ^[4]

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1. Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000 (Israel)
2. Institute of Chemistry, Hebrew University, Jerusalem 91904 (Israel)
3. Department of Chemistry, University of Warsaw, Pasteura 1, 02-093 Warsaw (Poland)
4. Institut fuer Theoretische Physik, Freie Universitaet Berlin, Arnimallee 14, 14195 Berlin (Germany)

The formation of diatomic molecules with rotational and vibrational coherence is demonstrated experimentally in free-to-bound two-photon femtosecond photoassociation of hot atoms. In a thermal gas at a temperature of 1000 K, pairs of magnesium atoms, colliding in their electronic ground state, are excited into coherent superpositions of bound rovibrational levels in an electronically excited state. The rovibrational coherence is probed by a time-delayed third photon, resulting in quantum beats in the UV fluorescence. A comprehensive theoretical model based on ab initio calculations rationalizes the generation of coherence by Franck-Condon filtering of collision energies and partial waves, quantifying it in terms of an increase in quantum purity of the thermal ensemble. Our results open the way to coherent control of a binary reaction.

• OSTI ID: 21612587
• Journal Information: Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 27 Vol. 107; ISSN 0031-9007; ISSN PRLTAO
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
71 CLASSICAL AND QUANTUM MECHANICS
GENERAL PHYSICS
ALKALINE EARTH METALS
BOSONS
CHEMISTRY
ELEMENTARY PARTICLES
ELEMENTS
EMISSION
ENERGY LEVELS
EXCITED STATES
FLUORESCENCE
GROUND STATES
HOT ATOM CHEMISTRY
LUMINESCENCE
MAGNESIUM
MASSLESS PARTICLES
MECHANICS
METALS
PARTIAL WAVES
PHOTON EMISSION
PHOTONS
QUANTUM MECHANICS
RADIOCHEMISTRY
TEMPERATURE RANGE
TEMPERATURE RANGE 0400-1000 K
TIME DELAY