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

Leonid Rybak, Saieswari Amaran, Liat Levin, Michał Tomza, Robert Moszynski, Ronnie Kosloff, Christiane P. Koch, and Zohar Amitay
Phys. Rev. Lett. 107, 273001 – Published 27 December 2011

Abstract

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.

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  • Received 24 July 2011

DOI:https://doi.org/10.1103/PhysRevLett.107.273001

© 2011 American Physical Society

Authors & Affiliations

Leonid Rybak1, Saieswari Amaran2, Liat Levin1, Michał Tomza3, Robert Moszynski3, Ronnie Kosloff2, Christiane P. Koch4,5, and Zohar Amitay1,*

  • 1The Shirlee Jacobs Femtosecond Laser Research Laboratory, Schulich Faculty of Chemistry, Technion-Israel Institute of Technology, Haifa 32000, Israel
  • 2Institute of Chemistry, Hebrew University, Jerusalem 91904, Israel
  • 3Department of Chemistry, University of Warsaw, Pasteura 1, 02-093 Warsaw, Poland
  • 4Institut für Theoretische Physik, Freie Universität Berlin, Arnimallee 14, 14195 Berlin, Germany
  • 5Theoretische Physik, Universität Kassel, Heinrich-Plett-Straße 40, 34132 Kassel, Germany

  • *amitayz@tx.technion.ac.il

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Vol. 107, Iss. 27 — 30 December 2011

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