We demonstrate laser control of the electronic product state distribution of photodesorbed halogen atoms from alkali halide crystals. Our general model of surface exciton desorption dynamics is developed into a simple method for laser control of the relative halogen atom spin–orbit laser desorption yield. By tuning the excitation laser photon energy in a narrow region of the absorption threshold, the yield of excited state chorine atoms, can be made to vary from near 0 to 80% for KCl and from near 0 to 50% for NaCl relative to the total yield of Cl atoms. We describe the physical properties necessary to obtain a high degree of product state control and the limitation induced when these requirements are not met. These results demonstrate that laser control can be applied to solid state surface reactions and provide strong support for surface exciton-based desorption models.
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1 February 2004
Research Article|
February 01 2004
Laser control of product electronic state: Desorption from alkali halides Available to Purchase
Kenneth M. Beck;
Kenneth M. Beck
Pacific Northwest National Laboratory, William R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 99352
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Alan G. Joly;
Alan G. Joly
Pacific Northwest National Laboratory, William R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 99352
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Nicholas F. Dupuis;
Nicholas F. Dupuis
Department of Chemistry, University of California, Santa Barbara, California 93106
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Peggy Perozzo;
Peggy Perozzo
Department of Physics, Mary Baldwin College, Staunton, Virginia 24401
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Wayne P. Hess;
Wayne P. Hess
Pacific Northwest National Laboratory, William R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 99352
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Peter V. Sushko;
Peter V. Sushko
Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom
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Alexander L. Shluger
Alexander L. Shluger
Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom
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Kenneth M. Beck
Pacific Northwest National Laboratory, William R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 99352
Alan G. Joly
Pacific Northwest National Laboratory, William R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 99352
Nicholas F. Dupuis
Department of Chemistry, University of California, Santa Barbara, California 93106
Peggy Perozzo
Department of Physics, Mary Baldwin College, Staunton, Virginia 24401
Wayne P. Hess
Pacific Northwest National Laboratory, William R. Wiley Environmental Molecular Sciences Laboratory, Richland, Washington 99352
Peter V. Sushko
Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom
Alexander L. Shluger
Department of Physics and Astronomy, University College London, London WC1E 6BT, United Kingdom
J. Chem. Phys. 120, 2456–2463 (2004)
Article history
Received:
August 11 2003
Accepted:
November 05 2003
Citation
Kenneth M. Beck, Alan G. Joly, Nicholas F. Dupuis, Peggy Perozzo, Wayne P. Hess, Peter V. Sushko, Alexander L. Shluger; Laser control of product electronic state: Desorption from alkali halides. J. Chem. Phys. 1 February 2004; 120 (5): 2456–2463. https://doi.org/10.1063/1.1637336
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