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Originally published in Science Express on 29 March 2001
Science 27 April 2001:
Vol. 292. no. 5517, pp. 709 - 713
DOI: 10.1126/science.1059133
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Reports

Selective Bond Dissociation and Rearrangement with Optimally Tailored, Strong-Field Laser Pulses

Robert J. Levis,1* Getahun M. Menkir,1 Herschel Rabitz2

We used strong-field laser pulses that were tailored with closed-loop optimal control to govern specified chemical dissociation and reactivity channels in a series of organic molecules. Selective cleavage and rearrangement of chemical bonds having dissociation energies up to approximately 100 kilocalories per mole (about 4 electron volts) are reported for polyatomic molecules, including (CH3)2CO (acetone), CH3COCF3 (trifluoroacetone), and C6H5COCH3 (acetophenone). Control over the formation of CH3CO from (CH3)2CO, CF3 (or CH3) from CH3COCF3, and C6H5CH3 (toluene) from C6H5COCH3 was observed with high selectivity. Strong-field control appears to have generic applicability for manipulating molecular reactivity because the tailored intense laser fields (about 1013 watts per square centimeter) can dynamically Stark shift many excited states into resonance, and consequently, the method is not confined by resonant spectral restrictions found in the perturbative (weak-field) regime.

1 Department of Chemistry, Wayne State University, Detroit, MI 48202, USA.
2 Department of Chemistry, Princeton University, Princeton, NJ 08540, USA.
*   To whom correspondence should be addressed.

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Science. ISSN 0036-8075 (print), 1095-9203 (online)