Selective bond dissociation and rearrangement with optimally tailored, strong-field laser pulses

R. J. Levis, G. M. Menkir, H. Rabitz

Research output: Contribution to journalArticle

802 Scopus citations

Abstract

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.

Original languageEnglish (US)
Pages (from-to)709-713
Number of pages5
JournalScience
Volume292
Issue number5517
DOIs
StatePublished - Apr 27 2001
Externally publishedYes

All Science Journal Classification (ASJC) codes

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