Note to users. If you're seeing this message, it means that your browser cannot find this page's style/presentation instructions -- or possibly that you are using a browser that does not support current Web standards. Find out more about why this message is appearing, and what you can do to make your experience of our site the best it can be.

Published Online March 29, 2001
Science DOI: 10.1126/science.1059133

Reports

Submitted on January 18, 2001
Accepted on March 15, 2001

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

Robert J. Levis 1*, Getahun M. Menkir 2, Herschel Rabitz 3

1 Department of Chemistry, Wayne State University, Detroit, MI 48202, USA.
2 Department of Chemistry, Wayne State University, Detroit, MI 48202, USA.
3 Department of Chemistry, Princeton University, Princeton, NJ 08540, USA.

We report the use of strong-field laser pulses tailored using 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 ~100 kcal/mol (~4eV) is reported for polyatomic molecules including acetone, trifluoroacetone and acetophenone. Control over the formation of CH3CO from (CH3)2CO, CF3 (or CH3) from CH3COCF3 and C6H5CH3 (toluene) from C6H5COCH3 is observed with high selectivity. Strong field control appears to have generic applicability for manipulating molecular reactivity because the tailored intense laser fields (~1013 watt cm-2) 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.


THIS ARTICLE HAS BEEN CITED BY OTHER ARTICLES:
Energy Flow Under Control.
V. S. Batista (2009)
Science 326, 245-246
   Abstract »    Full Text »    PDF »
Mapping Excited-State Dynamics by Coherent Control of a Dendrimer's Photoemission Efficiency.
D. G. Kuroda, C. P. Singh, Z. Peng, and V. D. Kleiman (2009)
Science 326, 263-267
   Abstract »    Full Text »    PDF »
Strong-field control and spectroscopy of attosecond electron-hole dynamics in molecules.
O. Smirnova, S. Patchkovskii, Y. Mairesse, N. Dudovich, and M. Y. Ivanov (2009)
PNAS 106, 16556-16561
   Abstract »    Full Text »    PDF »
Coherent Control of Decoherence.
M. P. A. Branderhorst, P. Londero, P. Wasylczyk, C. Brif, R. L. Kosut, H. Rabitz, and I. A. Walmsley (2008)
Science 320, 638-643
   Abstract »    Full Text »    PDF »
Dynamic Stark Control of Photochemical Processes.
B. J. Sussman, D. Townsend, M. Yu. Ivanov, and A. Stolow (2006)
Science 314, 278-281
   Abstract »    Full Text »    PDF »
Use of coherent control methods through scattering biological tissue to achieve functional imaging.
J. M. Dela Cruz, I. Pastirk, M. Comstock, V. V. Lozovoy, and M. Dantus (2004)
PNAS 101, 16996-17001
   Abstract »    Full Text »    PDF »
Quantum Optimally Controlled Transition Landscapes.
H. A. Rabitz, M. M. Hsieh, and C. M. Rosenthal (2004)
Science 303, 1998-2001
   Abstract »    Full Text »    PDF »
Deciphering the Reaction Dynamics Underlying Optimal Control Laser Fields.
C. Daniel, J. Full, L. Gonzalez, C. Lupulescu, J. Manz, A. Merli, &S.;t. Vajda, and L. Woste (2003)
Science 299, 536-539
   Abstract »    Full Text »    PDF »
Spatiotemporal Coherent Control of Lattice Vibrational Waves.
T. Feurer, J. C. Vaughan, and K. A. Nelson (2003)
Science 299, 374-377
   Abstract »    Full Text »    PDF »


To Advertise     Find Products

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