Optimal control of selective vibrational excitation in harmonic linear chain molecules

Shenghua Shi, Andrea Woody, Herschel Rabitz

Research output: Contribution to journalArticlepeer-review

416 Scopus citations


A formalism for designing an optical field for selective vibrational excitation in linear harmonic chain molecules is presented based on optimal control theory. The optimizing functional producing the field designs is flexible to allow for the imposition of desirable laboratory and theoretical constraints. The designed optimal fields, which successfully lead to local bond excitations, exhibit complex structure on the time scale of 10 fs. Analysis of the optimal fields shows a high degree of cooperatively between the temporal structure of the fields and the dynamical capabilities of the molecules. It is generally impossible using only spectral information to devise the optical field needed to selectively excite a local bond in a polyatomic molecule. These results explain why the previous intuitively based laboratory attempts at site specific chemistry have yielded disappointing results.

Original languageEnglish (US)
Pages (from-to)6870-6883
Number of pages14
JournalThe Journal of chemical physics
Issue number11
StatePublished - 1988

All Science Journal Classification (ASJC) codes

  • General Physics and Astronomy
  • Physical and Theoretical Chemistry


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