Control of quantum dynamics by a locally optimized laser field. Application to ring puckering isomerization

M. Sugawara, Y. Fujimura

Research output: Contribution to journalArticle

96 Citations (Scopus)

Abstract

We presented a theoretical method for controlling quantum dynamics by locally optimized nonstationary laser fields, within the semiclassical theory of the molecule-radiation field interaction. The external laser field is optimized based on the control theory of a linear time-invariant (LTI) system, so that both the summation of the population of the nontarget states and the total energies of the laser fields are minimized. The optimization procedure involves operation of the so-called feedback gain matrix to the time-dependent state vector. This procedure is carried out at every successive short stage, in which the time-dependent Schrödinger equation can be approximated to the equation of motion of the LTI system. As an example, the control theory was applied to laser-induced ring-puckering isomerization, the dynamics of which can be described as the wave packet in the one-dimensional double minimum potential under locally optimized laser fields. The result indicated that nearly 100% of the population can be transferred to the final product state by irradiation of the optimized laser fields. The optimized laser fields were analyzed to obtain information on the carrier frequencies or the frequency modulation by using the fast Fourier transform method. These results were then compared with the result of isomerization induced by nonoptimized laser fields.

Original languageEnglish
Pages (from-to)5646-5655
Number of pages10
JournalThe Journal of Chemical Physics
Volume100
Issue number8
DOIs
Publication statusPublished - 1994 Jan 1

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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