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Chemical Physics Letters

Optimal control of isotope selective fragmentation

Albrecht Lindinger, Andrea Merli, Mateusz Plewicki, Franziska Vetter, Stefan M. Weber, Ludger H. Wöste

Published Aug 20, 2005• 17 citations
Publisher
DOI
10.1016/j.cplett.2005.07.100

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We present a joint theoretical and experimental study of the maximization of the isotopomer ratio (23)Na(39)K(23)Na(41)K using tailored phase-only as well as amplitude and phase modulated femtosecond laser fields obtained in the framework of optimal control theory and closed loop learning (CLL) technique. A good agreement between theoretically and experimentally optimized pulse shapes is achieved which allows to assign the optimized processes directly to the pulse shapes obtained by the experimental isotopomer selective CLL approach. By analyzing the dynamics induced by the optimized pulses we show that the mechanism involving the dephasing of the wave packets between the isotopomers (23)Na (39)K and (23)Na (41)K on the first excited state is responsible for high isotope selective ionization. Amplitude and phase modulated pulses, moreover, allow to establish the connection between the spectral components of the pulse and corresponding occupied vibronic states. It will be also shown that the leading features of the theoretically shaped pulses are independent from the initial conditions. Since the underlying processes can be assigned to the individual features of the shaped pulses, we show that optimal control can be used as a tool for analysis.
We report on selective optimization of different isotopes in an ionization process by means of spectrally broad shaped fs-laser pulses. This is demonstrated for (39,39)K2 and (39,41)K2 by applying evolution strategies in a feedback loop, whereby a surprisingly high enhancement of one isotope versus the other and vice versa is achieved (total factor approximately 140). Information about the dynamics on the involved vibrational states is extracted from the optimal pulse shapes, which provides a new spectroscopical approach of yielding distinct frequency pattern on fs-time scales. The method should, in principle, be feasible for all molecules.