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International Conference Physics and Control

Quantum control of dissociation of an iodine molecule by one and two femtosecond laser pulses excitation

Mikhail S. Ananyevskiy, A. S. Vetchinkin, Oleg M. Sarkisov, Stanislav Ya Umanskii, Аlexander L. Fradkov, Yu. A. Zotov

Published Oct 4, 2006• 3 citations
Publisher

Abstract

We introduce two approaches to the synthesis of the optimized schemes of dissociation control of diatomic molecules. The first one bases on the early introduced speed-gradient algorithms of the quantum control. We use the semi classical model of molecular dynamics onto the ground state. The introduced algorithm is a robust and it has only one tuning parameter. The numerical results of the control of the predissociation of iodine molecule illustrate the high possibility of the dissociation for 100 fs laser pulse. The second approach bases on quantum model of dissociation through B excited electronic state. This model doesn't assume the solving of any time-depended equations. The optimized scheme of iodine dissociation with different nuclear isotopes is obtained. The best isotope separation achieves up to 300 fs with 80% efficiency.

DOI
10.1109/phycon.2005.1514061

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We introduce two approaches to the synthesis of the optimized schemes of dissociation control of diatomic molecules. The first one bases on the early introduced speed-gradient algorithms of the quantum control. We use the semi classical model of molecular dynamics onto the ground state. The introduced algorithm is a robust and it has only one tuning parameter. The numerical results of the control of the predissociation of iodine molecule illustrate the high possibility of the dissociation for 100 fs laser pulse. The second approach bases on quantum model of dissociation through B excited electronic state. This model doesn't assume the solving of any time-depended equations. The optimized scheme of iodine dissociation with different nuclear isotopes is obtained. The best isotope separation achieves up to 300 fs with 80% efficiency.
We theoretically study the control of two-photon excitation to bound and dissociative states in a molecule induced by trains of laser pulses, which are equivalent to certain sets of spectral phase modulated pulses. To this end, we solve the time-dependent Schr\"odinger equation for the interaction of molecular model systems with an external intense laser field. Our numerical results for the temporal evolution of the population in the excited states show that, in the case of an excited dissociative state, control schemes, previously validated for the atomic case, fail due to the coupling of electronic and nuclear motion. In contrast, for excitation to bound states the two-photon excitation probability is controlled via the time delay and the carrier-envelope phase difference between two consecutive pulses in the train.
In the last 20 years, advancements in laser technology have allowed for the production of intense laser pulses with durations in the femtosecond (10⁻¹⁵ second) regime, giving scientists the ability to probe nuclear dynamics on their natural time scale. Study of the dissociated fragments created by these intense fields can be used to learn about the molecular structure and dynamics. The work presented in this thesis focuses on controlling this light–molecule interaction in such a way that we can preferentially dissociate the molecule to a desired final product. The hydrogen molecular ion, HD⁺, as well as LiF serve as simple systems that can be studied theoretically for a broad range of laser parameters. Our goal in using these relatively simple systems is to capture the essential physics of the light–molecule interaction and develop general methods to describe these interactions in more complex systems.
The predissociation of a diatomic molecule after excitation by an ultrashort laser pulse leads to a succession of partial nuclear wave packets on the dissociative potential curve. Matter wave interferences result from their evolution. We show here theoretically how control pulses inducing Rabi oscillations on the electronic atomic part of the wave function can change totally the shape of the nuclear interference pattern. This is a consequence of the entanglement between the electronic and nuclear parts of the wave function. Application to information storage is finally discussed.
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.
Three-pulse four-wave mixing (FWM) is used here to study and control laser excitation processes. For general laser excitation processes, after a molecule interacts resonantly with a laser pulse, the molecule has a probability of being in the ground or in the excited state. Control over this process depends on the phase and amplitude of the electric fields that interact with the molecular system. Here we show how three-pulse FWM can be used to control the excitation of iodine molecules. Depending on the time delay between the first two pulses, the observed signal reflects the dynamics of the ground or excited state. A theoretical formalism based on the density matrix formulation is presented and solved for a four-level system. Experiments are found to be in excellent agreement with the theory. The influence of linear chirp on three-pulse FWM experiments is explored. Spectrally dispersed three-pulse FWM is found to be extremely useful for studying the effect of chirp on laser excitation of molecular systems. Experimental demonstrations of these effects are included.