11 February 2011 Optimal control of the population dynamics of the ground vibrational state of a polyatomic molecule
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Simulating coherent control with femtosecond pulses on a polyatomic molecule with anharmonic splitting was demonstrated. The simulation mimicked pulse shaping of a Spatial Light Modulator (SLM) and the interaction was described with the Von Neumann equation. A transform limited pulse with a fluence of 600 J/m2 produced 18% of the population in an arbitrarily chosen upper vibrational state, n =2. Phase only and amplitude only shaped pulse produced optimum values of 60% and 40% respectively, of the population in the vibrational state, n=2, after interaction with the ultra short pulse. The combination of phase and amplitude shaping produced the best results, 80% of the population was in the targeted vibrational state, n=2, after interaction. These simulations were carried out with all the population initially in the ground vibrational level. It was found that even at room temperatures (300 Kelvin) that the population in the selected level is comparable with the case where all population is initially in the ground vibrational state. With a 10% noise added to the amplitude and phase masks, selective excitation of the targeted vibrational state is still possible.
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Ludwig E. de Clercq, Ludwig E. de Clercq, Lourens R. Botha, Lourens R. Botha, Erich G. Rohwer, Erich G. Rohwer, Hermann Uys, Hermann Uys, Anton Du Plessis, Anton Du Plessis, "Optimal control of the population dynamics of the ground vibrational state of a polyatomic molecule", Proc. SPIE 7925, Frontiers in Ultrafast Optics: Biomedical, Scientific, and Industrial Applications XI, 79250V (11 February 2011); doi: 10.1117/12.874562; https://doi.org/10.1117/12.874562

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