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Quasi-classical model of dynamic molecular structure and non-destructive wavepacket manipulation by ultrashort laser pulses

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 Added by William Bryan
 Publication date 2010
  fields Physics
and research's language is English




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A quasi-classical model (QCM) of molecular dynamics in intense femtosecond laser fields has been developed, and applied to a study of the effect of an ultrashort `control pulse on the vibrational motion of a deuterium molecular ion in its ground electronic state. A nonadiabatic treatment accounts for the initial ionization-induced vibrational population caused by an ultrashort `pump pulse. In the QCM, the nuclei move classically on the molecular potential as it is distorted by the laser-induced Stark shift and transition dipole. The nuclei then adjust to the modified potential, non-destructively shifting the vibrational population and relative phase. This shift has been studied as a function of control pulse parameters. Excellent agreement is observed with predictions of time-dependent quantum simulations, lending confidence to the validity of the model and permitting new observations to be made. The applicability of the QCM to more complex multi-potential energy surface molecules (where a quantum treatment is at best difficult) is discussed.



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We investigate experimentally the effect of quantum resonance in the rotational excitation of the simplest quantum rotor - a diatomic molecule. By using the techniques of high-resolution femtosecond pulse shaping and rotational state-resolved detection, we measure directly the amount of energy absorbed by molecules interacting with a periodic train of laser pulses, and study its dependence on the train period. We show that the energy transfer is significantly enhanced at quantum resonance, and use this effect for demonstrating selective rotational excitation of two nitrogen isotopologues, $ ^{14}N_2$ and $ ^{15}N_2$. Moreover, by tuning the period of the pulse train in the vicinity of a fractional quantum resonance, we achieve spin-selective rotational excitation of para- and ortho-isomers of $ ^{15}N_2$.
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