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Register a new userControlling the degree of rotational directionality in laser-induced molecular dynamics
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We demonstrate experimentally a method of varying the degree of directionality in laser-induced molecular rotation. To control the ratio between the number of clockwise and counter-clockwise rotating molecules (with respect to a fixed laboratory axis), we change the polarization ellipticity of the laser field of an optical centrifuge. The experimental data, supported by the numerical simulations, show that the degree of rotational directionality can be varied in a continuous fashion between unidirectional and bidirectional rotation. The control can be executed with no significant loss in the total number of rotating molecules. The technique could be used for studying the effects of orientation of the molecular angular momentum on molecular collisions and chemical reactions. It could also be utilized for controlling magnetic and optical properties of gases, as well as for the enantioselective detection of chiral molecules.
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The relative orientation of colliding molecules plays a key role in determining the rates of chemical processes. Here we examine in detail a prototypical example: rotational quenching of HD in cold collisions with H2. We show that the rotational quenching rate from j=2 -> 0, in the v=1 vibrational level, can be maximized by aligning the HD along the collision axis and can be minimized by aligning the HD at the so called magic angle. This follows from quite general helicity considerations and suggests that quenching rates for other similar systems can also be controlled in this manner.
We consider deflection of polarizable molecules by inhomogeneous optical fields, and analyze the role of molecular orientation and rotation in the scattering process. It is shown that molecular rotation induces spectacular rainbow-like features in the distribution of the scattering angle. Moreover, by preshaping molecular angular distribution with the help of short and strong femtosecond laser pulses, one may efficiently control the scattering process, manipulate the average deflection angle and its distribution, and reduce substantially the angular dispersion of the deflected molecules. We provide quantum and classical treatment of the deflection process. The effects of strong deflecting field on the scattering of rotating molecules are considered by the means of the adiabatic invariants formalism. This new control scheme opens new ways for many applications involving molecular focusing, guiding and trapping by optical and static fields.
We present models for a heteronuclear diatomic molecular ion in a linear Paul trap in a rigid-rotor approximation, one purely classical, the other where the center-of-mass motion is treated classically while rotational motion is quantized. We study the rotational dynamics and their influence on the motion of the center-of-mass, in the presence of the coupling between the permanent dipole moment of the ion and the trapping electric field. We show that the presence of the permanent dipole moment affects the trajectory of the ion, and that it departs from the Mathieu equation solution found for atomic ions. For the case of quantum rotations, we also evidence the effect of the above-mentioned coupling on the rotational states of the ion.
A theoretical justification of the empirical surface hopping method for the laser-driven molecular dynamics is given utilizing the formalism of the exact factorization of the molecular wavefunction [Abedi et al., PRL $textbf{105}$, 123002 (2010)] in its quantum-classical limit. Employing an exactly solvable $textrm H_2^{;+}$-like model system, it is shown that the deterministic classical nuclear motion on a single time-dependent surface in this approach describes the same physics as stochastic (hopping-induced) motion on several surfaces, provided Floquet surfaces are applied. Both quantum-classical methods do describe reasonably well the exact nuclear wavepacket dynamics for extremely different dissociation scenarios. Hopping schemes using Born-Oppenheimer surfaces or instantaneous Born-Oppenheimer surfaces fail completely.
The transition between two distinct mechanisms for the laser-induced field-free orientation of CO molecules is observed via measurements of orientation revival times and subsequent comparison to theoretical calculations. In the first mechanism, which we find responsible for the orientation of CO up to peak intensities of 8 x 10^13 W/cm^2, the molecules are impulsively oriented through the hyperpolarizability interaction. At higher intensities, asymmetric depletion through orientation-selective ionization is the dominant orienting mechanism. In addition to the clear identification of the two regimes of orientation, we propose that careful measurements of the onset of the orientation depletion mechanism as a function of the laser intensity will provide a relatively simple route to calibrate absolute rates of non-perturbative strong-field molecular ionization.
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