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Physical Review Letters

Rabi Oscillations Between Dissociative Molecular States

S. Magnier, Maurizio Persico, N. K. Rahman

Published Sep 13, 1999• 44 citations
Publisher

Abstract

We establish for the first time the proper conditions to observe Rabi oscillations between vibrationally dissociative states belonging to different electronic terms of a diatomic molecule. We show by wave packet dynamics simulations that such a process is feasible with the molecular ion ${\mathrm{Na}}_{2}^{+}$.

DOI
10.1103/physrevlett.83.2159

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We establish for the first time the proper conditions to observe Rabi oscillations between vibrationally dissociative states belonging to different electronic terms of a diatomic molecule. We show by wave packet dynamics simulations that such a process is feasible with the molecular ion Na2+{\mathrm{Na}}_{2}^{+}Na2+​.
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 observe large-amplitude Rabi oscillations between an atomic and a molecular state near a Feshbach resonance. The experiment uses 87Rb in an optical lattice and a Feshbach resonance near 414 G. The frequency and amplitude of the oscillations depend on the magnetic field in a way that is well described by a two-level model. The observed density dependence of the oscillation frequency agrees with theoretical expectations. We confirmed that the state produced after a half-cycle contains exactly one molecule at each lattice site. In addition, we show that, for energies in a gap of the lattice band structure, the molecules cannot dissociate.
The vibrational motion equations of both homo- and hetero-nuclei diatomic molecules are here derived for the first time. A diatomic molecule is first considered as a quantum mechanics oscillator. The second- and third-order Hamiltonian operators are then formed by substituting the number operator for the quantum number in the corresponding energy eigenvalues. The temporal variations of relative position and linear momentum of two oscillating atoms are calculated by solving Heisenberg's equations of motion. The results indicate that the oscillatory behaviour of diatomic molecules are described by the wave packets which consisted of two different frequencies. The stability theory of optical oscillators (lasers) is then exploited to determine the stability conditions of an oscillating diatomic molecule in the different energy levels of Morse potential. It peculiarly turned out that the diatomic molecules are exactly dissociated at the energy level in which their equations of motion become unstable. We also determine the minimum oscillation frequency (cut-off frequency) of a diatomic molecule at the dissociation level of Morse potential.
Wave-mechanical phenomena such as resonance and interference, in both light and matter, are central to the principles of quantum coherent control over molecular processes. Focusing on the dynamical aspects, this dissertation is a compilation of studies on the interaction physics involving wave packets in molecules, the driving light field, and the underlying coherence and control. In each work, we will demonstrate interesting correlations between the properties of a carefully designed excitation light field and desirable outcomes of the molecules quantum dynamics. We will analyze the dynamical effect of a Feshbach resonance in the adiabatic Raman photoassociation for ultracold diatomic molecule formation from ultracold atoms. A narrow resonance is shown to be able to increase the effective number of collisions, in an ultracold atomic gas, that are available for photoassociation. This results in an optimal resonance width much smaller than the atomic collision energy bandwidth, due to the balance between the effective collision rate and single-collision transfer probability. Next, we demonstrate the linear molecular response to high-intensity, broadband, shaped optical fields. We show that this originates from interferences based on intra-pulse Raman excitations, and thus response linearity is not unique to the first-order perturbative limit and can not be used to infer the strength of the field. In the last study, we simulate the stochastic vibrational wave packet and dissociation-flux dynamics in a molecule excited by light with temporal and spectral incoherent properties. Between this case and that using a coherent pulse with the same spectral profile, we compare the vibrational wave functions and the loss of electronic and vibrational coherence, and demonstrate the qualitative difference between coherently and incoherently driven dynamics in molecules.