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Physical Review A

Coherent control of matter-wave interference in molecular predissociation

J. Degert, Christoph Meier, B. Chatel, B. Girard

Published Apr 25, 2003• 13 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.67.041402

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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.
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Laser Induced Dissociation Control of H2+H_2^+H2+​ and H32+H_3^{2+}H32+​
Laser induced dissociation control of the symmetric diatomic molecular ion H2+H_2^+H2+​ and the triatomic molecular ion H32+H_3^{2+}H32+​ is discussed. The simulation results demonstrate that a long-wavelength terahertz or mid-infrared laser pulse can be used to control the electrons of the dissociative states after the excitation of an ultrashort ultraviolet (UV) laser pulse. For H2+,H_2^+,H2+​, there exists an effective time, which increases with increasing pulse duration of the UV laser pulse, for controlling the molecular dissociation. For the electrons of the 1sσg1sσ_g1sσg​ state, they move along the polarization direction of the dissociation control electric field. In contrast, for the electrons of the 2pσu2pσ_u2pσu​ state, they move in the opposite direction to that of the electric force. And for the triatomic molecule H32+H_3^{2+}H32+​, the electron dissociation control can also be realized by changing the central wavelength of the exciting UV pulse.
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 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+​.
We study wave packet interferometry (WPI) considering the laser pulse fields both classical and quantum mechanically. WPI occurs in a molecule after subjecting it to the interaction with a sequence of phase-locked ultrashort laser pulses. Typically, the measured quantity is the fluorescence of the molecule from an excited electronic state. This signal has imprinted the interference of the vibrational wave packets prepared by the different laser pulses of the sequence. The consideration of the pulses as quantum entities in the analysis allows us to study the entanglement of the laser pulse states with the molecular states. With a simple model for the molecular system, plus several justified approximations, we solve for the fully quantum mechanical molecule-electromagnetic field state. We then study the reduced density matrices of the molecule and the laser pulses separately. We calculate measurable corrections to the case where the fields are treated classically.
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.