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The Journal of Chemical Physics

Pump-dump iterative squeezing of vibrational wave packets

Bo Y. Chang, Ignacio R. Solá

Published Dec 22, 2005• 9 citations
Publisher

Abstract

The free motion of a nonstationary vibrational wave packet in an electronic potential is a source of interesting quantum properties. In this work we propose an iterative scheme that allows continuous stretching and squeezing of a wave packet in the ground or in an excited electronic state, by switching the wave function between both potentials with pi pulses at certain times. Using a simple model of displaced harmonic oscillators and delta pulses, we derive the analytical solution and the conditions for its possible implementation and optimization in different molecules and electronic states. We show that the main constraining parameter is the pulse bandwidth. Although in principle the degree of squeezing (or stretching) is not bounded, the physical resources increase quadratically with the number of iterations, while the achieved squeezing only increases linearly.

DOI
10.1063/1.2139091

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Iterative vibrational wave packet squeezing by a sequence of femtosecond pulses is proposed. Analytic formulas are derived for the harmonic oscillator case, and the practical implementation of the scheme is tested on different electronic transitions in Rb2{\mathrm{Rb}}_{2}Rb2​.
We propose a scheme for squeezing vibrational wave packets in the ground (or excited) states of diatomic molecules that uses pulse sequences of strong nonresonant short pulses. The physical mechanism of the scheme is a two step process involving adiabatic and diabatic transformations of the wave packet. The first step is the adiabatic stretching of the wave packet on a light-induced potential, and the second step is dynamic squeezing by free evolution after ultrashort (i.e., diabatic) population transfer. We show that this sequence of transformations can be performed very efficiently with a simple two pulse sequence with slow switch on and fast switch off pulse shapes, and we analyze the required physical resources that are needed. We test the scheme on a model of harmonic oscillators and on the Rb2{\mathrm{Rb}}_{2}Rb2​ dimer. Finally, different possible generalizations are proposed.
We combine theories of optimal pump-dump control and the related transient probe absorption spectroscopy in order to elucidate the relation between these two optical processes and the possibility of experimental realization. In the weak response regime, we identify the globally optimal pair of pump-dump control fields, and further propose a second-order difference detection scheme to monitor the wave packets dynamics that is jointly controlled by both the pump and dump fields. The globally optimal solution serves also as the initial input for the iterative search for the optimal control fields in the strong response regime. We use a model I2 molecule to demonstrate numerically the pump-dump control and the detection of a highly vibrationally excited wave packet focusing dynamics on the ground X surface in both the weak and strong response regimes. The I2B surface serves as the intermediate to assist the pump-dump control and the optical detection processes. Demonstrated in the strong response regime are the optimal pair of pump-dump molecular-π pulses that invert nearly total population onto the predefined target region within a half period of vibration motion.
In a model system, i.e. the K2 dimer molecule, a vibrationally excited wave packet around a prechosen target state in the electronic ground state is generated by an ultrafast resonant stimulated Raman process. By choosing the pump and dump wavelengths along the difference potential between the excited electronic |B〉-state and the electronic ground state |X〉 and optimizing the delay time between the pump and dump processes, one can increase considerably the efficiency of the population transfer of this quantum control experiment. Copyright © 2000 John Wiley & Sons, Ltd.
We introduce a general formalism, based on the stochastic formulation of quantum mechanics, to obtain localized quasi-classical wave packets as dynamically controlled systems, for arbitrary anharmonic potentials. The control is in general linear, and it amounts to introduce additional quadratic and linear time-dependent terms to the given potential. In this way one can construct for general systems either coherent packets moving with constant dispersion, or dynamically squeezed packets whose spreading remains bounded for all times. In the standard operatorial framework our scheme corresponds to a suitable generalization of the displacement and scaling operators that generate the coherent and squeezed states of the harmonic oscillator.
The evolution operator of a Caldirola-Kanai type quantum parametric oscillator with a generalized quadratic Hamiltonian is obtained using the Wei-Norman Lie algebraic approach, and time evolution of the eigenstates of a harmonic oscillator and Glauber coherent states is found explicitly. Behavior of this oscillator is investigated under the influence of the external mixed term B(t)(q^p^+p^q^)/2, which affects the squeezing properties of the wave packets, and linear terms D0(t)q^, E0(t)p^ responsible for their displacement in time. According to this, we construct all exact quantum models with different parameters B(t), for which the structure of the Caldirola-Kanai oscillator in position space is preserved. Then, for each model, we obtain explicit solutions and analyze the squeezing and displacement properties of the wave packets according to the frequency modification by B(t) and periodic forces in the corresponding classical equation of motion.