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Physical Review A

Nonspreading wave packets of diatomic molecules: Generation and control

Jung‐Hoon Kim, Jian‐Min Yuan, Wing‐Ki Liu, Chang Hee Nam

Published Mar 21, 2001• 4 citations
Publisher

Abstract

A circularly polarized electric field is used to create a trap that can guide the rotational motion of diatomic molecules. Theoretical analyses and numerical calculations support the existence of trapped nonspreading wave packets rotating with a electric field. Optimal coherent control of the rotational motion of diatomic molecules can be achieved by manipulating the nonspreading wave packets with a circularly polarized electric field whose amplitude and frequency are changed adiabatically.

DOI
10.1103/physreva.63.043420

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A circularly polarized electric field is used to create a trap that can guide the rotational motion of diatomic molecules. Theoretical analyses and numerical calculations support the existence of trapped nonspreading wave packets rotating with a electric field. Optimal coherent control of the rotational motion of diatomic molecules can be achieved by manipulating the nonspreading wave packets with a circularly polarized electric field whose amplitude and frequency are changed adiabatically.
Selection of state-insensitive or ``magic'' trapping conditions with ultracold atoms or molecules, where pairs of internal states experience identical trapping potentials, brings substantial benefits to precision measurements and quantum computing schemes. Working at such conditions could ensure that the detrimental effects of inevitable inhomogeneities across an ultracold sample are significantly reduced. However, this aspect of confinement remains unexplored for ultracold polar molecules. Here, we present means to control the ac Stark shift of rotational states of ultracold diatomic polar molecules, when subjected to both trapping laser light and an external electric field. We show that both the strength and relative orientation of the two fields influence the trapping potential. In particular, we predict ``magic electric field strengths'' and a ``magic angle,'' where the Stark shift is independent of the dc external field for certain rotational states of the molecule.
Tailored microwave pulses, to guide asymmetric-top molecules from selected rotational states belonging to the vibronic ground state to generalized angular-momentum coherent states, are designed by using optimal control theory. Characteristics that the molecules have to fulfill in order to achieve the goal with feasible pulses are discussed. Properties of the pulses are discussed as well. The further dephasing among the components of the wave packet which, for the simplest coherent state, is a form of dynamical tunneling, can be locked by exploiting the changes that energy levels and eigenfunctions undergo in the presence of an external static electric field with appropriate intensity. For the special case with M=0M=0M=0, periodic fields are more flexible in avoiding dephasing. This is shown by examining properties of quasienergies and dressed states resulting from the diagonalization of a truncated Floquet matrix.
We study the quantum dynamics of diatomic molecule driven by a circularly polarized resonant electric field. We look for a quantum effect due to classical chaos appearing due to the overlapping of nonlinear reso-nances associated to the vibrational and rotational motion. We solve the Schrödinger equation associated with the wave function expanded in term of proper stationary states, |n> |lm> (vibrational angular momentum states). Looking for quantum-classic correspondence, we consider the Liouville dynamics in the two dimensional phase space defined by the coherent-like state of vibrational states. We consider the rela-tionship between the overlapping of the classical resonances and the mixing of the quantum states, and it is found some similarities when the quantum dynamics is pictured in terms of number and phase operators.
The paper is devoted to the theoretical study of the possibility of coherent control of the vibrational-rotational transitions in diatomic molecule under the action of bichromatic laser field. Two possible absorption branches are considered. Dependencies of the control efficiency upon the parameters involved such as gas temperature and electric field amplitudes of the monochromatic components are investigated. Numerical calculations are performed for the case of CO molecule in Morse approximation. The possibility of the efficient coherent control of the considered process is demonstrated.
Summary form only given. One of the most enticing notions of modern optical physics is the idea that one can manipulate the quantum state of atoms and molecules, and thus engineer the properties of matter at its most fundamental level. Homonuclear diatomic molecules are model systems for studying quantum control. They have several degrees of freedom associated with different particles (three are particularly useful: the internuclear vibrational and rotational coordinates and the electronic coordinate) and each degree of freedom has a low dissipation rate as compared to its characteristic frequency. The coupling of the electronic and vibrational degree of freedom allows the preparation of arbitrary vibrational wave packets in both excited and ground electronic states of the molecules by the application of optical radiation.
In this paper we propose to control the bond length of a diatomic molecule and its vibrational coherent motion over arbitrary distances. The method requires (a) mixing a dissociative potential with bound electronic configurations in order to stabilize the continuum, and (b) manipulating the wave-packet transfer below the threshold of adiabatic passage. Using asymmetric pulses it is possible to implement sudden-adiabatic transitions to stop or induce the motion in the light-induced potential, controlling the nonadiabatic dynamics in a most efficient way.