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Physical Review A

Photoassociation of cold heteronuclear dimers in static electric fields

Rosario González‐Férez, Matthias Weidemüller, Peter Schmelcher

Published Aug 3, 2007• 21 citations
Publisher

Abstract

The formation of heteronuclear molecules in their electronic ground states from a mixture of two ultracold atomic species via a one-photon stimulated emission process is investigated. The presence of an additional external homogeneous and static electric field is shown to severely influence the induced emission process. Using the LiCs molecule as a prototype, we study the corresponding cross section and its dependence on the continuum energy, final rovibrational state, and static electric field strength. The possibility of controlling the single-photon association process via an additional static electric field is demonstrated.

DOI
10.1103/physreva.76.023402

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The formation of heteronuclear molecules in their electronic ground states from a mixture of two ultracold atomic species via a one-photon stimulated emission process is investigated. The presence of an additional external homogeneous and static electric field is shown to severely influence the induced emission process. Using the LiCs molecule as a prototype, we study the corresponding cross section and its dependence on the continuum energy, final rovibrational state, and static electric field strength. The possibility of controlling the single-photon association process via an additional static electric field is demonstrated.
The formation of ultracold molecules via stimulated emission followed by a radiative de-excitation cascade in the presence of a static electric field is investigated. By analyzing the corresponding cross-sections, we demonstrate the possibility to populate the lowest rotational excitations via photoassociation. The modification of the radiative cascade due to the electric field leads to narrow rotational state distributions in the vibrational ground state. External fields might therefore represent an additional valuable tool towards the ultimate goal of quantum state preparation of molecules.
We theoretically study saturation effects induced by an external static electric field on photoassociation (PA) of a heteronuclear atom pair. A static electric field influences scattering wave-function of two heteronuclear atoms as described in [D. Chakraborty, J. Hazra and B. Deb, J. Phys. B. {\bf 44} 095201 (2011)]. For certain values of electric field strengths there exist anisotropic resonances in ground state scattering leading to a large modification of scattering wave-function at short and intermediate separations where photoassociative Franck-Condon overlap is significant. Photoassociation rate as a function of collision energy shows a splitting near resonant electric field in the mili Kelvin energy regime. This splitting with a prominent dip occurs due to resonant enhancement of free-bound stimulated linewidth leading to saturation in free-bound transitions. We study electric field induced saturation effects on both one- and two-colour PA. Our results suggest that a static electric field may influence the formation of ground state polar molecules in two-colour PA.
We study non-perturbative effects of a static electric field on two-color photoassociation of different atoms. A static electric field induces anisotropy in scattering between two different atoms and hybridizes field-free rotational states of heteronuclear dimers or polar molecules. In a previous paper [D. Chakraborty et al., J. Phys. B 44, 095201 (2011)], the effects of a static electric field on one-color photoassociation between different atoms has been described through field-modified ground-state scattering states, neglecting electric field effects on heteronuclear diatomic bound states. To study the effects of a static electric field on heteronuclear bound states, and the resulting influence on Raman-type two-color photoassociation between different atoms in the presence of a static electric field, we develop a non-perturbative numerical method to calculate static electric field-dressed heteronuclear bound states. We show that the static electric field induced scattering anisotropy as well as hybridization of rotational states strongly influence two-color photoassociation spectra, leading to significant enhancement in PA rate and large shift. In particular, for static electric field strengths of a few hundred kV/cm, two-color PA rate involving high-lying bound states in electronic ground-state increases by several orders of magnitude even in the weak photoassociative coupling regime.
We study the effects of a static electric field on the photoassociation of a heteronuclear atom pair into a polar molecule. The interaction of permanent dipole moment with a static electric field largely affects the ground state continuum wavefunction of the atom pair at short separations where photoassociation transitions occur according to the Franck–Condon principle. Electric field-induced anisotropic interaction between two heteronuclear ground state atoms leads to scattering resonances at some specific electric fields. Near such resonances the amplitude of the scattering wavefunction at short separation increases by several orders of magnitude. As a result, the photoassociation rate is enhanced by several orders of magnitude near the resonances. We discuss in detail electric field-modified atom–atom scattering properties and resonances. We calculate the photoassociation rate that shows giant enhancement due to electric field tunable anisotropic resonances. We present selected results among which particularly important are the excitations of higher rotational levels in ultracold photoassociation due to electric field tunable resonances.
We consider the formation of cold diatomic molecules in the electronic ground state by photoassociation of atoms of dissimilar species. A combination of two transition pathways from the free colliding pair of atoms to a bound vibrational level of the electronic molecular ground state is envisioned. The first pathway consists of a pump-dump scheme with two time-delayed laser pulses in the near-infrared frequency domain. The pump pulse drives the transition to a bound vibrational level of an excited electronic state, while the dump pulse transfers the population to a bound vibrational level of the electronic ground state. The second pathway takes advantage of the existing permanent dipole moment and employs a single pulse in the far-infrared domain to drive the transition from the unbound atoms directly to a bound vibrational level in the electronic ground state. We show that this scheme offers the possibility to coherently control the photoassociation yield by manipulating the relative phase and timing of the pulses. The photoassociation mechanism is illustrated for the formation of cold LiCs molecules.