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Physical Review A

Coherent photoassociation of a Bose-Einstein condensate

Juha Javanainen, Matt Mackie

Published May 1, 1999• 168 citations
Publisher

Abstract

We propose a phenomenological Hamiltonian for the analysis of photoassociation of a Bose-Einstein condensate. We find that, by adiabatically sweeping the frequency of the driving laser, a condensate of atoms may be converted rapidly to a condensate of molecules.
DOI
10.1103/physreva.59.r3186

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We study coherent photoassociation, phenomena analogous to coherent optical transients in few-level systems, which may take place in photoassociation of an atomic Bose-Einstein condensate but not in a nondegenerate gas. We develop a second-quantized Hamiltonian to describe photoassociation, and apply the Hamiltonian both in the momentum representation and in the position representation (field theory). The solution of the two-mode problem, including only one mode each for the atomic and molecular condensates, displays analogs of Rabi oscillations and rapid adiabatic passage. A classical version of the field theory for atoms and molecules is used to demonstrate that, in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of density fluctuations. Experimental complications, including spontaneous emission and unwanted ``rogue'' photodissociation from a photoassociated molecule, are analyzed. A two-color Raman scheme is studied as a method to set up an effective two-mode scheme with reduced spontaneous-emission losses. We discuss photoassociation rates and photoassociation Rabi frequencies for high-lying vibrational states in alkali dimers both on the basis of molecular-structure calculations, and by comparing with an experiment [Wynar et al., Science 287, 1016 (2000)].
A study of coherent photoassociation is presented for the case of an atomic Bose-Einstein condensate. It is shown that the phenomenon is analogous to coherent optical transient in a few-level system, with a difference that the participating levels have Bose enhanced populations. A second-quantized Hamiltonian in momentum and position representation is developed to describe photoassociation. A classical version of the field theory for atoms and molecules is used to demonstrate that in the presence of photoassociating light, a joint atom-molecule condensate is unstable against the growth of the density fluctuations. ^ A simple mean-field model of atom-molecule Bose-Einstein condensate is constructed and it is shown that in the model there is no collapse, irrespective of the sign of the effective atom-atom scattering length. The properties of the two most important eigenstates, the ground state and the twin state, are determined for different values of the system parameters δ and K, the detuning and the atom-molecule coupling, respectively. It is shown that in a coupled atom-molecule system a collapse is replaced by a dynamical instability. The lines in the parameter space where these instabilities occur are in fact fractures where the underlying eigenstates discontinuously change. The features of instability are in good qualitative agreement with the experimental observations of collapse. ^
A dynamical many-body theory of single color photoassociation in a Bose-Einstein condensate is presented. The theory describes the time evolution of a condensed atomic ensemble under the influence of an arbitrarily varying near-resonant laser pulse, which strongly modifies the binary scattering properties. In particular, when considering situations with rapid variations and high light intensities the approach described in this article leads, in a consistent way, beyond standard mean-field techniques. This allows one to address the question of limits to the photoassociation rate due to many-body effects which has caused extensive discussions in the recent past. Both the possible loss rate of condensate atoms and the amount of stable ground-state molecules achievable within a certain time are found to be stronger limited than according to mean-field theory. By systematically treating the dynamics of the connected Green's function for pair correlations the resonantly driven population of the excited molecular state as well as scattering into the continuum of noncondensed atomic states are taken into account. A detailed analysis of the low-energy stationary scattering properties of two atoms modified by the near resonant photoassociation laser, in particular of the dressed state spectrum of the relative motion prepares for the analysis of the many-body dynamics. The consequences of the finite lifetime of the resonantly coupled bound state are discussed in the two-body as well as in the many-body context. Extending the two body description to scattering in a tight trap reveals the modifications to the near resonant adiabatic dressed levels caused by the decay of the excited molecular state.
We analyze coherent two-color photoassociation of a Bose-Einstein condensate, focusing on stimulated Raman adiabatic passage (STIRAP) in free-bound-bound transitions from atoms to molecules. This problem raises an interest because STIRAP has been predicted to be absent in the nondegenerate case [Javanainen and Mackie, Phys. Rev. A 58, R789 (1998)]. Nevertheless, we find that Bose stimulation enhances the free-bound dipole matrix element for an atomic condensate, and photoassociative STIRAP turns out to be a viable mechanism for converting an atomic condensate to a molecular condensate with near-unit efficiency.