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Physical Review A

Quantum superchemistry: Role of trapping profile and quantum statistics

M. K. Olsen

Published Jan 5, 2004• 24 citations

Abstract

The process of Raman photoassociation of a trapped atomic condensate to form condensed molecules has been labeled superchemistry because it can occur at 0 K and experiences coherent bosonic stimulation. We show here that the differences from ordinary chemical processes go even deeper, with the conversion rates depending on the quantum state of the reactants, as expressed by the Wigner function. We consider different initial quantum states of the trapped atomic condensate and different forms of the confining potentials, demonstrating the importance of the quantum statistics and the extra degrees of freedom which massive particles and trapping potentials make available over the analogous optical process of second-harmonic generation. We show that both mean-field analyses and quantum calculations using an inappropriate initial condition can make inaccurate predictions for a given system. This is possible whether using a spatially dependent analysis or a zero-dimensional approach as commonly used in quantum optics.

DOI: 10.1103/physreva.69.013601

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The process of Raman photoassociation of a trapped atomic condensate to form condensed molecules has been labeled superchemistry because it can occur at 0 K and experiences coherent bosonic stimulation. We show here that the differences from ordinary chemical processes go even deeper, with the conversion rates depending on the quantum state of the reactants, as expressed by the Wigner function. We consider different initial quantum states of the trapped atomic condensate and different forms of the confining potentials, demonstrating the importance of the quantum statistics and the extra degrees of freedom which massive particles and trapping potentials make available over the analogous optical process of second-harmonic generation. We show that both mean-field analyses and quantum calculations using an inappropriate initial condition can make inaccurate predictions for a given system. This is possible whether using a spatially dependent analysis or a zero-dimensional approach as commonly used in quantum optics.

We show that the photoassociation of an atomic Bose-Einstein condensate to form condensed molecules is a chemical process which not only does not obey the Arrhenius rules for chemical reactions, but that it can also depend on the quantum statistics of the reactants. Comparing the predictions of a truncated Wigner representation for different initial quantum states, we find that, even when the quantum prediction for an initial coherent state is close to the Gross-Pitaevskii prediction, other quantum states may result in very different dynamics.

We use numerical integration of coupled differential equations in a truncated Wigner representation to show that the initial quantum state of an atomic Bose-Einstein condensate plays an important role in the process of Raman photoassociation to form a molecular condensate. Comparing the predictions for different initial quantum states, we find that, even when the stochastic prediction for an initial coherent state is close to the Gross-Pitaevskii prediction, other possible states may result in very different dynamics. The mean-field dynamics can be appreciably different, depending on the initial conditions.

By stochastic modeling of the process of Raman photoassociation of Bose-Einstein condensates, we show that, the farther the initial quantum state is from a coherent state, the farther the one-dimensional predictions are from those of the commonly used zero-dimensional approach. We compare the dynamics of condensates, initially in different quantum states, finding that, even when the quantum prediction for an initial coherent state is relatively close to the Gross-Pitaevskii prediction, an initial Fock state gives qualitatively different predictions. We also show that this difference is not present in a single-mode type of model, but that the quantum statistics assume a more important role as the dimensionality of the model is increased. This contrasting behavior in different dimensions, well known with critical phenomena in statistical mechanics, makes itself plainly visible here in a mesoscopic system and is a strong demonstration of the need to consider physically realistic models of interacting condensates.

Photoassociation is a process by which two cold, trapped atoms can be optically excited during a collision to make a vibrational level of an excited electronic state of a molecular dimer. High-resolution photoassociation spectra are now well-known for most alkali dimers. The upper level normally decays by spontaneous emission to a number of final molecular levels, bound and unbound. A laser of a second color can be used to stimulate a transition from the upper level to a particular ground state vibrational level. Such a Raman photoassociation process can be used to form translationally cold molecules in a cold atomic gas or a Bose-Einstein condensate. Coupled channels scattering calculations show that the collisional rate coefficient for coherent production of molecules in specific target states,

> 10^{-10} cm^{3}/s,

can greatly exceed the rate coefficient for forming products due to excited state spontaneous decay. This implies the feasibility of rapid coherent conversion of atom pairs in a condensate to molecules on a time scale short compared to the trap oscillation time. The untrapped molecules can form a coherent molecular beam. We will examine the prospects for the experimental realization of photoassociative molecule formation in cold alkali gases or condensates.

A Raman photoassociation process can be used to form translationally cold molecules from a Bose-Einstein condensate. Coupled-channels scattering calculations show that the rate coefficient for coherent production of molecules in specific target states, $>{10}^{\ensuremath{-}10} {\mathrm{cm}}^{3}/\mathrm{s},$ can greatly exceed the rate coefficient for heating and loss channels due to excited-state spontaneous decay. This implies the feasibility of rapid coherent conversion of atom pairs in a condensate to molecules on a time scale short compared to the trap oscillation time.