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arXiv:cond-mat/0409327 · Physical Review Letters

Coherent Molecular Optics Using Ultracold Sodium Dimers

J. R. Abo-Shaeer, Daniel E. Miller, J. K. Chin, K. Xu, Takashi Mukaiyama, Wolfgang Ketterle

Published Feb 3, 2005• 30 citations
arXivHTMLPDF

Abstract

Coherent molecular optics is performed using two-photon Bragg scattering. Molecules were produced by sweeping an atomic Bose-Einstein condensate through a Feshbach resonance. The spectral width of the molecular Bragg resonance corresponded to an instantaneous temperature of 20 nK, indicating that atomic coherence was transferred directly to the molecules. An autocorrelating interference technique was used to observe the quadratic spatial dependence of the phase of an expanding molecular cloud. Finally, atoms initially prepared in two momentum states were observed to cross pair with one another, forming molecules in a third momentum state. This process is analogous to sum-frequency generation in optics.

DOI
10.1103/physrevlett.94.040405

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Coherent molecular optics is performed using two-photon Bragg scattering. Molecules were produced by sweeping an atomic Bose-Einstein condensate through a Feshbach resonance. The spectral width of the molecular Bragg resonance corresponded to an instantaneous temperature of 20 nK, indicating that atomic coherence was transferred directly to the molecules. An autocorrelating interference technique was used to observe the quadratic spatial dependence of the phase of an expanding molecular cloud. Finally, atoms initially prepared in two momentum states were observed to cross pair with one another, forming molecules in a third momentum state. This process is analogous to sum-frequency generation in optics.
Abstract Recent advances in the precise control of ultracold atomic systems have led to the realisation of Bose–Einstein condensates (BECs) and degenerate Fermi gases. An important challenge is to extend this level of control to more complicated molecular systems. One route for producing ultracold molecules is to form them from the atoms in a BEC. For example, a two-photon stimulated Raman transition in a 87Rb BEC has been used to produce 87Rb2 molecules in a single rotational-vibrational state1, and ultracold molecules have also been formed2 through photoassociation of a sodium BEC. Although the coherence properties of such systems have not hitherto been probed, the prospect of creating a superposition of atomic and molecular condensates has initiated much theoretical work3, 4, 5, 6, 7. Here we make use of a time-varying magnetic field near a Feshbach resonance8, 9, 10, 11, 12 to produce coherent coupling between atoms and molecules in a 85Rb BEC. A mixture of atomic and molecular states is created and probed by sudden changes in the magnetic field, which lead to oscillations in the number of atoms that remain in the condensate. The oscillation frequency, measured over a large range of magnetic fields, is in excellent agreement with the theoretical molecular binding energy, indicating that we have created a quantum superposition of atoms and diatomic molecules—two chemically different species.
Ultracold sodium molecules were produced from an atomic Bose-Einstein condensate by ramping an applied magnetic field across a Feshbach resonance. More than 10(5) molecules were generated with a conversion efficiency of approximately 4%. Using laser light resonant with an atomic transition, the remaining atoms could be selectively removed, preventing fast collisional relaxation of the molecules. Time-of-flight analysis of the pure molecular sample yielded an instantaneous phase-space density greater than 20.
Chemical reactions in a statistical ensemble are conventionally regarded as incoherent processes driven by thermodynamics. In the quantum degenerate regime, where atoms and molecules form coherent matter waves, reactions are theoretically described by nonlinear mixing of matter-wave fields. In this scenario, we expect phase matching between reactants and products, analogous to the mixing of photonic fields in nonlinear optics. Here we report on the observation of phase coherent reaction dynamics of Bose-condensed atoms and molecules near a Feshbach resonance. Using matter-wave diffraction with optical lattices, we verify spatial coherence of both atoms and molecules and observe phase doubling when atomic waves combine into molecular waves, the matter-wave analogue of optical frequency doubling. The diffraction patterns further reveal two-atom entanglement generated during the reaction. Our observations establish phase coherence and entanglement generation as two essential features of "quantum many-body chemistry". Moreover, our work opens a pathway to control of reaction dynamics by manipulation of matter-wave phases.
This thesis reports on the first observation of optical tuning of interactions in an ultracold atomic gas. To control the elastic interactions, we use optically induced scattering resonances. They are realized by coupling pairs of atoms to a bound molecular state with the help of laser light. In comparison to the well-known magnetic Feshbach resonances, these optical Feshbach resonances allow a very fast switching of interactions in a spatially resolved way. This is because laser light can be switched on and off much faster than magnetic fields and because the light intensity can be spatially structured. Our experiments are performed with a Bose-Einstein condensate (BEC) of Rb atoms, which we produce in our new BEC setup. This apparatus has been constructed in the framework of this thesis and offers excellent optical access to the ultracold atom cloud. To investigate the tunability of atomic interactions with single-frequency laser light, we optically couple pairs of free atoms to an electronically excited molecular state. The coupling is achieved with a laser that is tuned close to the respective free-bound photoassociation transition. By changing the laser detuning we are able to adjust the atomic scattering length to any value between 10 a0 and 190 a0, where a0 denotes the Bohr radius. The atomic scattering length is a single quantity that fully describes ultracold elastic interactions. Since laser induced atom losses restrict the duration of our experiments, Bragg spectroscopy is employed as a fast method to measure the scattering length. We also demonstrate that optical Feshbach resonances can be realized with a two-color Raman coupling scheme. To implement this scheme, a second laser is added that couples the excited molecular state to a weakly bound molecular level in a ground state potential. Tuning the second laser results in a modification of the atomic scattering length similar to the one observed with a single laser. In addition, this scheme allows to control the width of the resonance via the detuning of the first laser. For the one-color and two-color coupling schemes, we investigate how the elastic scattering properties depend on the different available parameters, i.e. the laser detunings and intensities. Our experimental findings can successfully be described with an available theoretical model, which treats ultracold collisions in the presence of laser light. Optical Feshbach resonances have the possibility of becoming a valuable tool for fast switching of interactions. This is of special interest in quantum computation schemes with neutral atoms, where interactions between different atomic qubits need to be controlled.
We calculate the number statistics of a single-mode molecular field excited by photo-association or via a Feshbach resonance from an atomic Bose-Einstein condensate (BEC), a normal atomic Fermi gas, and a Fermi system with pair correlations (BCS state). We find that the molecule formation from a BEC leads for short times to a coherent molecular state in the quantum optical sense. Atoms in a normal Fermi gas, on the other hand, result for short times in a molecular field analog of a classical chaotic light source. The BCS situation is intermediate between the two and goes from producing an incoherent to a coherent molecular field with an increasing gap parameter. This distinct signature of the initial atomic state in the resulting molecular field makes single molecule counting into a powerful diagnostic tool.