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arXiv:cond-mat/0508201

Raman-induced oscillation between an atomic and a molecular quantum gas

Changhyun Ryu, Du, X., Emek Yesilada, Artem M. Dudarev, Shoupu Wan, Qian Niu, Daniel J. Heinzen

Published Aug 8, 2005• 10 citations
arXivHTMLPDF

Abstract

It has recently been demonstrated that quantum degenerate gases of very weakly bound molecules can be produced by atomic gases with Feshbach resonances. More strongly bound molecules can be produced with Raman photoassociation of a quantum gas, although this process has not yet been shown to produce a quantum degenerate molecular gas. In principle, Feshbach resonance and Raman photoassociation can be quantum-mechanically reversible, and lead to collective coherent phenomena such as Rabi cycling between an atomic and a molecular gas. However, such atom-molecular coherence has only partly been realized experimentally. Effects that may limit coherence include thermalizing elastic collisions, inelastic collisions, spontaneous Raman scattering, and pairing field formation. Here, we demonstrate a method that circumvents these limitations, based on Raman photoassociation of atoms in an optical lattice and driven into a Mott insulator state. We find that the Raman photoassociation transition is resolved into discrete lines corresponding to the quantized lattice site occupancies, and demonstrate that this provides a new method to accurately determine the distribution of site occupancies and the atom-molecule scattering length. Furthermore, we observe a Raman-induced oscillation of the central core of the gas, containing about 30% of the atoms, between an atomic and a molecular gas.

DOI
10.48550/arxiv.cond-mat/0508201

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It has recently been demonstrated that quantum degenerate gases of very weakly bound molecules can be produced by atomic gases with Feshbach resonances. More strongly bound molecules can be produced with Raman photoassociation of a quantum gas, although this process has not yet been shown to produce a quantum degenerate molecular gas. In principle, Feshbach resonance and Raman photoassociation can be quantum-mechanically reversible, and lead to collective coherent phenomena such as Rabi cycling between an atomic and a molecular gas. However, such atom-molecular coherence has only partly been realized experimentally. Effects that may limit coherence include thermalizing elastic collisions, inelastic collisions, spontaneous Raman scattering, and pairing field formation. Here, we demonstrate a method that circumvents these limitations, based on Raman photoassociation of atoms in an optical lattice and driven into a Mott insulator state. We find that the Raman photoassociation transition is resolved into discrete lines corresponding to the quantized lattice site occupancies, and demonstrate that this provides a new method to accurately determine the distribution of site occupancies and the atom-molecule scattering length. Furthermore, we observe a Raman-induced oscillation of the central core of the gas, containing about 30% of the atoms, between an atomic and a molecular gas.
This thesis describes the results of several experiments that studied the photoassociation of an ultracold atomic Rb gas. In the first experiment, we produced ultracold diatomic molecules from an atomic gas via single-color photoassociation. The molecules were detected with resonance-enhanced multiphoton ionization. Trapping of these molecules in a quadrupole magnetic trap, with lifetimes up to 20 seconds, was also demonstrated. In addition, the rate constant for inelastic collisions between the trapped molecules and atoms was determined from measurements of the atomic density dependence of the decay rate of the trapped molecules. In another experiment, stimulated Raman photoassociation of Rb atoms in a Mott insulator state was studied. A Bose-Einstein condensate (BEC) of 87Rb atoms was loaded into a three-dimensional optical lattice formed by the interference pattern of three orthogonal standing wave laser fields. This system constitutes a very good realization of the Bose-Hubbard model, which predicts a quantum phase transition between a superfluid state and a Mott insulator state at a particular lattice height. A time-of-flight imaging method was used to study the state of the atomic gas, and the quantum phase transition was observed at the predicted lattice height. The signature of the phase transition was the disappearance and reappearance of peaks in the image that arose from the interference of atoms originating from different lattice sites. Two coherent laser fields were applied to the gas in its Mott insulating state, and tuned close to a Raman photoassociation resonance, and this resulted in an observable loss of atoms due to the formation of molecules. This transition exhibited a double-peaked spectrum, with one of the peaks arising from photoassociation of atoms in sites containing only two atoms, and the other from sites containing three atoms. Also, the loss of atoms vs. the duration of the Raman photoassociation period was studied, with the lasers tuned to the peak corresponding to two atoms per site. It was found that a central core of the gas, containing about 40 percent of the atoms, exhibited a coherent oscillation between an atomic and molecular quantum gas.
We observe large-amplitude Rabi oscillations between an atomic and a molecular state near a Feshbach resonance. The experiment uses 87Rb in an optical lattice and a Feshbach resonance near 414 G. The frequency and amplitude of the oscillations depend on the magnetic field in a way that is well described by a two-level model. The observed density dependence of the oscillation frequency agrees with theoretical expectations. We confirmed that the state produced after a half-cycle contains exactly one molecule at each lattice site. In addition, we show that, for energies in a gap of the lattice band structure, the molecules cannot dissociate.
Photoassociation and the Feshbach resonance are, in principle, feasible means for creating a molecular Bose-Einstein condensate from an already-quantum-degenerate gas of atoms; however, mean-field shifts and irreversible decay place practical constraints on the efficient delivery of stable molecules using either mechanism alone. We therefore propose Feshbach-stimulated Raman photoproduction, i.e., a combination of magnetic and optical methods, as a means to collectively convert degenerate atoms into a stable molecular condensate with near-unit efficiency.
We reveal the existence of high-density Feshbach resonances in the collision between the ground and metastable states of ^{171}Yb and coherently produce the associated Feshbach molecules by photoassociation. The extremely small transition rate is overcome by the enhanced Franck-Condon factor of the weakly bound Feshbach molecule, allowing us to observe Rabi oscillations with long decay time between an atom pair and a molecule in an optical lattice. We also perform the precision measurement of the binding energies, which characterizes the observed resonances. The ultranarrow photoassociation will be a basis for practical implementation of optical Feshbach resonances.
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, >10−10cm3/s,> 10^{-10} cm^{3}/s,>10−10cm3/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.