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arXiv:1308.4118 · Physical Review Letters

Rabi Oscillations between Atomic and Molecular Condensates Driven with Coherent One-Color Photoassociation

Mi Yan, B. J. DeSalvo, Ying Huang, Pascal Naidon, T. C. Killian

Published Oct 10, 2013• 36 citations
arXivHTMLPDF

Abstract

We demonstrate coherent one-color photoassociation of a Bose-Einstein condensate, which results in Rabi oscillations between atomic and molecular condensates. We attain atom-molecule Rabi frequencies that are comparable to decoherence rates by driving photoassociation of atoms in an ^{88}Sr condensate to a weakly bound level of the metastable 1S0+3P1 molecular potential, which has a long lifetime and a large Franck-Condon overlap integral with the ground scattering state. Transient shifts and broadenings of the excitation spectrum are clearly seen at short times, and they create an asymmetric excitation profile that only displays Rabi oscillations for blue detuning from resonance.

DOI
10.1103/physrevlett.111.150402

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We demonstrate coherent one-color photoassociation of a Bose-Einstein condensate, which results in Rabi oscillations between atomic and molecular condensates. We attain atom-molecule Rabi frequencies that are comparable to decoherence rates by driving photoassociation of atoms in an ^{88}Sr condensate to a weakly bound level of the metastable 1S0+3P1 molecular potential, which has a long lifetime and a large Franck-Condon overlap integral with the ground scattering state. Transient shifts and broadenings of the excitation spectrum are clearly seen at short times, and they create an asymmetric excitation profile that only displays Rabi oscillations for blue detuning from resonance.
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)].
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.
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.
The dynamics of coherent Rabi oscillations in coupled atomic and molecular Bose-Einstein condensates is considered taking into account the atom-atom, atom-molecule, and molecule-molecule elastic interactions. The exact solution for the molecule formation probability is derived in terms of the elliptic functions. The two-dimensional space of the involved parameters intensity and detuning is analyzed and divided into two regions where the Rabi oscillations show different characteristics. A resonance curve is found, on which the molecular formation probability monotonically increases as a function of time. The maximum value of the final transition probability on this curve is 1∕21∕21∕2 (i.e., total transition to the molecular state) and it is achieved at high field intensities starting from a minimal threshold defined by the interspecies interaction scattering lights. The explicit form of the resonance curve is determined, and it is shown that the resonance frequency position reveals a nonlinear dependence on the Rabi frequency of the applied field. A singular point is found on the resonance curve, where a power-law time evolution of the system is observed.
We investigate the interaction of femtosecond laser pulses with an ensemble of ultracold rubidium atoms by applying shaped excitation pulses with two different types of spectral filtering. Although the pulses, which are frequency filtered with a high pass, have no spectral overlap with molecular states, we observe coherent molecular transients. Similar transients obtained with nearly transform-limited pulses, where only the atomic resonance is removed, reveal two differing oscillatory components. The resulting transients are compared among themselves and supported with quantum dynamical simulations which indicate a photoassociation process. The effect is due to the strong field interaction of the pulse with the colliding atom pair.