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Physical Review Letters

Photoassociation in Cold Atoms via Ladder Excitation

M. L. Trachy, G. Veshapidze, M. H. Shah, Hyounguk Jang, Brett D DePaola

Published Jul 25, 2007• 13 citations
Publisher

Abstract

We explore 2-color photoassociative ionization in cold Rb vapor and present experimental evidence that the molecular ions are produced from the stepwise excitation of a ladder of molecular states. We also explore a new process, dubbed photoassociative-dissociative ionization, by which atomic ions are created by excitation through a ladder of molecular states, finally autoionizing to a dissociative potential curve of Rb2+. We submit that these experiments could be the starting point for the same sort of high resolution spectroscopy that has already been done for lower electronic states of cold Rb2 at large internuclear separation.

DOI
10.1103/physrevlett.99.043003

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We explore 2-color photoassociative ionization in cold Rb vapor and present experimental evidence that the molecular ions are produced from the stepwise excitation of a ladder of molecular states. We also explore a new process, dubbed photoassociative-dissociative ionization, by which atomic ions are created by excitation through a ladder of molecular states, finally autoionizing to a dissociative potential curve of Rb2+. We submit that these experiments could be the starting point for the same sort of high resolution spectroscopy that has already been done for lower electronic states of cold Rb2 at large internuclear separation.
Many people in the science community are interested in the prospect of cold molecules for such applications as quantum computing and molecular Bose-Einstein condensates. Current methods of production fall short of the requirements for such projects. Photoassociation is a promising technique for forming cold molecules, but is currently facing significant obsta-cles. By understanding the photoassociation process and utilizing higher excited states, it is hoped that cold molecules can be formed from more easily produced cold atoms. Photoasso-ciative Ionization (PAI) is presented as a means to study excited state molecular dynamics at large internuclear separation, including photoassociation. This thesis presents a number of techniques for studying PAI in cold rubidium and a number of results obtained with the tech-niques. Excitation pathways for the process are explored in both narrow linewidth (MHz) and ultrafast (fs), large bandwidth (20 nm) domains.
In the molecular photoassociation process, two free cold atoms absorb one photon by a resonant way, to create an excited molecule in a well defined ro-vibrational state. The photoassociative spectroscopy of alkaline dimers yields accurate determinations for the long-range parts of molecular potential curves correlated to the first s + p asymptote. In contrast to atoms, laser cooling of molecules is very difficult because of the lack of a closed two-level scheme for recycling the population. The molecular photoassociation of cold atoms opens also a promising alternative for the formation of cold ground state molecules. Photoassociation of cold cesium atoms has permitted the first observation of translationally cold ground state molecules. The case of the cesium atom is very favorable because the 0 g - and 1 u purely long-range states below the dissociation limit 6s 1/2 +6p 3/2 present Condon points at intermediate distances. Such configurations offer rather efficient channels for the creation of singlet or triplet ground state Cs 2 molecules after spontaneous decay.
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.
We demonstrate a number of two-colour spectroscopy techniques where the first step is the photoassociation of laser-cooled and trapped sodium atoms to form bound states of . High-resolution spectra of are obtained. Spectra of the `purely long-range' state demonstrates the use of two-colour spectroscopy to open up an ionization channel for detecting the occurrence of photoassociation. The utility of photoassociation as a technique for producing cold molecular samples in a well defined rovibrational state is demonstrated with spectra showing and (Condon internal diffraction) transitions after the photoassociation. Starting from states in the and potentials, these transitions include upward transitions to autoionizing potentials dissociating near 3P + 3P and downward transitions back to the 3S + 3S ground-state potentials. Spectroscopic constants for six levels of a doubly excited state of are given.
We have produced ultracold polar RbCs molecules via photoassociation starting from laser-cooled 85 Rb and 133 Cs atoms in a dual-species, forced dark magneto-optical trap. The formed electronically excited RbCs* molecules correlated to the Rb(5S 1/2 ) + Cs(6P 1/2 ) dissociation limit are observed by trap loss spectroscopy. Following the decay of these excited RbCs* molecules, the formed ground state molecules are directly ionized by a two-photon single-color pulse dye laser, which is a new ionization mechanism for ground state RbCs molecules and thence detected by time-of-flight mass spectroscopy.
Abstract Molecular ions formed in cold hybrid ion-atom experiments may find interesting applications ranging from precision measurements to controlled chemical reactions. Here, we investigate electronic structure of the Sr2 + molecular ion, which may be produced by photoassociation of laser-cooled Sr+ ions immersed into an ultracold gas of Sr atoms or by ionization of ultracold Sr2 molecules. Using ab initio electronic structure methods, such as the coupled cluster and configuration interaction ones with small-core relativistic energy-consistent pseudopotentials and large Gaussian basis sets, we calculate potential energy curves for the ground and 41 excited electronic states, and electric dipole transition moments between them. We show that alkaline-earth molecular ions despite of their apparently simple structure with three valence electrons only are challenging for state-of-the-art quantum chemistry methods due to their multireference nature and high density of states. Finally, we calculate and analyze Franck-Condon factors governing the photoionization of ground-state Sr2 molecules into 2Σu + and 2Σg + states of Sr2 + molecular ions. The present results may be useful for studying and guiding formation and spectroscopy of cold Sr2 + molecular ions.