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Bulletin of the American Physical Society

The role of electronic excitation in ultracold atom-ion chemistry

Scott T. Sullivan, Wade G. Rellergert, Svetlana Kotochigova, Eric R. Hudson

Published Jun 8, 2012• 1 citation
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The role of electronic excitation in inelastic collisions between ultracold Ca atoms and Ba(+) ions, confined in a hybrid trap, is studied for the first time. Unlike previous investigations, this system is energetically precluded from undergoing inelastic collisions in its ground state, allowing a relatively simple experimental determination and interpretation of the influence of electronic excitation. It is found that while the electronic state of the ion can critically influence the inelastic collision rate, the polarizability mismatch of the neutral atom electronic states suppresses short-range collisions, and thus inelastic processes, involving electronically excited neutral atoms. As a result of these features, it is experimentally demonstrated that it is possible to mitigate inelastic collision loss mechanisms in these systems, marking an important step toward long-lived hybrid atom-ion devices.
Ultracold atom-ion collisions are an emerging field of research that can ultimately lead to their precise quantum control. In collisions in which the ion is prepared in an excited state, previous studies showed that the dominant reaction pathway was charge exchange. Here, we explored the outcome products and the energy released from a single ultracold collision between a single 88Sr+^{88}\mathrm{Sr}^{+}88Sr+ ion and a single 87Rb^{87}\mathrm{Rb}87Rb atom prepared in excited metastable and ground electronic states, respectively, with control over their relative spins. We found that the ion's long-lived D5/2{D}_{5/2}D5/2​ and D3/2{D}_{3/2}D3/2​ states quench after roughly three collisions, acquiring immense kinetic energy in the process. By performing single-shot thermometry on the ion after the collision, we identified two dominant reaction pathways: electronic excitation exchange and spin-orbit change. In contrast to previous experiments, we observed no charge-exchange events. These processes are theoretically understood to occur through Landau-Zener avoided crossings leading to the observed reaction pathways. We also found that spin orientation has almost no effect on the reaction pathways, due to strong Coriolis-spin mixing. Our results provide a deeper understanding of ultracold atom-ion inelastic collisions and offer additional quantum control tools for the cold chemistry field.