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Optics and Spectroscopy

Excited-state collisional relaxation by optical orientation of atoms with arbitrary electronic angular momentum

A. I. Okunevich

Published Mar 1, 1981• 0 citations
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Atom-ion interactions occur through the electric dipole which is induced by the ion on the neutral atom. In a Langevin collision, in which the atom and ion overcome the centrifugal barrier and reach a short internuclear distance, their internal electronic states deform due to their interaction and can eventually alter. Here we explore the outcome products and the energy released from a single Langevin collision between a single cold 88^{88}88Sr+^{+}+ ion initialized in the metastable 4d2D5/2,3/24d^2D_{5/2,3/2}4d2D5/2,3/2​ states, and a cold 87^{87}87Rb atom in the 5s2S1/25s^2S_{1/2}5s2S1/2​ ground state. We found that the long-lived D5/2D_{5/2}D5/2​ and D3/2D_{3/2}D3/2​ states quench after roughly three Langevin collisions, transforming the excitation energy into kinetic energy. We identify two types of collisional quenching. One is an Electronic Excitation-Exchange process, during which the ion relaxes to the SSS state and the atom is excited to the PPP state, followed by energy release of ∼\sim∼ 3000 K⋅\cdot⋅kB_BB​. The second is Spin-Orbit Change where the ion relaxes from the higher fine-structure D5/2D_{5/2}D5/2​ level to the lower D3/2D_{3/2}D3/2​ level releasing ∼\sim∼ 400 K⋅\cdot⋅kB_BB​ into kinetic motion. These processes are theoretically understood to occur through Landau-Zener avoided crossings between the different molecular potential curves. We also found that these relaxation rates are insensitive to the mutual spin orientation of the ion and atoms. This is explained by the strong inertial Coriolis coupling present in ultracold atom-ion collisions due to the high partial wave involved, which strongly mixes different angular momentum states. This inertial coupling explains the loss of the total electronic angular-momentum which is transferred to the external rotation of nuclei. Our results provide deeper understanding of ultracold atom-ion inelastic collisions and offer additional quantum control tools for the cold chemistry field.