Abstract
We propose a new approach to excite ion-pair states of ultracold dimers. The central idea is a two-step process where first long-range Rydberg molecules are formed by photoassociation, which are then driven by stimulated emission towards the ion-pair state, a process bearing features of a photo-induced harpooning reaction. We assess the feasibility of this approach through a detailed experimental and theoretical study on a specific system, p-wave-scattering dominated long-range Rydberg molecules in caesium, and discuss potential applications for the study of strongly correlated plasmas consisting of oppositely charged particles of equal or similar mass.
Highlights
In recent years, a solid understanding of the properties of long-range Rydberg molecules has been established and the developed theoretical tools explain experimental observations reliably, often even quantitatively [1, 2]
We assess the feasibility of this approach through a detailed experimental and theoretical study on a specific system, p-wave-scattering dominated long-range Rydberg molecules in caesium, and discuss potential applications for the study of strongly correlated plasmas consisting of oppositely charged particles of equal or similar mass
In this article we have presented a novel route to excite heavyRydberg states with high values of nHR via photoassociation of long-range Rydberg molecules and stimulated emission into the ion-pair state
Summary
A solid understanding of the properties of long-range Rydberg molecules has been established and the developed theoretical tools explain experimental observations reliably, often even quantitatively [1, 2]. We will separately discuss the following steps: (i) photoassociation of a pair of colliding atoms into metastable long-range Rydberg molecules with an electronic character that has significant contributions from 1P1 scattering and (ii) driving stimulated emission from the longrange Rydberg to the ion-pair state. This photoinduced charge-transfer process bears features of a harpoon reaction, where the Rydberg atom captures the ground-state atom by donating its electron to the neutral and a more strongly bound ion pair is formed. Much shorter internuclear distances than considered here, where covalent and ionic molecular states are strongly mixed [16, 17]
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