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arXiv:2001.11754 · Journal of Physics B Atomic Molecular and Optical Physics

Formation of ultracold ion pairs through long-range Rydberg molecules

Michael Peper, Johannes Deiglmayr

Published Feb 14, 2020• 15 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/1361-6455/ab63ac

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We propose a realizable and efficient approach for exciting long-range ion-pair molecules, known as heavy Rydberg states, in an ultracold 85{}^{85}85Rb gas via Feshbach resonances. Heavy Rydberg states, the molecular analogs of electronic Rydberg states, with the electron replaced by an atomic anion, offer opportunities for novel physics, including the formation of ultracold anions and strongly coupled plasmas. We map the positions, lifetimes, and Franck-Condon factors of heavy Rydberg resonances across a wide range of excitation energies, and we calculate the rates of formation for the most promising transitions through long-lived intermediate interferometric resonances.
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In a combined experimental and theoretical effort we report on two novel types of ultracold long-range Rydberg molecules. First, we demonstrate the creation of triatomic molecules of one Rydberg atom and two ground-state atoms in a single-step photoassociation. Second, we assign a series of excited dimer states that are bound by a so far unexplored mechanism based on internal quantum reflection at a steep potential drop. The properties of the Rydberg molecules identified in this work qualify them as prototypes for a new type of chemistry at ultracold temperatures.
We propose a novel type of Rydberg dimer, consisting of a Rydberg-state atom bound to a distant positive ion.The molecule is formed through long-range electric-multipole interaction between the Rydberg atom and the pointlike ion.We present potential energy curves (PECs) that are asymptotically connected with Rydberg nP or nD states of rubidium or cesium.The PECs exhibit deep, long-range wells which support many vibrational states of Rydberg-atom-ion molecules (RAIMs).We consider photoassociation of RAIMs in both the weak and the strong optical-coupling regimes between initial and Rydberg states of the neutral atom.Experimental considerations for the realization of RAIMs are discussed.
We present a mechanism contributing to the detection of photoassociated long-range Rydberg molecules via pulsed-field ionization: ionic products, created by the decay of a long-range Rydberg molecule, modify the excitation spectrum of surrounding ground-state atoms and facilitate the excitation of further atoms into Rydberg states by the photoassociation light. Such an ion-mediated excitation mechanism has been previously called a Coulomb antiblockade. Pulsed-field ionization typically does not discriminate between the ionization of a long-range Rydberg molecule and an isolated Rydberg atom, and thus the number of atomic ions detected by this mechanism is not proportional to the number of long-range Rydberg molecules present in the probe volume. By combining high-resolution UV and rf spectroscopy of a dense, ultracold gas of cesium atoms, theoretical modeling of the molecular-level structures of long-range Rydberg molecules bound below n2P3/2n\phantom{\rule{0.16em}{0ex}}^{2}P_{3/2}n2P3/2​ Rydberg states of cesium, and a rate model of the photoassociation and decay processes, we unambiguously identify the signatures of this detection mechanism in the photoassociation of long-range Rydberg molecules bound below atomic asymptotes with negative Stark shifts.