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Physical Review A

Approach to form long-range ion-pair molecules in an ultracold Rb gas

Adam Kirrander, Seth T. Rittenhouse, Marco Ascoli, Edward E. Eyler, P. L. Gould, H. R. Sadeghpour

Published Mar 22, 2013• 20 citations
Publisher

Abstract

We propose a realizable and efficient approach for exciting long-range ion-pair molecules, known as heavy Rydberg states, in an ultracold ${}^{85}$Rb 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.

DOI
10.1103/physreva.87.031402

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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.
Abstract We propose a scheme to realize a heavy Rydberg system (HRS), a bound pair of oppositely charged ions, from a gas of ultracold atoms. The intermediate step to achieve large internuclear separations is the creation of a unique class of ultra-long-range Rydberg molecules bound in a stairwell potential energy curve. Here, a ground-state atom is bound to a Rydberg atom in an oscillatory potential emerging due to attractive singlet p-wave electron scattering. The utility of our approach originates in the large electronic dipole transition element between the Rydberg and the ionic molecule, while the nuclear configuration of the ultracold gas is preserved. The Rabi coupling between the Rydberg molecule and the heavy Rydberg system is typically in the MHz range and the permanent electric dipole moments of the HRS can be as large as one kilo-Debye. We identify specific transitions which place the creation of the heavy Rydberg system within immediate reach of experimental realization.
Thermal collisions between potassium Rydberg atoms with intermediate values of quantum number n and target molecules that capture free low-energy electrons are investigated. The velocity, binding energy, and angular distributions of heavy-Rydberg ion-pair states formed through such collisions are measured. The experimental data are analyzed with the aid of semiclassical Monte Carlo simulations to investigate the dynamics of electron attachment to a variety of target species. Multiple reaction channels involving short- and long-lived intermediates are seen for electron capture by 1,1,1-C2Cl3F3 and CBrCl3 (where dissociation of CBrCl3 intermediates involves production of Br- and Cl- ions). Electron attachment to BrCN produces long-lived BrCN-* intermediates whose dissociation results in the creation of rotationally-hot CN- anions. Electron capture by Fe(CO)5 leads to formation of Fe(CO)5-* intermediates which can fragment producing Fe(CO)4- anions, either directly or after partial redistribution of the excess energy within the intermediate has occurred. Electron transfer in Rydberg atom collisions with C2Cl4 provide no evidence of formation of long-lived C2Cl4 ions, only Cl- ions are seen. Moreover, strong Rydberg atom scattering is observed following collisions of K(12p) Rydberg states with CH3NO2. This finding is consistent with a theory which predicts that collisions between Rydberg atoms with intermediate values of n and polar molecules can lead to strong resonant quenching of Rydberg states, i.e., n and l changing, through formation of short-lived K+...CH3NO2- ion-pair states. Finally, the improvements in sensitivity to electron capture reaction dynamics that might be achieved using different Rydberg species and a crossed molecular beam are examined. Simulations are performed to demonstrate that the use of a hyperthermal helium Rydberg atomic beam and a crossed beam of target molecules such as CCl4, BrCN and CF3I can provide new insights into dissociative electron attachment reactions. The calculations show that not only can much detailed information on translational energy release distributions and intermediate lifetimes be obtained, but also on the electron radial probability density distributions in the Rydberg atoms themselves.
Abstract We propose an experimentally realizable scheme to produce triatomic ultralong-range Rydberg molecules (TURM), formed in ultracold KRb traps. A near resonant coupling of the non-zero quantum defect Rydberg levels with the KRb molecule in N = 0 and N = 2 rotational levels, is engineered which exploits the unique Rydberg electron–molecule anisotropic dipole interaction. This near resonant coupling enhances the TURM binding and produces favorable Franck–Condon factors. Schemes for both postassium and rubidium excitations are demonstrated.
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.
Summary form only given. The discovery of ultracold and dilute ensembles of atoms and molecules in magneto-optical traps (MOT) and in atomic Bose-Einstein condensates (BECs) has ushered in a new era of precision atomic and molecular spectroscopy. Since the atoms in such cold environments predominantly interact via long-range forces, the creation of BECs and dilute atomic samples has made the study of very long-range molecular states possible. In this work (Greene et al, Phys. Rev. Lett. vol. 85, p. 2458, 2000), we discuss a particular interatomic arrangement that should be favored in modern-day MOT and BEC setups and should result in the production of molecular Rydberg states whose vibrational wave functions are localized at internuclear distances of order n/sup 2/ Bohr radii, where n is the principal quantum number. The vibrational binding energies of these molecules for n=20-50 fall in the MHz and GHz range, for molecules excited from /sup 87/Rb ultracold atomic gas. We predict two distinct classes of molecular Rydberg states. The nonpolar class of Rydberg molecules form from the interaction between a Rb(nl/sub j/) Rydberg atom with low orbital angular momentum l/sub j//spl les/2 and a distant Rb ground state atom. Rydberg molecules of the second class form from the interaction between an excited Rb atom in high (l/sub j/>2) orbital angular momentum states with a ground state Rb atom.
Abstract In excited molecules, the interaction between the covalent Rydberg and ion-pair channels forms a unique class of excited states, in which the infinite manifold of vibrational levels are the equivalent of atomic Rydberg states with a heavy electron mass. Production of the ion-pair states usually requires excitation through one or several interacting Rydberg states; these interacting channels lead to loss of flux, diminishing the rate of ion-pair production. Here, we develop an analytical, asymptotic charge-transfer model for the interaction between ultracold Rydberg molecular states, and employ this method to demonstrate the utility of off-resonant field control over the ion-pair formation, with near unity efficiency.