Abstract

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 point-like 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 photo-association 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.

Highlights

  • Ultralong-range Rydberg molecules (ULRM) [1,2] have become an active field of research ever since they were first predicted [3,4] and experimentally observed [5,6]

  • We present potential energy curves (PECs) that are asymptotically connected with Rydberg nP or nD states of rubidium or cesium

  • The second type of ULRM is formed by a pair of atoms that are both excited to Rydberg states, often referred to as Rydberg macrodimers [4,6,26]

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Summary

INTRODUCTION

Ultralong-range Rydberg molecules (ULRM) [1,2] have become an active field of research ever since they were first predicted [3,4] and experimentally observed [5,6]. The second type of ULRM is formed by a pair of atoms that are both excited to Rydberg states, often referred to as Rydberg macrodimers [4,6,26] In this case, the binding mechanism arises from the multipolar electrostatic interaction between the two atoms as has been studied in numerous theoretical works [27,28,29,30,31]. While RAIMs exist over a wider range of n, here we show results for Rb and Cs RAIMs with Rydberg levels between n = 45 and 55, because these levels are laser-excitable and their ionization electric fields [61], ∼50 V/cm, are low enough for convenient RAIM detection Their RAIM bonding lengths and vibrational frequencies are conducive to experimental study.

Hamiltonian and potential energy curves
Weak optical coupling
Strong optical coupling
Determination of lmax
Comparison of Rb and Cs
Vibrational states
Collisions on Rydberg-atom-ion PECs
EXPERIMENTAL CONSIDERATIONS
Laser spectroscopy with narrow-band lasers
Vibrational wave packets
CONCLUSION
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