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arXiv:1511.06793 · Physical Review A

Lifetimes of ultra-long-range strontium Rydberg molecules

F. Camargo, J. D. Whalen, Roger Ding, H. R. Sadeghpour, S. Yoshida, Joachim Burgdörfer, F. B. Dunning, T. C. Killian

Published Feb 4, 2016• 44 citations
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Abstract

The lifetime of ultra-long-range strontium Rydberg molecules is measured in the low-lying vibrational states, where its resemblance to the lifetime of the parent Rydberg atoms demonstrates that a $p$-wave resonance, which is absent in the present case but prevalent in Rydberg molecules comprised of alkali-metal atoms, plays an important role in determining the lifetime of such molecules.

DOI
10.1103/physreva.93.022702

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Journal of Physics Conference Series•Sep 7, 2015•1 citation
The lifetime of ultra-long-range strontium Rydberg molecules is measured in the low-lying vibrational states, where its resemblance to the lifetime of the parent Rydberg atoms demonstrates that a ppp-wave resonance, which is absent in the present case but prevalent in Rydberg molecules comprised of alkali-metal atoms, plays an important role in determining the lifetime of such molecules.
In this work I describe the excitation spectra of Rydberg atoms in ultracold gases of strontium and their decay mechanisms. In a few-body regime, we observe a highly structured spectrum re ecting excitation of ultralong-range molecules consisting of one or more ground-state atoms bound to the Rydberg core in potential wells formed by the Rydbergelectron wave function. In a many-body regime, with hundreds of ground-state atoms within the Rydberg orbital, the Rydberg atoms can be viewed as an impurity in a quantum gas, connecting to important concepts in condensed matter physics. The spectrum for impurity excitation displays signatures of polaronic states, in which the Rydberg atom signi cantly perturbs the density of the background gas. Additionally, decay channels of Rydberg excitations are examined by monitoring the time evolution of Rydberg populations. The measured lifetimes reveal new information on the decay processes of Rydberg molecules and place limits on the time scales over which studies involving Rydberg species in cold, dense atomic gases can be undertaken and limit the coherence times for such measurements.
The lifetimes and decay channels of ultralong-range Rydberg molecules created in a dense Bose-Einstein condensate (BEC) are examined by monitoring the time evolution of the Rydberg population using field ionization. The Rydberg molecules, which contain tens to hundreds of ground state atoms within the electron orbit, have lifetimes of ∼ 1 to 5 µ s, their destruction being attributed to two main processes: formation of ions through associative ionization, and dissociation induced through L -changing reactions. The observed loss rates are consistent with a reaction model that emphasizes the interaction between the Rydberg core ion and its nearest neighbor ground state atom. The application of this model to earlier measurements of strontium dimer lifetimes at lower densities is discussed.
The lifetimes and decay channels of ultralong-range Rydberg molecules created in a dense Bose-Einstein condensate are examined by monitoring the time evolution of the Rydberg population using field ionization. Studies of molecules with values of the principal quantum number, nnn, in the range n=49n=49n=49 to n=72n=72n=72 that contain tens to hundreds of ground-state atoms within the Rydberg electron orbit show that their presence leads to marked changes in the field ionization characteristics. The Rydberg molecules have lifetimes of $\ensuremath{\sim}1\ensuremath{-}5\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}\mathrm{s}$, their destruction being attributed to two main processes: formation of Sr2+{\mathrm{Sr}}_{2}{}^{+}Sr2​+ ions through associative ionization and dissociation induced through LLL-changing collisions. The observed loss rates are consistent with a reaction model that emphasizes the interaction between the Rydberg core ion and its nearest-neighbor ground-state atom. The measured lifetimes place strict limits on the time scales over which studies involving Rydberg species in cold, dense atomic gases can be undertaken and limit the coherence times for such measurements.
Spectroscopy of ⁸⁷Sr Rydberg Atoms and Molecules This dissertation describes the development of an apparatus to undertake spectroscopic studies of ⁸⁷Sr Rydberg states and their application in the production of ultra-long-range Rydberg molecules (ULRRMs). Most previous spectroscopic studies of strontium have been performed with the bosonic isotope ⁸⁸Sr which has no nuclear spin (I=0), resulting in a relatively simple and well-understood Rydberg excitation spectrum. In contrast, fermionic ⁸⁷Sr has a large nuclear spin (I=9/2) that leads to strong hyperfine interactions which greatly complicate the Rydberg excitation spectrum. In order to understand the Rydberg states in ⁸⁷Sr, two-photon spectroscopy was performed to measure and identify the (5sns)³S and (5snd)³D hyperfine Rydberg states for 30≲n≲99. Working with theory collaborators, a detailed understanding of how the hyperfine interaction affects the Rydberg levels is developed and used to extract revised quantum defects. The detailed understanding of the ⁸⁷Sr hyperfine Rydberg structure was exploited to produce the first ULRRMs in a fermionic gas. Unlike traditional molecular binding mechanisms, ULRRMs comprise of one or more ground-state atoms embedded in the electron cloud of a Rydberg atom with the entire system bound together through the weak Rydberg electron-neutral atom scattering. Therefore, production of ULRRMs is dependent on both the principal quantum number (n) of the parent Rydberg atom and the initial spatial distribution of atoms. At low temperatures, the effects of quantum statistics becomes important and result in bunching (bosons) and antibunching (fermions). These differences in spatial distributions can influence the excitation rates of ULRRMs. Current progress in exploring the role of quantum statistics in the excitation of ULRRMs using cold, dense strontium gases is described, with an emphasis on ⁸⁷Sr, and how such measurements can be used to extract the pair correlation function g⁽²⁾(R).