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Journal of Physics Conference Series

Lifetimes of ultralong-range strontium Rydberg molecules in cold dense gases

J. D. Whalen, F. Camargo, Roger Ding, T. C. Killian, F. B. Dunning, Jesús Pérez‐Ríos, S. Yoshida, Joachim Burgdörfer

Published Nov 1, 2017• 2 citations
Publisher

Abstract

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.

DOI
10.1088/1742-6596/875/2/012013

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We report the experimental measurements of the decay rate of polar cesium nD5/2 - 6S1/2 Rydberg-ground molecules with a large principal quantum number range of 35 ≤ n ≤ 40. Rydberg molecules are prepared employing the method of two-photon photoassociation and the molecular (atomic) ions, due to autoionization (blackbody photoionization), are detected with a microchannel plate detector. The decay rate Γ of the vibrational ground state of the deep and shadow bound molecules for triplet (TΣ) and mixed singlet-triplet (S,TΣ) are measured by fitting the molecular population with the exponential function. Comparing with the parent atom, the decay rate of the polar Rydberg-ground molecule shows an obvious increase with a magnitude of a few μs. The possible dissociation mechanism of polar Rydberg-ground molecules including a collisional decay, blackbody induced decay, and coupling of adjacent Rydberg states and tunneling decay are discussed in detail. The theoretical model is induced to simulate the measurements, showing agreement.

The Journal of Chemical Physics•Nov 15, 2023•2 citations
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.
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.
Long-range Rydberg molecules (LRMs) form when a highly excited Rydberg electron scatters from ground-state atoms inside its orbit, creating oscillatory, long-range potentials. We present a combined theoretical and experimental study of caesium dimers correlated to 402P3/2 Rydberg states, with an emphasis on decay via autoionisation (associative ionisation). Our model includes a relativistic treatment of electron-atom scattering with spin-orbit coupling, the perturber's hyperfine structure, and coupling of vibrational levels to a continuum of short-range decay channels. Calculated potential-energy curves predict two families of wells: outer wells near the classical outer turning point supporting long-lived states, and inner wells at shorter range whose lifetimes are limited by tunneling and subsequent vibronic decay. Using photoassociation in an ultracold Cs gas and an analysis of pulsed-field-ionisation signals which are highly selective for the detection of molecules, we assign resonances by binding energy and measure lifetimes. The measured lifetimes of inner-well states increase systematically with increasing detuning and agree with calculated lifetimes; detection of Cs2+ product ions supports autoionisation as a dominant channel. We show that the lifetimes are strongly reduced by spin-orbit interactions in the transient Cs-collision complex, which lift the near-degeneracy in Omega observed for states in the outer well and control the inner-well binding. The identified states also provide promising pathways to create ultracold molecules in ion-pair states.
Within a dense environment (ρ ≈ 10 14 atoms=cm 3 ) at ultracold temperatures (T < 1 μK), a single atom excited to a Rydberg state acts as a reaction center for surrounding neutral atoms.At these temperatures, almost all neutral atoms within the Rydberg orbit are bound to the Rydberg core and interact with the Rydberg atom.We have studied the reaction rate and products for nS 87 Rb Rydberg states, and we mainly observe a state change of the Rydberg electron to a high orbital angular momentum l, with the released energy being converted into kinetic energy of the Rydberg atom.Unexpectedly, the measurements show a threshold behavior at n ≈ 100 for the inelastic collision time leading to increased lifetimes of the Rydberg state independent of the densities investigated.Even at very high densities (ρ ≈ 4.8 × 10 14 cm -3 ), the lifetime of a Rydberg atom exceeds 10 μs at n > 140 compared to 1 μs at n ¼ 90.In addition, a second observed reaction mechanism, namely, Rb þ 2 molecule formation, was studied.Both reaction products are equally probable for n ¼ 40, but the fraction of Rb þ 2 created drops to below 10% for n ≥ 90.
We report the experimental measurements of the decay rate of polar cesium nD5/2 - 6S1/2 Rydberg-ground molecules with a large principal quantum number range of 35 ≤ n ≤ 40. Rydberg molecules are prepared employing the method of two-photon photoassociation and the molecular (atomic) ions, due to autoionization (blackbody photoionization), are detected with a microchannel plate detector. The decay rate Γ of the vibrational ground state of the deep and shadow bound molecules for triplet (TΣ) and mixed singlet-triplet (S,TΣ) are measured by fitting the molecular population with the exponential function. Comparing with the parent atom, the decay rate of the polar Rydberg-ground molecule shows an obvious increase with a magnitude of a few μs. The possible dissociation mechanism of polar Rydberg-ground molecules including a collisional decay, blackbody induced decay, and coupling of adjacent Rydberg states and tunneling decay are discussed in detail. The theoretical model is induced to simulate the measurements, showing agreement.