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Europhysics Letters (EPL)

Measurement of the atomic Na(3 P ) lifetime and of retardation in the interaction between two atoms bound in a molecule

K. M. Jones, Paul S. Julienne, Paul D. Lett, William D. Phillips, Eite Tiesinga, Carl J. Williams

Published Jul 10, 1996• 122 citations
Publisher

Abstract

From molecular spectroscopy of the Na 2 purely long-range 0 − g state we determine the Na(3 P ) lifetime and measure the predicted but previously unobserved effect of retardation in the interaction between two atoms. Our lifetime τ( P 3/2 ) = 16.230(16) ns helps to remove a longstanding discrepancy between experiment and theory. Electron cloud overlap is unimportant in the 0 − g state ( R > 55 a 0 ) and the spectrum is calculated, ab initio , from atomic properties. By measuring the binding energies the 120 MHz correction due to retardation of the resonant-dipole R −3 interaction is confirmed.

DOI
10.1209/epl/i1996-00536-9

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From molecular spectroscopy of the Na 2 purely long-range 0 − g state we determine the Na(3 P ) lifetime and measure the predicted but previously unobserved effect of retardation in the interaction between two atoms. Our lifetime τ( P 3/2 ) = 16.230(16) ns helps to remove a longstanding discrepancy between experiment and theory. Electron cloud overlap is unimportant in the 0 − g state ( R > 55 a 0 ) and the spectrum is calculated, ab initio , from atomic properties. By measuring the binding energies the 120 MHz correction due to retardation of the resonant-dipole R −3 interaction is confirmed.
We report resolution of the 1% discrepancy between theory and experiment for the lifetime of the first excited state of Na. Determining the atomic lifetime by a novel method, we have measured the natural linewidth of the $3{}^{2}{S}_{1/2}\ensuremath{\rightarrow}3{}^{2}{P}_{3/2}$ transition with <0.25<0.25%<0.25 accuracy through precision spectroscopy on an optically prepared sample of ultracold, two-level atoms. The resulting 32P3/23{}^{2}{P}_{3/2}32P3/2​ lifetime of 16.237(35) ns disagrees with previous time-domain measurements but is in good agreement with recent calculations and a new fast beam result.
We observe the formation of long-range Cs2 Rydberg molecules consisting of a Rydberg and a ground-state atom by photoassociation spectroscopy in an ultracold Cs gas near 6s1/2(F=3,4)→np3/2 resonances (n=26-34). The spectra reveal two types of molecular states recently predicted by D. A. Anderson, S. A. Miller, and G. Raithel [Phys. Rev. A 90, 062518 (2014)]: states bound purely by triplet s-wave scattering with binding energies ranging from 400 MHz at n=26 to 80 MHz at n=34, and states bound by mixed singlet-triplet s-wave scattering with smaller and F-dependent binding energies. The experimental observations are accounted for by an effective Hamiltonian including s-wave scattering pseudopotentials, the hyperfine interaction of the ground-state atom, and the spin-orbit interaction of the Rydberg atom. The analysis enables the characterization of the role of singlet scattering in the formation of long-range Rydberg molecules and the determination of an effective singlet s-wave scattering length for low-energy-electron-Cs collisions.
In this work the existence of a novel type of molecule is shown whose binding is based solely on electron-atom scattering. These molecules are composed of a Rydberg atom and a ground state atom - here Rb(ns) and Rb(5s) - where the binding arises from scattering of the Rydberg electron from the ground state atom. The ground state atom is bound to the Rydberg wavefunction, which has radii on the order of 100nm, and thus these molecules are of long-range. Although the theoretical description of this interaction goes back to the famous work of Fermi in the year 1934 which was expanded in the following decades by Omont and Greene, the experimental proof of their existence was still missing. Up to now, experimental evidence for the ultralong-range Rydberg molecules was found only in spectral line broadenings. The present experiments have demonstrated the direct photoassociation of these ultralong-range Rydberg molecules for Rb(ns)-Rb(5s) triplet states from a cold and dense sample of rubidium 87 atoms for a range of principal quantum numbers, n, between 34 and 40. The high-resolution photoassociation spectra allowed for the observation of several vibrational states separated by only a few Megahertz. Based on the model by Greene the vibrational ground states v=0 are assigned and the dependence of their binding energy on the principal quantum number, n, is used to extract the triplet s-wave scattering length for electron-Rb(5s) collisions from the data. The remarkably good agreement between experiment and theory for the vibrational ground state v=0 over a range of principal quantum numbers attests to the accuracy of Fermi's original pseudopotential approach in describing interactions in excited multi-atom systems. Aside from this good agreement for the state v=0, the measurements also show that contributions from p-wave scattering cannot be neglected, as a number of excited vibrational states is observed in the experiment that are not predicted from the theory assuming only s-wave scattering. Calculations of Li, Pohl and coworkers have shown that a full solution of the electron-atom scattering is necessary for the assignment of all vibrational states. This work finds the molecular bound states to be very sensitive to both s-wave as well as p-wave electron-atom scattering and the Rydberg molecules turn out to be an accurate experimental platform to study electron-atom collisions in a previously inaccessible ultralow-energy regime. In general, the ultralong-range Rydberg molecules investigated here for rubidium are expected for all species with negative scattering length for electron-atom interaction, e. g. the other alkali atoms. Rydberg atom and ground state atom do not even have to be of the same chemical element, the only requirement is a negative scattering length of the ground state atom for electron scattering. Moreover, the binding force of the Rydberg electron is not restricted to a single ground state atom and molecules with more than one ground state atom can be created. The fact that these exotic molecules have huge bond lengths but nevertheless a vibrational spectrum with several states make a new type of ultracold Rydberg chemistry feasible. In the future, larger polymers or even heteronuclear molecules can be realized, where the number of atoms, the constituent atomic elements and the addressed Rydberg state allow to precisely select the properties of the long-range molecule.
We review the information on the interactions between cold ground-state Na atoms following from Na2{\mathrm{Na}}_{2}Na2​ bound states, a Na photoassociation experiment, and a recent observation of field-induced Feshbach resonances in a Na Bose condensate. We obtain a set of Na interaction parameters that is in excellent agreement with all these experimental data. The existing discrepancy between different values for the scattering length ${a}_{1,\ensuremath{-}1}$ of Na atoms in the $|1,\ensuremath{-}1〉$ hyperfine state is resolved. The present interaction parameters enable us to give accurate predictions for the singlet and triplet scattering lengths aS{a}_{S}aS​ and aT,{a}_{T},aT​, ${a}_{1,\ensuremath{-}1},$ scattering lengths for collisions between Na atoms in other hyperfine states, and resonance fields of several yet unobserved Feshbach resonances. We find ${a}_{S}=(19.1\ifmmode\pm\else\textpm\fi{}{2.1)a}_{0},{a}_{T}=(65.3\ifmmode\pm\else\textpm\fi{}{0.9)a}_{0},$ and ${a}_{1,\ensuremath{-}1}(B=0)=(55.4\ifmmode\pm\else\textpm\fi{}{1.2)a}_{0}.$
Calculations of the adiabatic potential energy curves and the transition dipole moments between the ground (A 1 Σ + ) and the first excited (A 1 Σ + ) states have been determined for the LiCs and NaCs molecules. The calculations are performed using an ab initio approach based on non-empirical pseudopotentials for Cs + , Li + and Na + cores, parameterized l -dependent polarization potentials and full configuration interaction calculations. The potential energy curves and the transition dipole moment are used to estimate the radiative lifetimes of the vibrational levels of the A + Σ + state using the Franck–Condon (FC) approximation and the approximate sum rule method. The radiative lifetimes associated with the A + Σ + state are presented here for the first time. These data can help experimentalists to optimize photoassociative formation of ultracold molecules and their longevity in a trap or in an optical lattice.