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Physical Review A

Observation of the pure long-range 1u state of an alkali-metal dimer by photoassociative spectroscopy

Xiaotian Wang, He Wang, P. L. Gould, William C. Stwalley, Eite Tiesinga, Paul S. Julienne

Published Jun 1, 1998• 22 citations
Publisher

Abstract

The pure long-range ${1}_{u}$ state of an alkali-metal dimer is observed in ${}^{39}{\mathrm{K}}_{2}$ using photoassociative spectroscopy of ultracold atoms. High-resolution spectra for vibrational levels $v=\stackrel{\ensuremath{\rightarrow}}{0}7$ are recorded by resonance-enhanced two-photon ionization. Strong rotation-hyperfine couplings are observed. Major molecular constants and a hyperfine structure analysis are presented. This ${1}_{u}$ state is useful as an ungerade Franck-Condon ``window'' at large internuclear distance for studies of highly excited long-range interactions.

DOI
10.1103/physreva.57.4600

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•Jan 1, 1998•0 citations
The pure long-range 1u{1}_{u}1u​ state of an alkali-metal dimer is observed in 39K2{}^{39}{\mathrm{K}}_{2}39K2​ using photoassociative spectroscopy of ultracold atoms. High-resolution spectra for vibrational levels v=0\ensuremath→7v=\stackrel{\ensuremath{\rightarrow}}{0}7v=0\ensuremath→​7 are recorded by resonance-enhanced two-photon ionization. Strong rotation-hyperfine couplings are observed. Major molecular constants and a hyperfine structure analysis are presented. This 1u{1}_{u}1u​ state is useful as an ungerade Franck-Condon ``window'' at large internuclear distance for studies of highly excited long-range interactions.
We have examined and identified the excited long-range Hund’s case (c) molecular states of the ten heteronuclear alkali metal diatomic molecules which support bound states and can be probed by ultracold photoassociative spectroscopy. Analytical expressions for the heteronuclear long-range free-bound Franck–Condon factors as a function of the internuclear distance R and the vibrational quantum number v are derived and discussed. The KRb system has considerably stronger excited long-range interactions than any other heteronuclear alkali diatomic molecule and has very favorable Franck–Condon factors for the photoassociation process. The heteronuclear photoassociative spectroscopy will provide spectroscopic measurements of the binary elastic scattering lengths of heteronuclear cold collisions which are the crucial parameters for sympathetic cooling of mixed atomic gases.
The photoassociation of colliding ultracold trapped atoms permits the observation of high resolution molecular spectra of high lying vibrational levels with low total angular momentum and outer turning points greater than 50 Å. This paper describes how the hyperfine structure of alkali dimer molecules at large internuclear separation can be used to assign the electronic character of the observed photoassociation spectra and how hyperfine structure helps to explain the observed photoassociation spectrum of the attractive electronic states of the Na2 molecule that correlate with Na(3 2S)+Na(3 2P3/2) atoms.
We report the first observation of optical-optical double resonance photoassociative spectroscopy of ultracold 39{}^{39}39K atoms near the highly excited 39K(4s)+39K(4d,5d,6d,6s,7s)^{39}K(4s)+^{39}K(4d,5d,6d,6s,7s)39K(4s)+39K(4d,5d,6d,6s,7s) asymptotes in a high density magneto-optical trap. Using the ${v}^{\ensuremath{'}}\phantom{\rule{0ex}{0ex}}=\phantom{\rule{0ex}{0ex}}0$ level of the ${0}_{g}^{\ensuremath{-}}$ ``pure long-range'' state (a localized long-range Franck-Condon window) as the intermediate state, we observe simple and assignable rovibrational progressions dissociating to these asymptotes. The dominant long-range potential constants are determined. Line broadening, presumably due to autoionization, and rotational excitations due to strong field effects are observed.
We report a full theoretical calculation of the rovibrational structure of the ${\mathrm{Na}}_{2} {0}_{g}^{\ensuremath{-}}$ state, including hyperfine structure. The purely long-range ${0}_{g}^{\ensuremath{-}}$ state has been observed in the photoassociation spectroscopy of ultracold trapped alkali-metal atoms. For the lighter alkali-metal atoms (Li, Na, and K), the purely long-range states are completely characterized by atomic data since the inner turning point of the potentials are at internuclear separations where exchange interactions are still negligible.
Understanding high-precision photoassociative spectroscopy of laser-cooled alkali-metal atoms involves modeling an extremely dense level structure of weakly bound molecules in the region where coriolis and hyperfine interactions become comparable to electronic interactions. We describe an iterative eigenvalue solver suitable for resolving these bound states that is based on finding eigenvalues of the shifted inverse or Green-function operator. Nonlinear coordinate transformations applied to the nuclear motion are introduced to minimize the dimensionality of the discretized Hamiltonian. The formalism is applied to resolve the hyperfine structure of rovibrational levels of the Na(2P)+Na(2S)\mathrm{Na}{(}^{2}P)+\mathrm{Na}{(}^{2}S)Na(2P)+Na(2S) dimer.
The field of laser cooling and trapping of atoms has had a profound impact on many areas of atomic, molecular and optical science. In particular, ultracold atoms colliding in magneto-optical traps typically have relative kinetic energies of 300muK(sim7MHz)300\\mu K (\\sim 7 MHz)300muK(sim7MHz), so free-bound absorption lines are as sharp as bound-bound lines. Moreover, because of very long range centrifugal barriers, only a few collisional partial waves are important (Jprimeprime=0,1J^{\\prime\\prime} = 0, 1Jprimeprime=0,1 and 2 in our work on 39K^{39}K39K). Such photoassociative free-bound absorption allows observation of ``pure long-range molecule'' states (Re=28R_{e} = 28Re​=28 and 39 {\\AA} in 39K2^{39}K_{2}39K2​) as well as long-range levels of known short range states with outer classical turning points of sim20−250AA\\sim 20 - 250 {\\AA}sim20−250AA. Such spectra have been observed by ``trap loss'' (decrease in atomic fluorescence), molecular ionization, and fragment ionization. Optical-optical double resonance (OODR), e.g. through the ``Franck-Condon windows'' of the ``pure long-range'' states, produces readily assignable spectra at higher asymptotes as well. Further extensions of ultracold photoassociative spectroscopy and applications to determination of long range potentials, atomic properties, and Bose-Einstein condensate stability will be presented.