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Journal of Physics Conference Series

Photoassociation spectroscopy of purely long-range krypton molecules

Z. S. Smith, J Banister, R Norman, K Hoogeboom, M. Walhout

Published Nov 1, 2009• 0 citations
Publisher

Abstract

Photoassociation spectra for purely long-range (PLR) krypton molecules are both computed and measured. The photoassociation laser is tuned just red of the 5s[3/2]2-5p[5/2]2 transition at 810.6 nm, over a frequency range in which fourteen different PLR potential wells support hundreds of vibrational bound states. In the experiment, laser light is directed into a cloud of magneto-optically trapped 84Kr atoms, and the emission of both ultraviolet photons and ions is monitored. Peaks in these signals are observed for laser frequencies within 200 MHz of the atomic resonance. Ongoing work is aimed at improving the experimental signal and understanding the degree of agreement between empirical data and computed molecular spectra.

DOI
10.1088/1742-6596/194/12/122009

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Journal of the Optical Society of America B•Oct 18, 2016•0 citations
Photoassociation spectra for purely long-range (PLR) krypton molecules are both computed and measured. The photoassociation laser is tuned just red of the 5s[3/2]2-5p[5/2]2 transition at 810.6 nm, over a frequency range in which fourteen different PLR potential wells support hundreds of vibrational bound states. In the experiment, laser light is directed into a cloud of magneto-optically trapped 84Kr atoms, and the emission of both ultraviolet photons and ions is monitored. Peaks in these signals are observed for laser frequencies within 200 MHz of the atomic resonance. Ongoing work is aimed at improving the experimental signal and understanding the degree of agreement between empirical data and computed molecular spectra.
Diatomic potentials for krypton are computed and also probed experimentally. For a probe-laser wavelength near 811811811 nm, several strong dipole-dipole interactions produce purely-long-range potential wells in the singly excited manifold of (s+ps+ps+p) potentials and in the doubly excited manifold of (p+pp+pp+p) and (s+ds+ds+d) potentials. Evidence of resonant photoassociation into bound states of these potential wells is observed in the emission of ions and ultraviolet photons from a magneto-optically trapped krypton cloud.
Creating ultracold molecules has attracted considerable interest in the last decade. Once created, such molecules can be used for precision spectroscopy or to study chemical reactions at ultracold tem peratures. Several techniques have been developed to produce ultracold molecules; the most common is photoassociation where two ultracold atoms collide in the presence of light that induces a free-bound transition to an excited molecular state. Photoassociation can also be used to perform spectroscopy in order to map out the ro-vibrational levels of a molecular state. In this dissertaiotn, we report on our Photoasociative Spectroscopy (PAS) studies conducted separately in argon and krypton. For each species, we have studied transitions near two different atomic limits ns[3/2]2 —> np[5/2]2 and ns[3/2]2 —» np[5/2]3where n = 4 for argon and n = 5 for krypton. The former atomic transition is called the “quench transition” since it forms a strong coupled channel to the ground state. As a result for this strong coupling the original atomic sample is degraded and quenched. The latter transition is the one used to cool and confine the atoms and is known as the “trapping transition.” Spectroscopy near the trapping transition in argon was studied previously in our group [1] and specific features were observed in the spectrum. At the time, the features were not definitively identified, but more than one explanation was suggested for further testing. One possible explanation was that these features were a result of resonances happening at “doubly-excited” molecular levels. The population of such states could take place as a result of absorbing two photons of the same frequency which causes photoassociation. In this dissertation we report on a series of experiments that were performed to study and conclusively identify the origin of those features. These experiments led to the conclusion that the features in the spectra were an artifact of otherwise undetectable frequency sidebands on our semiconductor diode laser. Once identified as such, a new laser was constructed to repeat the spectroscopy measurements in argon and take new measurements in krypton that would be free from laser artifacts. In those spectra, no specific vibrational features were observed and resolved in either species. Results were consistent with published results obtained by other groups using other noble gases. Finally, we report on our attempts to perform PAS on a quench transition in order to confirm results obtained for krypton by another group [2]. We were not able to observe any photoassociation signal for both argon and krypton on this transition. We were able to observe similar effects to those reported in Ref. [2] but we attribute these to artifacts from an acousto-optic modulator and not as arising from molecular structure.
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.
Ultracold atomic physics offers an experimentalist the opportunity to perform sensitive tests and measurements that are not possible at higher temperatures. In this case it allows for access to molecular states, through photoassociation, that are inaccessible to conventional techniques. We use photoassociation to measure quasi-bound levels of the 2 1Σg+ state of 85Rb2 . With these data, we examine a coupling between the short-range Hund’s case (c) 2 (0g+ ) component and the long-range 2 (1g ) state, which corresponds to the 1 1Πg state. A second experiment studies the mechanism of short-range photoassociation and finds our simple model to have strong predictive power. In a third experiment, we photoassociatively form vibrationally excited a 3 Σu+ molecules. We then excite these molecules using a frequency-doubled pulse-amplified CW laser to create low-n long-range Rydberg states of 85Rb2 . Autoionization and ion detection of these states gives high-resolution spectra, which are compared to theoretical potential curves.
We report photoassociative spectroscopy performed separately on Kr84 and Ar40. The spectra were obtained as a function of laser intensity with the spectroscopy laser tuned around the ns[3/2]2→np[5/2]3 trapping transition, where n=4 for argon and n=5 for krypton. The resulting spectra are the first ever obtained for krypton on this important transition. This transition in argon was previously studied in our group. At that time, discrete features were observed in the spectrum, but their origin was not conclusively identified. We have now identified these features as artifacts from laser sidebands. We discuss the origin of these sidebands, how they imprint their presence on the spectra, and present spectra for argon with the artifacts removed. For both krypton and argon, while we observe photoassociation, we do not observe any resolved vibrational structure. We present a theoretical analysis of the expected vibrational level spacings based on calculated potential curves and show that the absence of resolved structure in the spectra of our experiments (as configured) is not surprising. Finally, we discuss the requirements of future experiments in which resolution of vibrational structure in this system might be obtained.
We report photoassociative spectroscopy performed separately on Kr84 and Ar40. The spectra were obtained as a function of laser intensity with the spectroscopy laser tuned around the ns[3/2]2→np[5/2]3 trapping transition, where n=4 for argon and n=5 for krypton. The resulting spectra are the first ever obtained for krypton on this important transition. This transition in argon was previously studied in our group. At that time, discrete features were observed in the spectrum, but their origin was not conclusively identified. We have now identified these features as artifacts from laser sidebands. We discuss the origin of these sidebands, how they imprint their presence on the spectra, and present spectra for argon with the artifacts removed. For both krypton and argon, while we observe photoassociation, we do not observe any resolved vibrational structure. We present a theoretical analysis of the expected vibrational level spacings based on calculated potential curves and show that the absence of resolved structure in the spectra of our experiments (as configured) is not surprising. Finally, we discuss the requirements of future experiments in which resolution of vibrational structure in this system might be obtained.