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Physical Review Letters

Two-color spectroscopy of colliding ultracold atoms

Vanderlei Salvador Bagnato, Luís Gustavo Marcassa, Chia‐Wen Tsao, Youjun Wang, J. Weiner

Published May 24, 1993• 72 citations
Publisher

Abstract

We present experimental results of two-color photoassociative ionization (TCPAI) spectroscopy in a magneto-optical trap. A probe light beam traces out the frequency (and intensity) dependence of TCPAI. By manipulating the intensities of the trap and repumper lasers we investigate the participation of different hyperfine ground-state levels and demonstrate the conditions under which molecular bound states figure in the collision intermediate.

DOI
10.1103/physrevlett.70.3225

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We present experimental results of two-color photoassociative ionization (TCPAI) spectroscopy in a magneto-optical trap. A probe light beam traces out the frequency (and intensity) dependence of TCPAI. By manipulating the intensities of the trap and repumper lasers we investigate the participation of different hyperfine ground-state levels and demonstrate the conditions under which molecular bound states figure in the collision intermediate.
We study photo-associative ionization (PAI) for sodium atoms held in a magneto-optical trap (T < 1 mK). The process is investigated using one and two laser frequencies. For a single color PAI, we measure the rate constant as a function of light intensity and the result is compared with calculation based on semiclassical Bloch equation theory. The measured rate constant appears to saturate sooner than theory. In the two-color PAI (TCPAI) we investigate individual steps of the process. Different combinations of laser frequencies prepare different populations in each of the hyperfine ground state and the contribution of each one in this collisional process is investigated. The comparison with theory allows a fairly clear understanding of PAI and TCPAI.
We describe the experimental observation of ultracold NaCs+{\mathrm{NaCs}}^{+}NaCs+ molecular formation in a novel two-species magneto-optical trap. We interpret our observations in terms of a photoassociative ionization pathway similar to that observed in a sodium trap: $\mathrm{Na}+\mathrm{Cs}+\ensuremath{\Elzxh}{\ensuremath{\omega}}_{\mathrm{Na}}+\ensuremath{\Elzxh}{\ensuremath{\omega}}_{\mathrm{Cs}}\ensuremath{\rightarrow}{\mathrm{NaCs}}^{+}{+e}^{\ensuremath{-}}$. We have directly measured the NaCs+{\mathrm{NaCs}}^{+}NaCs+ production rate as a function of the excitation laser frequency and intensity elucidating the role of ground-state hyperfine levels. We have observed resonance structures in the frequency-dependent ion rate which we associate with the molecular character of the process.
The spectra of the high-lying vibrational levels of the Asp1Sigmasbspu+A\\sp1\\Sigma\\sbsp{u}{+}Asp1Sigmasbspu+ and 1sp3Sigmasbspg+1\\sp3\\Sigma\\sbsp{g}{+}1sp3Sigmasbspg+ singly excited states of both sp6rmLisb2\\sp6\\rm Li\\sb2sp6rmLisb2 and sp7rmLisb2\\sp7\\rm Li\\sb2sp7rmLisb2 are obtained via photoassociation of colliding ultracold atoms confined in a magneto-optical trap. The least bound state of the asp3Sigmasbspu+a\\sp3\\Sigma\\sbsp{u}{+}asp3Sigmasbspu+ ground state potential, obtained by two-photon photoassociative spectroscopy, is also presented for both sp7rmLisb2\\sp7\\rm Li\\sb2sp7rmLisb2 and sp6rmLisb2\\sp6\\rm Li\\sb2sp6rmLisb2. The vibrational levels have resolved hyperfine structure, whose relative energy splittings and transition strengths are accurately modeled. The photoassociative spectra are used to precisely determine both the singlet and triplet s-wave scattering lengths for both isotopes, which are important parameters in systems designed to observe quantum degenerate effects and Bose-Einstein condensation.
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.