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Physical Chemistry Chemical Physics

Photoassociation studies of ultracold NaCs from the Cs 62P3/2 asymptote

Amy Wakim, Patrick Zabawa, N. P. Bigelow

Published Jan 1, 2011• 12 citations
Publisher

Abstract

A combination of pulsed depletion spectroscopy and photoassociation spectroscopy is utilized to assign photoassociation spectra of NaCs. These methods investigate the ab initio Ω = 2 potential energy curve and indicate a previously unknown avoided crossing between the (3)Ω = 1 and (4)Ω = 1 electronic states. We present rotational assignments of deeply bound singlet ground state molecules, an improved C(6) coefficient for the (4)Ω = 1 and assignments for all twenty-three photoassociation resonances detuned from the Cs 6(2)P(3/2) asymptote.

DOI
10.1039/c1cp20928k

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A combination of pulsed depletion spectroscopy and photoassociation spectroscopy is utilized to assign photoassociation spectra of NaCs. These methods investigate the ab initio Ω = 2 potential energy curve and indicate a previously unknown avoided crossing between the (3)Ω = 1 and (4)Ω = 1 electronic states. We present rotational assignments of deeply bound singlet ground state molecules, an improved C(6) coefficient for the (4)Ω = 1 and assignments for all twenty-three photoassociation resonances detuned from the Cs 6(2)P(3/2) asymptote.
We present photoassociation spectroscopy of ultracold NaCs molecules formed in a dual-species magneto-optical trap. Excited-state molecules are formed in states correlating to the Na(3S 1/2 )+Cs(6P 3/2 ) asymptote. We assign the most prominent observed vibrational progression to the Ω=2 long range state based on a comparison with ab initio potentials. Molecules are secondarily excited before decaying to deeply bound levels of the electronic ground X 1 Σ + state where they are ionized and detected by time-of-flight mass spectroscopy.
We demonstrate that a photoassociation resonance detuned less than a wave number below the Cs 62P3/26 {}^{2}{P}_{3/2}62P3/2​ atomic line can be used to create a deeply bound molecular sample of ultracold polar NaCs. We assign $1 {}^{1}{\ensuremath{\Sigma}}^{+}$ (v=4,5,6,11,19v=4,5,6,11,19v=4,5,6,11,19) vibrational levels utilizing a pulsed depletion spectroscopic method (scanning  700~700 700 cm${}^{\ensuremath{-}1}$ at a time) in which we observe the $1 {}^{1}{\ensuremath{\Sigma}}^{+}\ensuremath{\rightarrow}2 {}^{1}{\ensuremath{\Sigma}}^{+}\ensuremath{-}1 {}^{3}\ensuremath{\Pi}$ vibrational progression. These data are compared with results from a hot-molecule collision-enhanced laser-induced fluorescence experiment and shown to be in good agreement. This technique is a powerful tool to experimentally determine the population distribution in any ultracold molecular system.
We have performed high precision photoassociation spectroscopy of ultracold cesium gas. Using trap-loss fluorescence detection and controlling the background cesium pressure we were able to photoassociate atoms into excited states of ultracold molecules with large detunings up to 56 cm(-1) below the Cs(6S(1/2)) + Cs(6P(1/2)) atomic asymptote. Vibrational progressions are assigned to 0(g)(-), 0(u)(+), and 1(g) long-range states. By fitting the spectral data to the LeRoy-Bernstein expression, the effective coefficients of the leading long-range interactions and the vibrational quantum number at dissociation are obtained. In addition we have observed spectral perturbations between states of the same symmetry belonging to different asymptotes (6P(1/2) and 6P(3/2)). The perturbations are manifested through irregular vibrational level spacings and are especially pronounced in the 0(u)(+) symmetry. Many observed rotational levels indicate d- and higher partial wave contributions to the photoassociation cross section in the presence of trapping laser light, while spectral regions with only weak features suggest nodes in the lower state wave functions corresponding to the two ground state atoms asymptote.
Comprehensive spectroscopic studies of hot and ultracold samples of NaCs molecules were combined to complete the investigation of the $(3)\ensuremath{\Omega}=1$ $\ensuremath{\leftarrow}$ XXX ${}^{1}{\ensuremath{\Sigma}}^{+}$ transition for the NaCs molecule. Polarization labeling, photoassociation, and pulsed laser depletion spectroscopy were used to collect data on rovibrational levels of the $(3)\ensuremath{\Omega}=1$ state [here described as the ccc ${}^{3}{\ensuremath{\Sigma}}^{+}$ state in Hund's case (a) notation]. The highest observed level was v=72v=72v=72 located $~$5 GHz below the atomic asymptote Na(32S1/23{ }^{2}{S}_{1/2}32S1/2​) +++ Cs(62P3/26{ }^{2}{P}_{3/2}62P3/2​). Approximately 1400 levels were used to construct the potential energy curve of the $(3)\ensuremath{\Omega}=1$ state for the full range of interatomic distances.
High precision photoassociation spectroscopy is performed in ultracold cesium gas, with detunings as large as 51 cm(-1) below the Cs(6S(1/2))+Cs(6P(3/2)) asymptote. Trap-loss fluorescence detection is used for detecting the photoassociation to excited state ultracold molecules. Long vibrational progressions are assigned to electronic states of 0(g) (-), 0(u) (+), and 1(g) symmetry. The spectral data are fitted to a LeRoy-Bernstein equation, in order to obtain the effective coefficients of the leading long-range interaction term (C(3)/R(3)) and the relative vibrational quantum numbers measured down from dissociation. Additionally we present evidence for perturbations between the 0(g) (-) state and the dark 2(u) state.
We report production of ultracold $X{\phantom{\rule{0.16em}{0ex}}}^{1}{\ensuremath{\Sigma}}^{+}({v}^{\ensuremath{'}\ensuremath{'}}=0)$ NaCs molecules via photoassociation. We utilize a combination of spectroscopic techniques to determine formation pathways and label ground-state samples. Efficient free-bound excitation occurs due to coupling between $B{\phantom{\rule{0.16em}{0ex}}}^{1}\ensuremath{\Pi}$ and neighboring electronic states in the Na3S+Cs6P\text{Na}\phantom{\rule{0.28em}{0ex}}3S+\text{Cs}\phantom{\rule{0.28em}{0ex}}6PNa3S+Cs6P complex. An fff-wave shape resonance contributes to formation of a rotationally pure sample of $X{\phantom{\rule{0.16em}{0ex}}}^{1}{\ensuremath{\Sigma}}^{+}({v}^{\ensuremath{'}\ensuremath{'}}=0,{J}^{\ensuremath{'}\ensuremath{'}}=1)$ molecules.