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Physical Review A

Formation of ultracold X1Σ+(v′′=0) NaCs molecules via coupled photoassociation channels

Patrick Zabawa, Amy Wakim, Marek Haruza, N. P. Bigelow

Published Dec 5, 2011• 63 citations

Abstract

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 $\text{Na}\phantom{\rule{0.28em}{0ex}}3S+\text{Cs}\phantom{\rule{0.28em}{0ex}}6P$ complex. An $f$-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.

DOI: 10.1103/physreva.84.061401

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•Aug 17, 2016•47 citations

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

\text{Na}\phantom{\rule{0.28em}{0ex}}3S+\text{Cs}\phantom{\rule{0.28em}{0ex}}6P

complex. An

f

-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.

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

6 {}^{2}{P}_{3/2}

atomic line can be used to create a deeply bound molecular sample of ultracold polar NaCs. We assign $1 {}^{1}{\ensuremath{\Sigma}}^{+}$ (

v=4,5,6,11,19

) vibrational levels utilizing a pulsed depletion spectroscopic method (scanning

~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 report on the production of ultracold heteronuclear NaCs* molecules in a dual-species magneto-optical trap through photoassociation. The electronically excited molecules are formed below the Na (3S1/2) + Cs (6P1/2) dissociation limit. 12 resonance lines are detected using trap-loss spectroscopy based on a highly sensitive modulation technique. The highest observed rovibrational level exhibits clear hyperfine structure, which is detected for the first time. This structure is simulated within a simplified model consisting of 4 coupled levels belonging to the initially unperturbed Hund’s case “a” electronic states, which have been explored in our previous work that dealt with the Na (3S1/2) + Cs (6P3/2) asymptote [W. Liu et al., Phys. Rev. A 94, 032518 (2016)].

We demonstrate the direct formation of vibronic ground state RbCs molecules by photoassociation of ultracold atoms followed by radiative stabilization. The photoassociation proceeds through deeply bound levels of the (2)3Π0+ state. From analysis of the relevant free-to-bound and bound-to-bound Franck–Condon factors, we have predicted and experimentally verified a set of photoassociation resonances that lead to efficient creation of molecules in the v = 0 vibrational level of the X1Σ+ electronic ground state. We also compare the observed and calculated laser intensity required to saturate the photoassociation rate. We discuss the prospects for using short-range photoassociation to create and accumulate samples of ultracold polar molecules in their rovibronic ground state.