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Physical Review Letters

Observation of Ultracold Ground-State Potassium Molecules

Anguel Nikolov, Edward E. Eyler, X. T. Wang, J. Li, H. Wang, William C. Stwalley, P. L. Gould

Published Jan 25, 1999• 194 citations
Publisher

Abstract

Ultracold potassium molecules are produced in the $X^{1}\ensuremath{\Sigma}_{g}^{+}$ electronic ground state by photoassociation in a magneto-optical trap. They are detected sensitively and selectively by use of two-color resonant ionization, followed by time-of-flight mass spectroscopy. We observe deeply bound molecules with $\ensuremath{\nu}\ensuremath{\cong}36$, at a temperature of about $300\ensuremath{\mu}\mathrm{K}$. Presently about 1000 molecules/sec are produced, and much higher production rates should be attainable in the future.

DOI
10.1103/physrevlett.82.703

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Production and state-selective detection of ultracold molecular rubidium (85Rb2) in the singlet ground state and the metastable triplet state are described. Ultracold 85Rb2 molecules are produced via photoassociation followed by radiative decay. State-selective detection of high-ν ground-state and metastable-state molecules is carried out by resonant Two-photon ionization (R2PI) with a pulsed laser. The spectra of both the ground singlet and metastable triplet states are investigated. Spectroscopy of several intermediate excited states, some of which are observed for the first time, is also studied. Mixing between excited singlet and triplet states is observed in both the singlet and triplet spectra. A proposal for producing ν = 0 ground-state molecules by utilizing this singlet-triplet mixing is given. Magnetic trapping and filtering of metastable triplet-state molecules is also described, and a scheme for optical trapping of molecules is proposed.^

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Ultracold potassium molecules are produced in the X1\ensuremathΣg+X^{1}\ensuremath{\Sigma}_{g}^{+}X1\ensuremathΣg+​ electronic ground state by photoassociation in a magneto-optical trap. They are detected sensitively and selectively by use of two-color resonant ionization, followed by time-of-flight mass spectroscopy. We observe deeply bound molecules with \ensuremathν\ensuremath≅36\ensuremath{\nu}\ensuremath{\cong}36\ensuremathν\ensuremath≅36, at a temperature of about 300\ensuremathμK300\ensuremath{\mu}\mathrm{K}300\ensuremathμK. Presently about 1000 molecules/sec are produced, and much higher production rates should be attainable in the future.
In the first part of this dissertation we develop and successfully demonstrate two methods, based on photoassociation of ultracold potassium atoms, for producing ultracold K2 molecules, with sub mK temperatures, in deeply bound vibrational levels of the ground XS+g 1 state. The principal objective has been to develop an “ultracold molecule factory” that can be used to support experiments on spectroscopy, collisions, and chemistry of ultracold molecules. ^ In the first experiment the ground-state molecules are produced by the radiative decay of excited, n≅191 AS+u 1 state molecules, photoassociated from ultracold potassium atoms in a vapor-cell MOT. The decay is primarily into the vibrational continuum, but a small fraction decays into bound levels of the X state near n = 36. The experimentally observed molecule production rate is about 103 per second. ^ In our second experiment, we use two-step laser excitation to effect an “R-transfer” from long-range to intermediate internuclear separations, greatly increasing the efficiency for radiative production of low- n molecules in the X state. Molecules are formed in the Pg1 state by photoassociation, then excited by a second laser to the 51Pu or 61Pu Rydberg states, in selected vibrational levels from n = 13–18. Finally, radiative decay produces very large numbers of X state molecules with n≅25 and significant numbers of molecules in very low vibrational levels, including n = 0. We have observed production rates up to about 105 molecules/second per vibrational level. ^ In both experiments the ground-state molecules are detected with a sensitive and selective resonant two-color photoionization with nanosecond pulses. ^ In the second part of this dissertation we demonstrate a novel method for high sensitivity absorption measurements, that combines a phase modulated, high-resolution pulsed laser with an actively stabilized optical cavity to achieve a sensitivity of ∼10−9 per cm. This is comparable to the best existing methods for pulsed absorption measurements, but unlike most other methods, it can also be readily extended to the UV region and to Doppler-free spectroscopy. ^
We have produced ultracold polar RbCs molecules via photoassociation starting from laser-cooled 85 Rb and 133 Cs atoms in a dual-species, forced dark magneto-optical trap. The formed electronically excited RbCs* molecules correlated to the Rb(5S 1/2 ) + Cs(6P 1/2 ) dissociation limit are observed by trap loss spectroscopy. Following the decay of these excited RbCs* molecules, the formed ground state molecules are directly ionized by a two-photon single-color pulse dye laser, which is a new ionization mechanism for ground state RbCs molecules and thence detected by time-of-flight mass spectroscopy.
Summary form only given. We report results from an efficient new method for producing translationally cold (T<1 mK) potassium molecules in the ground X/sup 1//spl Sigma//sub g//sup +/ electronic state. We use the two-photon R-transfer scheme conceptually similar to a proposal by Band and Julienne (1995). First, ultracold potassium atoms in a MOT are photoassociated at long range to the 1/sub g/ molecular electronic state, which correlates to the 1/sup 1//spl Pi//sub g/ state at short range. The resulting molecules are then excited with a second laser to the 5/sup 1//spl Pi//sub u/ or 6/sup 1//spl Pi//sub u/ Rydberg states. These Rydberg states have favorable Franck-Condon factors for spontaneous decay into low vibrational levels of the ground state. The molecules are detected by use of two-color resonant ionization with pulsed lasers. By scanning one of the detection lasers, we observe transitions from several vibrational levels of the X state. The largest observed molecule formation rate in a single vibrational level is about 10/sup 5/ molecules/s for /spl nu/=25. Molecules in the lowest vibrational levels, including /spl nu/=0, are also observed with slightly lower rates of production. The translational temperature of the ground-state molecules is measured by analyzing their ballistic decay from the detection region. It is approximately 500 /spl mu/K, roughly the same as the estimated temperature of potassium atoms in the MOT.
We have produced ultracold heteronuclear KRb molecules by the process of photoassociation in a two-species magneto-optical trap. Following decay of the photoassociated KRb*, the molecules are detected using two-photon ionization and time-of-flight mass spectroscopy of KRb+{\mathrm{K}\mathrm{R}\mathrm{b}}^{+}KRb+. A portion of the metastable triplet molecules thus formed are magnetically trapped. Photoassociative spectra down to $91\text{ }\text{ }{\mathrm{c}\mathrm{m}}^{\ensuremath{-}1}$ below the K(4s)+Rb(5p1/2)\mathrm{K}(4s)+\mathrm{R}\mathrm{b}(5{p}_{1/2})K(4s)+Rb(5p1/2​) asymptote have been obtained. We have made assignments to all eight of the attractive Hund's case (c) KRb* potential curves in this spectral region.
We report the observation of translationally ultracold heteronuclear ground-state molecules in a two-species magneto-optical trap containing 39K and 85Rb atoms. The KRb molecules are produced via photoassociation and detected by multiphoton ionization. We had characterized their temperature and measured their formation rate constant. We believe that the two-species trap could be used as a reliable source of ultracold molecules to be captured by electrostatic, magnetic, or optical traps. This possibility will certainly motivate further investigation of quantum collective effects as well as high-resolution spectroscopy of the rovibrational level structure of cold heteronuclear molecular systems.
Production and state-selective detection of ultracold molecular rubidium (85Rb2) in the singlet ground state and the metastable triplet state are described. Ultracold 85Rb2 molecules are produced via photoassociation followed by radiative decay. State-selective detection of high-ν ground-state and metastable-state molecules is carried out by resonant Two-photon ionization (R2PI) with a pulsed laser. The spectra of both the ground singlet and metastable triplet states are investigated. Spectroscopy of several intermediate excited states, some of which are observed for the first time, is also studied. Mixing between excited singlet and triplet states is observed in both the singlet and triplet spectra. A proposal for producing ν = 0 ground-state molecules by utilizing this singlet-triplet mixing is given. Magnetic trapping and filtering of metastable triplet-state molecules is also described, and a scheme for optical trapping of molecules is proposed.^