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Quantum Electronics and Laser Science Conference

Efficient production and spectroscopy of ultracold potassium molecules in the electronic ground state

J. R. Ensher, Anguel Nikolov, Edward E. Eyler, H. Wang, William C. Stwalley, P. L. Gould

Published May 12, 2000• 0 citations
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Abstract

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.

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Production of ultracold potassium molecules and development of high sensitivity spectroscopic methods

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State-selective detection of near-dissociation ultracold KRb X Σ + 1 and a Σ + 3 molecules

Dajun Wang, Edward E. Eyler, P. L. Gould +1 more

We report on the state-selective detection of near-dissociation ultracold KRb molecules in the ground $X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+}$ state and the metastable $a\phantom{\rule{0.2em}{0ex}}^{3}\ensuremath{\Sigma}^{+}$ state. The molecules are produced by photoassociation of ultracold atoms followed by radiative decay into high vibrational levels of the $X$ and $a$ states. Detection utilizes resonance-enhanced one-color two-photon ionization, followed by time-of-flight mass spectroscopy. Scanning the detection laser frequency over the range $582--625\phantom{\rule{0.3em}{0ex}}\mathrm{nm}$, we observe transitions from the ${v}^{\ensuremath{''}}=86--92$ levels of the $X$ state, which are bound by up to $30\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$, and the ${v}^{\ensuremath{''}}=17--23$ levels of the $a$ state, which are also bound by up to $30\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The measured vibrational spacings are in excellent agreement with those previously measured and those calculated from the relevant potential curves. Relative vibrational populations are also consistent with Franck-Condon factors for decay from the photoassociated levels.

arXiv:physics/0506232•Physical Review A•Sep 13, 2005•28 citations
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 developed a two-step " R-transfer" method that efficiently produces translationally ultracold potassium molecules in the X (1)Sigma(+)(g) electronic ground state. Laser-cooled atoms are initially photoassociated at large internuclear separation R to form molecules in high vibrational levels of the 1 (1)Pi(g) state, which are in turn excited by an additional laser to shorter-range Rydberg states such as 5 (1)Pi(u) and 6 (1)Pi(u). Subsequent radiative decay produces ground-state molecules at rates up to 10(5) molecules/second per vibrational level.
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 investigate the production of ultracold ground state X 1 σ + (v = 0) RbCs molecules in the lowest vibrational level via short-range photoassociation followed by spontaneous emission. The starting point is the laser cooled 85 Rb and 133 Cs atoms in a dual species, forced dark magneto-optical trap. The special intermediate level (5)0 + (v = 10) correlated to the (2) 3 π electric state is achieved by the photoassociation process. The formed ground state X 1 σ + (v = 0) molecule is resonantly excited to the 2 1 π intermediate state by a 651 nm pulse laser and is ionized by a 532 nm pulse laser and then detected by the time-of-flight mass spectrum. Saturation of the photoionization spectroscopy at large ionization laser energy is observed and the ionization efficiency is obtained from the fitting. The production of ultracold ground state 85 Rb 133 Cs molecules is facilitative for the further research about the manipulation of ultracold molecules in the rovibrational ground state.
We form ultracold ground-state Rb 2 molecules by photoassociating pairs of atoms in a magneto-optical trap into the 0 u + state, which decays radiatively into high vibrational levels of the X 1 Σ g + state. Sensitive and vibrationally state-selective detection is achieved by means of resonantly-enhanced two-photon ionization with a pulsed laser. Frequency scans of the detection laser reveal a long vibrational progression to a previously unobserved electronic excited state, which we identify as the 2 1 Σ u + state. Most of its vibrational spectrum is in excellent agreement with predictions based on ab initio potentials, although the lowest vibrational levels exhibit strong perturbative mixing with the triplet 2 3 Π u state. The detection method reported here, with minor variations, should be effective for the entire potential well of the X state. In this work no transitions are observed from vibrational levels above v = 118, but this turns out to be a limitation not of the detection method but rather of the photoassociative formation scheme, due to re-excitation of the highest- v levels by the same photoassociation laser that produces them.
This thesis describes the spectroscopy work on ultracold 39K 85Rb molecules as part of our effort towards producing ground-state ultracold polar molecules. ^ The starting points of our experiment are laser cooled and trapped K and Rb atoms in dual-species MOTs and the molecule formation method is photoassociation (PA). A fraction of the PA-produced excited-state molecules can spontaneously emit to the two lowest electronic states, the X 1Σ + state and the a 3Σ + state, to form high vibrational level molecules. In order to develop a population transfer scheme to make deeply bound molecules, we have studied the spectroscopy of KRb in several steps. Besides the PA step, we have also carried out a state-selective detection experiment to study the population distribution of the high vibrational level molecules formed via spontaneous emission. The detection method is pulsed-laser based ion time-of-flight mass spectroscopy. Due to the linewidth limitations of the pulsed laser, this detection method can only resolve vibrational structures. A cw laser induced ion depletion spectroscopy technique has been developed in order to obtain rotational resolution. Using this ion depletion method, we have studied a possible stimulated Raman transfer scheme via the 3 1Σ+ state. To this end, we have obtained all the spectroscopic information required to produce deeply bound KRb molecules in a single vibrational and rotational level. ^ Several other spectroscopic studies using the high vibrational level ultracold molecules are also discussed. ^
We report on the state-selective detection of near-dissociation ultracold KRb molecules in the ground $X\phantom{\rule{0.2em}{0ex}}^{1}\ensuremath{\Sigma}^{+}$ state and the metastable $a\phantom{\rule{0.2em}{0ex}}^{3}\ensuremath{\Sigma}^{+}$ state. The molecules are produced by photoassociation of ultracold atoms followed by radiative decay into high vibrational levels of the XXX and aaa states. Detection utilizes resonance-enhanced one-color two-photon ionization, followed by time-of-flight mass spectroscopy. Scanning the detection laser frequency over the range 582−−625nm582--625\phantom{\rule{0.3em}{0ex}}\mathrm{nm}582−−625nm, we observe transitions from the ${v}^{\ensuremath{''}}=86--92$ levels of the XXX state, which are bound by up to $30\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$, and the ${v}^{\ensuremath{''}}=17--23$ levels of the aaa state, which are also bound by up to $30\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$. The measured vibrational spacings are in excellent agreement with those previously measured and those calculated from the relevant potential curves. Relative vibrational populations are also consistent with Franck-Condon factors for decay from the photoassociated levels.