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New Journal of Physics

Spectroscopy of39K85Rb triplet excited states using ultracold a3Σ+state molecules formed by photoassociation

J T Kim, Dajun Wang, Edward E. Eyler, P. L. Gould, William C. Stwalley

Published May 14, 2009• 27 citations
Publisher

Abstract

Convenient state-selective detection methods are proposed for exploring triplet Rydberg states from the metastable a 3 Σ + state of ultracold KRb molecules by resonance-enhanced two-photon ionization and time-of-flight (TOF) mass spectroscopy. This would allow the first accurate determination of the ionization potential. Particularly suitable resonant intermediate states include the 2 3 Π Ω , 3 3 Σ + and 4 3 Σ + states, and we report spectroscopic studies of these states. For the 2 3 Π Ω state, the spin–orbit components (Ω = 0 + , 0 − , 1 and 2) have been investigated and a shallow long-range state (5(0 + )) at ∼ 9.3 Å has been observed. We compare our observations of these three states with predictions based on ab initio potential energy curves. Such studies may also permit the direct observation of autoionizing resonances leading to efficient formation of low-lying rovibrational levels of the 2 Σ + ground state of KRb + , ideally in the v + = 0, N + = 0 level.

DOI
10.1088/1367-2630/11/5/055020

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Convenient state-selective detection methods are proposed for exploring triplet Rydberg states from the metastable a 3 Σ + state of ultracold KRb molecules by resonance-enhanced two-photon ionization and time-of-flight (TOF) mass spectroscopy. This would allow the first accurate determination of the ionization potential. Particularly suitable resonant intermediate states include the 2 3 Π Ω , 3 3 Σ + and 4 3 Σ + states, and we report spectroscopic studies of these states. For the 2 3 Π Ω state, the spin–orbit components (Ω = 0 + , 0 − , 1 and 2) have been investigated and a shallow long-range state (5(0 + )) at ∼ 9.3 Å has been observed. We compare our observations of these three states with predictions based on ab initio potential energy curves. Such studies may also permit the direct observation of autoionizing resonances leading to efficient formation of low-lying rovibrational levels of the 2 Σ + ground state of KRb + , ideally in the v + = 0, N + = 0 level.
We report the observation and analysis of the 3 (3)ΠΩ double-minimum electronic excited state of (39)K(85)Rb. The spin-orbit components (0(+), 0(-), 1, and 2) of this state are investigated based on potentials developed from the available ab initio potential curves. We have assigned the vibrational levels v' = 2-11 of the 3 (3)Π1,2 potentials and v' = 2-12 of the 3(3)Π0(+/-) potential. We compare our experimental observations of the 3 (3)ΠΩ state with predictions based on theoretical potentials. The observations are based on resonance enhanced multiphoton ionization of ultracold KRb in vibrational levels v" = 14-25 of the a (3)Σ(+) state. These a-state ultracold molecules are formed by photoassociation of ultracold (39)K and (85)Rb atoms to the 5(1) state of KRb followed by spontaneous emission to the a state.
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.
We have studied resonance-enhanced two-photon ionization of ultracold 39 K 85 Rb molecules in highly excited long-range vibrational levels of the X 1 Σ + and a 3 Σ + states. These molecules are formed by photoassociation (PA) of ultracold 39 K and 85 Rb atoms, followed by spontaneous emission to the X 1 Σ + and a 3 Σ + states. In the range 15 500–17 200 cm −1 , we observe many intermediate and long-range levels of the previously unobserved 4 3 Σ + and 4 1 Σ + states and evidence for the onset of the previously unobserved 3 3 Π state. The observed vibrational spectra of these states are in very good agreement with calculated vibrational levels based on the ab initio potentials of Rousseau, Allouche and Aubert-Frécon. Such experiments illustrate some of the unique advantages of using PA-produced ultracold molecules for investigation of long-range vibrational levels and long-range forces, and for unravelling dense spectra because only a few rotational levels are populated.
We report the formation of ultracold (7)Li(85)Rb molecules in the a(3)Σ(+) electronic state by photoassociation (PA) and their detection via resonantly enhanced multiphoton ionization (REMPI). With our dual-species Li and Rb magneto-optical trap apparatus, we detect PA resonances with binding energies up to ∼62 cm(-1) below the (7)Li 2s (2)S1/2 + (85)Rb 5p (2)P1/2 asymptote. In addition, we use REMPI spectroscopy to probe the a(3)Σ(+) state and excited electronic 3(3)Π and 4(3)Σ(+) states and identify a(3)Σ(+) (v″ = 7-13), 3(3)Π (vΠ' = 0-10), and 4(3)Σ(+) (vΣ' = 0-5) vibrational levels. Our line assignments agree well with ab initio calculations. These preliminary spectroscopic studies on previously unobserved electronic states are crucial to discovering transition pathways for transferring ultracold LiRb molecules created via PA to deeply bound rovibrational levels of the electronic ground state.