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The Journal of Chemical Physics

Spectroscopic investigation of the A and 3 1Σ+ states of 39K85Rb

Jin‐Tae Kim, Yonghoon Lee, Bongsoo Kim, Dajun Wang, P. L. Gould, Edward E. Eyler, William C. Stwalley

Published Dec 26, 2012• 9 citations
Publisher

Abstract

By using a combination of molecular beam (MB) excitation spectra and two distinct ultracold molecule excitation spectra (UM+ and UM-), we have assigned high vibrational levels of the A and 3 (1)Σ(+) states from absorption spectra of the mutually strongly perturbed A (1)Σ(+) - 3 (1)Σ(+) - 1 (1)Π - 2 (3)Σ(+) - b (3)Π states of ultracold (39)K(85)Rb molecules in the energy region between 15,116 and 16,225 cm(-1) above the minimum of the ground X (1)Σ(+) state. The ultracold molecules (UM+ and UM-) are formed by radiative decay following photoassociation (PA) to a specific level of the 3(0(+)) state (UM+) or to a specific level of the 3(0(-)) state (UM-). We observe that the A and 3 (1)Σ(+) states are observable in the UM+ spectra, but absent from the UM- spectra. This is explained by considering Hund's case (c) selection rules and transition dipole moments between the upper excited A (1)Σ(+) (2(0(+))) state and the three Ω components (0(+), 0(-), and 1) at the ground-state dissociation limit. We propose further investigations of the extended potential wells of the A and 3 (1)Σ(+) states by combining short-range MB excitation spectra in a narrow Franck-Condon (FC) window near R(e) of the X (1)Σ(+) state, and long-range UM (and PA) excitation spectra, which have much larger FC windows.

DOI
10.1063/1.4771661

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By using a combination of molecular beam (MB) excitation spectra and two distinct ultracold molecule excitation spectra (UM+ and UM-), we have assigned high vibrational levels of the A and 3 (1)Σ(+) states from absorption spectra of the mutually strongly perturbed A (1)Σ(+) - 3 (1)Σ(+) - 1 (1)Π - 2 (3)Σ(+) - b (3)Π states of ultracold (39)K(85)Rb molecules in the energy region between 15,116 and 16,225 cm(-1) above the minimum of the ground X (1)Σ(+) state. The ultracold molecules (UM+ and UM-) are formed by radiative decay following photoassociation (PA) to a specific level of the 3(0(+)) state (UM+) or to a specific level of the 3(0(-)) state (UM-). We observe that the A and 3 (1)Σ(+) states are observable in the UM+ spectra, but absent from the UM- spectra. This is explained by considering Hund's case (c) selection rules and transition dipole moments between the upper excited A (1)Σ(+) (2(0(+))) state and the three Ω components (0(+), 0(-), and 1) at the ground-state dissociation limit. We propose further investigations of the extended potential wells of the A and 3 (1)Σ(+) states by combining short-range MB excitation spectra in a narrow Franck-Condon (FC) window near R(e) of the X (1)Σ(+) state, and long-range UM (and PA) excitation spectra, which have much larger FC windows.
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 spectroscopic characterization of excited electronic states of KRb by combining spectra from molecular beam (MB) experiments with those from ultracold molecules (UM) formed by photoassociation (PA) of ultracold atoms. Spectra involving the 1(1)Π, 2(3)Σ(+), and b(3)Π states in a strongly perturbed region have been identified. This approach provides a powerful method to identify the vibrational levels of the excited electronic states perturbed globally by neighboring electronic states. This is because the two sets of spectra from the UM and the MB experiments probe the same energy region from very different initial electronic states. The UM experiments utilize high v'' levels of the a(3)Σ(+) state with large internuclear separations, while the MB experiments utilize low v'' levels of the ground X(1)Σ(+) state with near-equilibrium internuclear separations. Only the Ω = 1 levels of the 2(3)Σ(+) and b(3)Π states are observed in the MB spectra, while the Ω = 0(-), 1 levels of the 2(3)Σ(+) state and the Ω = 0(±), 1, 2 levels of the b(3)Π state are observed in the UM spectra.
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.
Ultracold atomic physics offers an experimentalist the opportunity to perform sensitive tests and measurements that are not possible at higher temperatures. In this case it allows for access to molecular states, through photoassociation, that are inaccessible to conventional techniques. We use photoassociation to measure quasi-bound levels of the 2 1Σg+ state of 85Rb2 . With these data, we examine a coupling between the short-range Hund’s case (c) 2 (0g+ ) component and the long-range 2 (1g ) state, which corresponds to the 1 1Πg state. A second experiment studies the mechanism of short-range photoassociation and finds our simple model to have strong predictive power. In a third experiment, we photoassociatively form vibrationally excited a 3 Σu+ molecules. We then excite these molecules using a frequency-doubled pulse-amplified CW laser to create low-n long-range Rydberg states of 85Rb2 . Autoionization and ion detection of these states gives high-resolution spectra, which are compared to theoretical potential curves.