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Physical Chemistry Chemical Physics

Formation of ultracold Rb2 molecules in the v′′ = 0 level of the a3Σ+u state via blue-detuned photoassociation to the 13Πg state

Michael Bellos, David Rahmlow, Ryan Carollo, Jayita Banerjee, Olivier Dulieu, A. Gerdes, Edward E. Eyler, P. L. Gould, William C. Stwalley

Published Jan 1, 2011• 36 citations
Publisher

Abstract

We report on the observation of blue-detuned photoassociation in Rb(2), in which vibrational levels are energetically above the corresponding excited atomic asymptote. (85)Rb atoms in a MOT were photoassociated at short internuclear distance to levels of the 1(3)Π(g) state at a rate of approximately 5 × 10(4) molecules s(-1). We have observed most of the predicted vibrational levels for all four spin-orbit components; 0(+)(g), 0(-)(g), 1(g), and 2(g), including levels of the 0(+)(g) outer well. These molecules decay to the metastable a(3)Σ(+)(u) state, some preferentially to the v'' = 0 level, as we have observed for photoassociation to the v' = 8 level of the 1(g) component.

DOI
10.1039/c1cp21383k

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Journal of Physics B Atomic Molecular and Optical Physics•Sep 25, 2006•20 citations
We report on the observation of blue-detuned photoassociation in Rb(2), in which vibrational levels are energetically above the corresponding excited atomic asymptote. (85)Rb atoms in a MOT were photoassociated at short internuclear distance to levels of the 1(3)Π(g) state at a rate of approximately 5 × 10(4) molecules s(-1). We have observed most of the predicted vibrational levels for all four spin-orbit components; 0(+)(g), 0(-)(g), 1(g), and 2(g), including levels of the 0(+)(g) outer well. These molecules decay to the metastable a(3)Σ(+)(u) state, some preferentially to the v'' = 0 level, as we have observed for photoassociation to the v' = 8 level of the 1(g) component.
We report on the observation of blue-detuned photoassociation in Rb2, in which vibrational levels are energetically above the corresponding excited atomic asymptote. 85Rb atoms in a MOT were photoassociated at short internuclear distances to levels of the (1)3Pi g state at a rate of approximately 5x10^4 molecules/s. We have observed most of the predicted vibrational levels for all four spin-orbit components 0g+, 0g-, 1g, and 2g, including levels of the 0g+ outer well. These molecules decay to the metastable a3Sigma u+ state, some preferentially to the v"=0 level, as we have observed for photoassociation to the v'=8 level of the 1g component.
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.
Ultracold metastable RbCs molecules are observed in a double species magneto-optical trap through photoassociation near the Rb(5S(1/2)) + Cs(6P(3/2)) dissociation limit followed by radiative stabilization. The molecules are formed in their lowest triplet electronic state and are detected by resonance enhanced two-photon ionization through the previously unobserved (3)(3)Π ← a (3)Σ(+) band. The large rotational structure of the observed photoassociation lines is assigned to the lowest vibrational levels of the 0(+) or 0(-) excited states correlated to the Rb(5P(1/2)) + Cs(6S(1/2)) dissociation limit. This demonstrates the possibility of inducing direct photoassociation in heteronuclear alkali-metal molecules at a short internuclear distance, as pointed out earlier [J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 13304].
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.
We report the observation of photoassociation to the $2{\phantom{\rule{0.16em}{0ex}}}^{1}\phantom{\rule{-0.16em}{0ex}}{\ensuremath{\Sigma}}_{g}^{+}$ state of 85{}^{85}85Rb2{}_{2}2​. We have observed two vibrational levels (${v}^{\ensuremath{'}}=98,99$) below the 5s1/2+5p1/25{s}_{1/2}+5{p}_{1/2}5s1/2​+5p1/2​ atomic limit and 11 vibrational levels (${v}^{\ensuremath{'}}=102$--112) above it. The photoassociation---and subsequent spontaneous emission---occur predominantly between 15 and 20 bohrs in a region of internuclear distance best described as a transition between Hund's case (a) and Hund's case (c) coupling. The presence of a ggg-wave shape resonance in the collision of two ground-state atoms affects the photoassociation rate and line shape of the ${J}^{\ensuremath{'}}=3$ and 5 rotational 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.