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The Journal of Chemical Physics

Photoassociation spectroscopy of the B Π1 state of LiCs

A. Grochola, A. Pashov, Johannes Deiglmayr, M. Repp, E. Tiemann, Roland Wester, Matthias Weidemüller

Published Aug 4, 2009• 23 citations
Publisher

Abstract

We present an accurate potential energy curve of the B (1)Pi state in the LiCs molecule for which vibrational levels between v(') = 0 and v(') = 35 (bound by 11.4 GHz) were measured by photoassociation spectroscopy in an ultracold ensemble of (7)Li and (133)Cs atoms. By the combination of conventional spectroscopic data of the B-X system and the new photoassociation measurements a very precise value of the dissociation energy of the ground state X (1)Sigma(+) of LiCs was determined to be D(0) = 5783.495(5) cm(-1).

DOI
10.1063/1.3180820

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We present an accurate potential energy curve of the B (1)Pi state in the LiCs molecule for which vibrational levels between v(') = 0 and v(') = 35 (bound by 11.4 GHz) were measured by photoassociation spectroscopy in an ultracold ensemble of (7)Li and (133)Cs atoms. By the combination of conventional spectroscopic data of the B-X system and the new photoassociation measurements a very precise value of the dissociation energy of the ground state X (1)Sigma(+) of LiCs was determined to be D(0) = 5783.495(5) cm(-1).
We recently reported the formation of ultracold LiCs molecules in the rovibrational ground state X1sigma+, v" = 0,J" = 0 (J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 133004). Here we discuss details of the experimental setup and present a thorough analysis of the photoassociation step including the photoassociation line shape. We predict the distribution of produced ground state molecules using accurate potential energy curves combined with an ab initio dipole transition moment and compare this prediction with experimental ionization spectra. Additionally we improve the value of the dissociation energy for the X1sigma+ state by high resolution spectroscopy of the vibrational ground state.
We present spectroscopic measurements of seven vibrational levels v=29−−35v=29--35v=29−−35 of the $A({1}^{1}{\ensuremath{\Sigma}}_{u}^{+})$ excited state of Li2{}_{2}2​ molecules by the photoassociation of a degenerate Fermi gas of 6{}^{6}6Li atoms. The absolute uncertainty of our measurements is $\ifmmode\pm\else\textpm\fi{}0.000\phantom{\rule{0.16em}{0ex}}02$ cm${}^{\ensuremath{-}1}$ ($\ifmmode\pm\else\textpm\fi{}600$ kHz) and we use these new data to further refine an analytic potential for this state. This work provides high accuracy photoassociation resonance locations essential for the eventual high-resolution mapping of the $X({1}^{1}{\ensuremath{\Sigma}}_{g}^{+})$ state enabling further improvements to the sss-wave scattering length determination of Li and enabling the eventual creation of ultracold ground-state 6{}^{6}6Li2{}_{2}2​ molecules.
Calculations of the adiabatic potential energy curves and the transition dipole moments between the ground (A 1 Σ + ) and the first excited (A 1 Σ + ) states have been determined for the LiCs and NaCs molecules. The calculations are performed using an ab initio approach based on non-empirical pseudopotentials for Cs + , Li + and Na + cores, parameterized l -dependent polarization potentials and full configuration interaction calculations. The potential energy curves and the transition dipole moment are used to estimate the radiative lifetimes of the vibrational levels of the A + Σ + state using the Franck–Condon (FC) approximation and the approximate sum rule method. The radiative lifetimes associated with the A + Σ + state are presented here for the first time. These data can help experimentalists to optimize photoassociative formation of ultracold molecules and their longevity in a trap or in an optical lattice.
We have obtained high-lying vibrational spectra for the rm1sp3Sigmasbspg+\\rm 1\\sp3\\Sigma\\sbsp{g}{+}rm1sp3Sigmasbspg+ and rm1sp1Sigmasbspu+\\rm 1\\sp1\\Sigma\\sbsp{u}{+}rm1sp1Sigmasbspu+ excited states of both rmsp7Lisb2\\rm \\sp7Li\\sb2rmsp7Lisb2 and rmsp6Lisb2\\rm \\sp6Li\\sb2rmsp6Lisb2 via photoassociation of colliding ultracold lithium atoms confined in a magneto-optical trap. Photoassociative spectroscopy of ultracold atoms is a powerful tool for probing molecular states near the dissociation energy that are inaccessible by other methods. For an ultracold lithium vapor, the distribution of unbound ground state energies is so small that precise free-bound spectroscopy is possible. Molecular hyperfine structure is resolved. We calculate accurate dissociation energies for both the rm1sp3Sigmasbspg+\\rm 1\\sp3\\Sigma\\sbsp{g}{+}rm1sp3Sigmasbspg+ and rm1sp1Sigmasbspu+\\rm 1\\sp1\\Sigma\\sbsp{u}{+}rm1sp1Sigmasbspu+ excited states of Lisb2\\sb2sb2. A model potential is constructed from a combination of experimental and theoretical information, and used to assign vibrational quantum numbers. We observe rotational structure and assign rotational quantum numbers.
In this thesis properties of ultracold alkali dimers are studied both theoretically and experimentally. In the first, theoretical, part, the prospects for the formation of ultracold LiCs dimers in deeply bound vibrational levels using photoassociation (PA) are investigated. Furthermore a previous systematic investigation of the structure of all alkali dimers is extended by the ab initio calculation of static dipole polarizabilities. An extensive comparison with other published results supports the reliability of the chosen method. Based on these results an experimental scheme for the creation of an sample of oriented ultracold dipolar molecules is developed. In the second, experimental part the formation of LiCs ground state molecules by PA is investigated. PA spectroscopy is used to improve the accuracy of the potential energy curve for the B1P and the value of the dissociation energy of the X1S+ state significantly. The rovibrational distribution of ground state molecules is probed in a combination of resonance-enhanced multi-photon ionization and depletion spectroscopy. A simple scheme is found to form ultracold polar LiCs molecules in the absolute ground state X1S+,v''=0,J''=0. In a quasi-electrostatic trap created by a CO2 laser, LiCs molecules are formed and stored. A lifetime of 24(3)s, limited by collisions with background gas, is observed and rate coefficients for inelastic collisions between LiCs in high vibrational states and Cs atoms are determined. The long storage time facilitates the observation of radiative decay of polar molecules towards lower vibrational levels.
We analyze the formation of ultracold 7 Li 133 Cs molecules in the rovibrational ground state through photoassociation into the B 1 Π state, which has recently been reported (Deiglmayr et al 2008 Phys. Rev. Lett. 101 133004). Absolute rate constants for photoassociation at large detunings from the atomic asymptote are determined and are found to be surprisingly large. The photoassociation process is modeled using a full coupled-channel calculation for the continuum state, taking all relevant hyperfine states into account. The enhancement of the photoassociation rate is found to be caused by an 'echo' of the triplet component in the singlet component of the scattering wave function at the inner turning point of the lowest triplet a 3 Σ + potential. This perturbation can be ascribed to the existence of a broad Feshbach resonance at low scattering energies. Our results elucidate the important role of couplings in the scattering wave function for the formation of deeply bound ground state molecules via photoassociation.