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The Journal of Chemical Physics

Observation and deperturbation of near-dissociation ro-vibrational structure of the Cs2 state u+ (A1Σu+∼b3Π+u) at the asymptote 6S1/2 + 6P1/2

Wenliang Liu, Rundong Xu, Jizhou Wu, Jinxin Yang, Sergey S. Lukashov, V. B. Sovkov, Xingcan Dai, Jie Ma, Liantuan Xiao, Suotang Jia

Published Sep 28, 2015• 19 citations
Publisher

Abstract

New ro-vibrational structures of cold Cs2 in the 0u(+) state near the asymptote 6S1/2 + 6P1/2 are resolved. The variation of the rotational constants shows that the related energy spectra are strongly perturbed. An analysis of new data along with the empirical and theoretical information available from other sources is performed. For this purpose the model of spin-orbit coupling of the Hund's case (a) states A(1)Σu(+)∼b(3)Πu proposed by Bai et al. [Phys. Rev. A 83, 032514 (2011)] is extrapolated to the dissociation limit, and the parameters of the extrapolation are fitted from the near-dissociation experimental data.

DOI
10.1063/1.4931646

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The Journal of Chemical Physics•May 22, 1999•237 citations
New ro-vibrational structures of cold Cs2 in the 0u(+) state near the asymptote 6S1/2 + 6P1/2 are resolved. The variation of the rotational constants shows that the related energy spectra are strongly perturbed. An analysis of new data along with the empirical and theoretical information available from other sources is performed. For this purpose the model of spin-orbit coupling of the Hund's case (a) states A(1)Σu(+)∼b(3)Πu proposed by Bai et al. [Phys. Rev. A 83, 032514 (2011)] is extrapolated to the dissociation limit, and the parameters of the extrapolation are fitted from the near-dissociation experimental data.
This article demonstrates new observation of the high-resolution ro-vibrational bichromatic photoassociation spectra (BPAS) of Cs2 in the 0u+ long-range state below the asymptotes 6S1/2 + 6P1/2. By combining with a modulation spectroscopic technique, precise references of the frequency differences have been engineered through the BPAS, with which the rotational constants of low-lying vibrational levels of the Cs20u+ long-range state have been accurately determined by fitting the frequency differences to the non-rigid-rotor model. The rotational constants for the newly observed seven ro-vibrational levels are summarized and disagreement for the level ῦ = 498 is clarified. The rotational constants of different vibrational levels demonstrate strong perturbations of the related energy structures. A simple analysis is performed and shows good agreement with experimental results.
We report on new observations of the photoassociation spectroscopy of ultracold cesium molecules using a highly sensitive detection technique and a combined analysis with all observed electronic states. The technique is achieved by directly modulating the frequency of the trapping lasers of a magneto-optical trap. New observations of the Cs2 0g(-), 0u(+), and 1g states at the asymptotes 6S1/2 + 6P1/2 and 6S1/2 + 6P3/2 are reported. The spectral range is extended to the red detuning of 112 cm(-1) below the 6S1/2 + 6P3/2 dissociation limit. Dozens of vibrational levels of the ultracold Cs2 0g(-), 0u(+), and 1g states are observed for the first time. The available experimental binding energies of these states are analyzed simultaneously in a framework of the generalized LeRoy-Bernstein theory and the almost degenerate perturbation theory by Marinescu and Dalgarno [Phys. Rev. A: At., Mol., Opt. Phys. 52, 311 (1995)]. The unique atomic-related parameter c3 governing the dispersion forces of all the molecular states is estimated as (10.29 ± 0.05) a.u.
We present perturbations in photoassociation spectra of ultracold caesium. High-precision photoassociation spectra up to 54 cm−1 below the Cs (6S1/2)+Cs(6P1/2) asymptote revealed perturbations related to resonant coupling between electronic states of the same symmetry but belonging to different asymptotes. The perturbations, which are manifested as irregularities in vibrational level spacings, are most pronounced for the 0u+ state, but to some extent present in the 1g and 0g− states, which are also affected by predissociation. We have performed theoretical calculations of perturbations for all three states and found qualitative agreement with the experimental results.
The photoassociation spectroscopic data of the long-range molecular 1g state of Cs 2 in the asymptotic range red detuned [-5.02, -2.45 cm -1 ] to the (6S 1/2 +6P 3/2 ) dissociation limit detected using photon counting technique are presented and 18 new high-lying vibrational energy levels are obtained. Fitting experimental data to the improved LeRoy–Bernstein (LRB) formula, we have obtained the long-range molecular coefficient c 3 with a high precision and also demonstrated the necessity of the improved LRB formula for more precise c 3 coefficient by analyzing the residual from fitting procedure.
The mapped Fourier grid method, using a coordinate adapted to the local de Broglie wavelength associated to the vibrational motion in a molecule, and recently developed by Kokoouline et al. [J. Chem. Phys. 110, 9865 (1999)], is used to compute the perturbed binding energies and rotational constants of the Cs20u+(6s+6p2P1/2,3/2){\mathrm{Cs}}_{2}{0}_{u}^{+}(6s+6p{}^{2}{P}_{1/2,3/2})Cs2​0u+​(6s+6p2P1/2,3/2​) photoassociation spectrum below the lower dissociation limit. The results are shown to be very sensitive to the molecular potential curves and spin-orbit coupling. In the case of Rb20u+(5s+5p2P1/2,3/2),{\mathrm{Rb}}_{2}{0}_{u}^{+}(5s+5p{}^{2}{P}_{1/2,3/2}),Rb2​0u+​(5s+5p2P1/2,3/2​), a strong isotopic effect is also predicted. The results can be interpreted in the framework of generalized two-channel quantum defect theory, and generalized Lu-Fano plots are presented. This work suggests that parameters could easily be fitted to experimental spectra, eliminating the difficulties caused by limitations in the accuracy of the short-range molecular potentials.
Numerical calculations of vibrational levels of alkali dimers close to the dissociation limit are developed in the framework of a Fourier Grid Hamiltonian method. The aim is to interpret photoassociation experiments in cold atom samples. In order to avoid the implementation of very large grids we propose a mapping procedure adapted to the asymptotic R−n behavior of the long-range potentials. On a single electronic potential, this allows us to determine vibrational wave functions extending up to 500a0 using a minimal number of grid points. Calculations with two electronic states, A 1Σu+ and b 3Πu states, both correlated to the Rb(5s)+Rb(5p) dissociation limit, coupled by fine structure are presented. We predict strong perturbation effects in the Rb2(0u+) spectrum, manifested under the 5s, 5p 2P1/2 dissociation limit by an oscillatory behavior of the rotational constants.