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The Journal of Chemical Physics

New observation and combined analysis of the Cs2g−, u+, and 1g states at the asymptotes 6S1/2 + 6P1/2 and 6S1/2 + 6P3/2

Jie Ma, Wenliang Liu, Jinxin Yang, Jizhou Wu, Weiguo Sun, Valery S. Ivanov, Alexei S. Skublov, V. B. Sovkov, Xingcan Dai, Suotang Jia

Published Dec 28, 2014• 23 citations
Publisher

Abstract

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.

DOI
10.1063/1.4904265

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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.
Photoassociation spectroscopy with high resolution for 0u+(6P3/2) long-range state of ultracold cesium molecules has been measured experimentally using the modulated trap loss fluorescence spectroscopy technology. The spectral range has been extended over 60 cm-1 below the 6S1/2 + 6P3/2 dissociation limit as compared with other groups. twenty-five new observations of the Cs2 0u+ in long-range state are reported. The vibrational binding energies of these states are analyzed by using the LeRoy-Bernstein formula. The long-range parameter C3 in molecular 0u+(6P3/2) state is derived for 16.1030.010, and the corresponding molecular potential curve is depicted.
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.
We have performed high precision photoassociation spectroscopy of ultracold cesium gas. Using trap-loss fluorescence detection and controlling the background cesium pressure we were able to photoassociate atoms into excited states of ultracold molecules with large detunings up to 56 cm(-1) below the Cs(6S(1/2)) + Cs(6P(1/2)) atomic asymptote. Vibrational progressions are assigned to 0(g)(-), 0(u)(+), and 1(g) long-range states. By fitting the spectral data to the LeRoy-Bernstein expression, the effective coefficients of the leading long-range interactions and the vibrational quantum number at dissociation are obtained. In addition we have observed spectral perturbations between states of the same symmetry belonging to different asymptotes (6P(1/2) and 6P(3/2)). The perturbations are manifested through irregular vibrational level spacings and are especially pronounced in the 0(u)(+) symmetry. Many observed rotational levels indicate d- and higher partial wave contributions to the photoassociation cross section in the presence of trapping laser light, while spectral regions with only weak features suggest nodes in the lower state wave functions corresponding to the two ground state atoms asymptote.
High precision photoassociation spectroscopy is performed in ultracold cesium gas, with detunings as large as 51 cm(-1) below the Cs(6S(1/2))+Cs(6P(3/2)) asymptote. Trap-loss fluorescence detection is used for detecting the photoassociation to excited state ultracold molecules. Long vibrational progressions are assigned to electronic states of 0(g) (-), 0(u) (+), and 1(g) symmetry. The spectral data are fitted to a LeRoy-Bernstein equation, in order to obtain the effective coefficients of the leading long-range interaction term (C(3)/R(3)) and the relative vibrational quantum numbers measured down from dissociation. Additionally we present evidence for perturbations between the 0(g) (-) state and the dark 2(u) state.
We report on the production of ultracold heteronuclear NaCs* molecules in a dual-species magneto-optical trap through photoassociation. The electronically excited molecules are formed below the Na (3S1/2) + Cs (6P1/2) dissociation limit. 12 resonance lines are detected using trap-loss spectroscopy based on a highly sensitive modulation technique. The highest observed rovibrational level exhibits clear hyperfine structure, which is detected for the first time. This structure is simulated within a simplified model consisting of 4 coupled levels belonging to the initially unperturbed Hund’s case “a” electronic states, which have been explored in our previous work that dealt with the Na (3S1/2) + Cs (6P3/2) asymptote [W. Liu et al., Phys. Rev. A 94, 032518 (2016)].
In this paper, ultracold cesium molecules are formed through photoassociation technology, which is carried out in a magneto-optical trap. High resolution photoassociaion spectra with the rotational progressions up to J = 7 are obtained. Three rovibrational levels of the long-range 0 u + state of Cs 2 below the (6S 1/2 + 6P 1/2 ) dissociation limit are specifically investigated. By fitting their binding energy intervals to the non-rigid rotational model, the rotational constant of the long-range 0 u + state is determined. A proportional dependence of the value of the rotational constant on the vibrational quantum number is demonstrated.