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Molecules

Bichromatic Photoassociation Spectroscopy for the Determination of Rotational Constants of Cs2 0 u + Long-Range State below the 6S1/2 + 6P1/2 Asymptote

Jizhou Wu, Jie Ma, Yuqing Li, Wenliang Liu, Peng Li, V. B. Sovkov

Published Aug 31, 2020• 1 citation
Publisher

Abstract

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.

DOI
10.3390/molecules25173963

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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.
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.
We report on a quantitative experimental determination of the rotational constants for the high-lying vibrational levels of the ultracold pure long-range Cesium molecules formed via photoassociation. The scheme relies on a precise reference of frequency difference in a double photoassociation spectroscopy, which is induced by two laser beams based on an acoustic-optical modulator. The rotational constants are obtained by fitting a nonrigid rotor model into the frequency intervals of the neighboring rotational levels deduced from the reference.
The high resolution spectrum of ultracold Cs2 pure long range 0g- state is experimentally measured using modulated trap loss spectroscopic technology. Based on Double photoassociation spectroscopic technique, precise frequency difference reference signals are constructed to accurately calibrate the resonant frequency intervals of the ro-vibrational levels, thus obtaining the relationship between the frequency interval of rotational level and the rotational quantum number. The experimental data are fitted by the non-rigid rotational model, and the molecular rotational constants corresponding to different vibrational levels in the ultracold Cs2 pure long range 0g- state are acquired. The experimental results demonstrate a linear decrease of the rotational constant with the increase of vibrational quantum number, and the linear decreasing rate is -0.41m MHz0.01 MHz.
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.
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.
We report on the photoassociation of cold Cs atoms giving spectroscopy data of the 0 u + long-range molecular state in the asymptotic range of [-6.2, -2.5 cm -1 ] close to the 6S 1/2 +6P 3/2 dissociation limit using photon counting technique. 24 new high-lying vibrational levels of the 0 u + long-range state are identified to lead to the formation of excited molecules in the photoassociation process. Fitting experimental data to improved LeRoy–Bernstein formula, we obtain long-range molecular coefficient with a high precision.