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The Journal of Physical Chemistry Letters

Experimental Determination of the Rotational Constants of High-Lying Vibrational Levels of Ultracold Cs2 in the 0g– Purely Long-Range State

Jie Ma, Jizhou Wu, Gang Chen, Qunchao Fan, Hao Feng, Xingcan Dai, Weiguo Sun, Liantuan Xiao, Suotang Jia

Published Oct 10, 2013• 13 citations
Publisher

Abstract

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.

DOI
10.1021/jz401769z

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Light-induced frequency shifts for the lowest vibrational levels of ultracold Cs2 in the molecular pure long-range 0g−0_g^-0g−​ state
The light-induced frequency shift (LIFS) of ultracold molecular ro-vibrational levels originates from the strong coupling of the atomic-scattering state and the bound-molecular state. In this paper, we present our experimental determination of the LIFSs of the lowest vibrational levels ( ν = 0, 1) in the purely long-range 0g−0_g^-0g−​ state of ultracold cesium molecules. A high-resolution double photoassociation spectroscopy is developed, which serves as frequency ruler to measure the frequency shifts of the lowest molecular levels for Cs 2 . The experimental results are qualitatively consistent with the theoretical expectations.
We experimentally present a technique for sensitively determining the laser-induced frequency shifts of the long-range molecular vibrational and rotational levels. The scheme relies on an optical frequency shifter, leading to two laser beams with a precise and adjustable frequency interval. A series of photoassociation spectra are recorded with both beams inducing molecular lines, whose peak separation provides an accurate frequency ruler to measure the frequency shifts of cesium molecular levels, which have not yet been observed in previous reports. The data are compared to theoretical predictions and show a good agreement.
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.