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The Journal of Chemical Physics

Analyzing the photoassociation spectrum of ultracold 85Rb 133Cs molecule in (3)3Σ+ state

Zi-wei Wang, Ziang Li, Xuhui Bai, Ting Gong, Zhonghua Ji, Yanting Zhao, Gao‐Ren Wang

Published Mar 19, 2024• 0 citations
Publisher

Abstract

We establish a theoretical model to analyze the photoassociative spectroscopy of 85Rb 133Cs molecules in the (3)3Σ+ state. The vibrational energy, spin-spin coupling constant, and hyperfine interaction constant of the (3)3Σ+ state are determined based on nine observed vibrational levels. Consequently, the Rydberg-Klein-Rees potential energy curve of the (3)3Σ+ state is obtained and compared with the ab initial potential energy curve. Our model can be adopted to analyze the photoassociative spectroscopy of other heteronuclear alkali-metal diatomic molecules in the (3)3Σ+ state.

DOI
10.1063/5.0182907

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•Jan 1, 2015•1 citation
We establish a theoretical model to analyze the photoassociative spectroscopy of 85Rb 133Cs molecules in the (3)3Σ+ state. The vibrational energy, spin-spin coupling constant, and hyperfine interaction constant of the (3)3Σ+ state are determined based on nine observed vibrational levels. Consequently, the Rydberg-Klein-Rees potential energy curve of the (3)3Σ+ state is obtained and compared with the ab initial potential energy curve. Our model can be adopted to analyze the photoassociative spectroscopy of other heteronuclear alkali-metal diatomic molecules in the (3)3Σ+ state.
Analyzing the photoassociation spectra of ultracold 85^{85}85Rb133^{133}133Cs molecule in (3)3Σ+(3)^3Σ^+(3)3Σ+ state
We establish a theoretical model to analyze the photoassociative (PA) spectroscopy of (3)3Σ+(3)^3Σ^+(3)3Σ+ state of 85^{85}85Rb133^{133}133Cs molecule. The term energy, spin-spin coupling constants and hyperfine interaction constant of nine vibrational levels in the (3)3Σ+(3)^3Σ^+(3)3Σ+ state are determined. Based on the fitted term energy and rotation constant, the potential energy curve of (3)3Σ+(3)^3Σ^+(3)3Σ+ state is obtained by using the RKR method which is compared with the ab initial potential curve.
We present the formation of ultracold (85)Rb(133)Cs molecules in the (5)0(+) electronic state by photoassociation and their detection via resonance-enhanced two-photon ionization. Up to v = 47 vibrational levels including the lowest v = 0 vibrational and lowest J = 0 levels are identified with rotationally resolved high resolution photoassociation spectra. Precise Dunham coefficients are determined for the (5)0(+) state with high accuracy, then the Rydberg-Klein-Rees potential energy curve is derived. The electric dipole moments with respect to the vibrational numbers of the (5)0(+) electronic state of (85)Rb(133)Cs molecule are also measured in the range between 1.9 and 4.8 D. These comprehensive studies on previously unobserved rovibrational levels of the (5)0(+) state are helpful to understand the molecular structure and discover suitable transition pathways for transferring ultracold atoms to deeply bound rovibrational levels of the electronic ground state.
We have examined and identified the excited long-range Hund’s case (c) molecular states of the ten heteronuclear alkali metal diatomic molecules which support bound states and can be probed by ultracold photoassociative spectroscopy. Analytical expressions for the heteronuclear long-range free-bound Franck–Condon factors as a function of the internuclear distance R and the vibrational quantum number v are derived and discussed. The KRb system has considerably stronger excited long-range interactions than any other heteronuclear alkali diatomic molecule and has very favorable Franck–Condon factors for the photoassociation process. The heteronuclear photoassociative spectroscopy will provide spectroscopic measurements of the binary elastic scattering lengths of heteronuclear cold collisions which are the crucial parameters for sympathetic cooling of mixed atomic gases.
We report the observation and analysis of the 3 (3)ΠΩ double-minimum electronic excited state of (39)K(85)Rb. The spin-orbit components (0(+), 0(-), 1, and 2) of this state are investigated based on potentials developed from the available ab initio potential curves. We have assigned the vibrational levels v' = 2-11 of the 3 (3)Π1,2 potentials and v' = 2-12 of the 3(3)Π0(+/-) potential. We compare our experimental observations of the 3 (3)ΠΩ state with predictions based on theoretical potentials. The observations are based on resonance enhanced multiphoton ionization of ultracold KRb in vibrational levels v" = 14-25 of the a (3)Σ(+) state. These a-state ultracold molecules are formed by photoassociation of ultracold (39)K and (85)Rb atoms to the 5(1) state of KRb followed by spontaneous emission to the a state.
Convenient state-selective detection methods are proposed for exploring triplet Rydberg states from the metastable a 3 Σ + state of ultracold KRb molecules by resonance-enhanced two-photon ionization and time-of-flight (TOF) mass spectroscopy. This would allow the first accurate determination of the ionization potential. Particularly suitable resonant intermediate states include the 2 3 Π Ω , 3 3 Σ + and 4 3 Σ + states, and we report spectroscopic studies of these states. For the 2 3 Π Ω state, the spin–orbit components (Ω = 0 + , 0 − , 1 and 2) have been investigated and a shallow long-range state (5(0 + )) at ∼ 9.3 Å has been observed. We compare our observations of these three states with predictions based on ab initio potential energy curves. Such studies may also permit the direct observation of autoionizing resonances leading to efficient formation of low-lying rovibrational levels of the 2 Σ + ground state of KRb + , ideally in the v + = 0, N + = 0 level.
Ultracold atomic physics offers an experimentalist the opportunity to perform sensitive tests and measurements that are not possible at higher temperatures. In this case it allows for access to molecular states, through photoassociation, that are inaccessible to conventional techniques. We use photoassociation to measure quasi-bound levels of the 2 1Σg+ state of 85Rb2 . With these data, we examine a coupling between the short-range Hund’s case (c) 2 (0g+ ) component and the long-range 2 (1g ) state, which corresponds to the 1 1Πg state. A second experiment studies the mechanism of short-range photoassociation and finds our simple model to have strong predictive power. In a third experiment, we photoassociatively form vibrationally excited a 3 Σu+ molecules. We then excite these molecules using a frequency-doubled pulse-amplified CW laser to create low-n long-range Rydberg states of 85Rb2 . Autoionization and ion detection of these states gives high-resolution spectra, which are compared to theoretical potential curves.