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The Journal of Chemical Physics

The determination of potential energy curve and dipole moment of the (5)0+ electronic state of 85Rb133Cs molecule by high resolution photoassociation spectroscopy

Jinpeng Yuan, Yanting Zhao, Zhonghua Ji, Zhonghao Li, Jin‐Tae Kim, Liantuan Xiao, Suotang Jia

Published Dec 9, 2015• 11 citations
Publisher

Abstract

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.

DOI
10.1063/1.4936914

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Journal of Physics B Atomic Molecular and Optical Physics•Sep 25, 2006•52 citations
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 present high resolution photoassociation spectroscopy of RbCs molecules in (2)0(+) long-range state below the Rb(5S1/2) + Cs(6P1/2) asymptote and derive the corresponding C6 coefficient, which is used to revise the potential energy curves. The excited state molecules are produced in a dual-species dark spontaneous force optical trap and detected by ionizing ground state molecules after spontaneous decay, using a high sensitive time-of-flight mass spectrum. With the help of resonance-enhanced two-photon ionization technique, we obtain considerable high resolution photoassociation spectrum with rovibrational states, some of which have never been observed before. By applying the LeRoy-Bernstein method, we assign the vibrational quantum numbers and deduce C6 coefficient, which agrees with the theoretical value of A(1)Σ(+) state correlated to Rb(5S1/2) + Cs(6P1/2) asymptote. The obtained C6 coefficient is used to revise the long-range potential energy curve for (2)0(+) state, which possesses unique A - b mixing characteristic and can be a good candidate for the production of absolutely ground state molecule.
The formation of ultracold metastable RbCs molecules is observed in a double species magneto-optical trap through photoassociation below the 85 Rb(5S 1/2 ) + 133 Cs(6P 3/2 ) dissociation limit followed by spontaneous emission. The molecules are detected by resonance enhanced two-photon ionization. Using accurate quantum chemistry calculations of the potential energy curves and transition dipole moment, we interpret the observed photoassociation process as occurring at short internuclear distance, in contrast with most previous cold atom photoassociation studies. The vibrational levels excited by photoassociation belong to the 5th 0 + or the 4th 0 − electronic states correlated to the Rb(5P 1/2, 3/2 ) + Cs(6S 1/2 ) dissociation limit. The computed vibrational distribution of the produced molecules shows that they are stabilized in deeply bound vibrational states of the lowest triplet state. We also predict that a noticeable fraction of molecules is produced in the lowest level of the electronic ground state.
We investigate the production of ultracold ground state X 1 σ + (v = 0) RbCs molecules in the lowest vibrational level via short-range photoassociation followed by spontaneous emission. The starting point is the laser cooled 85 Rb and 133 Cs atoms in a dual species, forced dark magneto-optical trap. The special intermediate level (5)0 + (v = 10) correlated to the (2) 3 π electric state is achieved by the photoassociation process. The formed ground state X 1 σ + (v = 0) molecule is resonantly excited to the 2 1 π intermediate state by a 651 nm pulse laser and is ionized by a 532 nm pulse laser and then detected by the time-of-flight mass spectrum. Saturation of the photoionization spectroscopy at large ionization laser energy is observed and the ionization efficiency is obtained from the fitting. The production of ultracold ground state 85 Rb 133 Cs molecules is facilitative for the further research about the manipulation of ultracold molecules in the rovibrational ground state.
We report the formation of ultracold (7)Li(85)Rb molecules in the a(3)Σ(+) electronic state by photoassociation (PA) and their detection via resonantly enhanced multiphoton ionization (REMPI). With our dual-species Li and Rb magneto-optical trap apparatus, we detect PA resonances with binding energies up to ∼62 cm(-1) below the (7)Li 2s (2)S1/2 + (85)Rb 5p (2)P1/2 asymptote. In addition, we use REMPI spectroscopy to probe the a(3)Σ(+) state and excited electronic 3(3)Π and 4(3)Σ(+) states and identify a(3)Σ(+) (v″ = 7-13), 3(3)Π (vΠ' = 0-10), and 4(3)Σ(+) (vΣ' = 0-5) vibrational levels. Our line assignments agree well with ab initio calculations. These preliminary spectroscopic studies on previously unobserved electronic states are crucial to discovering transition pathways for transferring ultracold LiRb molecules created via PA to deeply bound rovibrational levels of the electronic ground state.
We recently reported the formation of ultracold LiCs molecules in the rovibrational ground state X1sigma+, v" = 0,J" = 0 (J. Deiglmayr et al., Phys. Rev. Lett., 2008, 101, 133004). Here we discuss details of the experimental setup and present a thorough analysis of the photoassociation step including the photoassociation line shape. We predict the distribution of produced ground state molecules using accurate potential energy curves combined with an ab initio dipole transition moment and compare this prediction with experimental ionization spectra. Additionally we improve the value of the dissociation energy for the X1sigma+ state by high resolution spectroscopy of the vibrational ground state.
We form ultracold ground-state Rb 2 molecules by photoassociating pairs of atoms in a magneto-optical trap into the 0 u + state, which decays radiatively into high vibrational levels of the X 1 Σ g + state. Sensitive and vibrationally state-selective detection is achieved by means of resonantly-enhanced two-photon ionization with a pulsed laser. Frequency scans of the detection laser reveal a long vibrational progression to a previously unobserved electronic excited state, which we identify as the 2 1 Σ u + state. Most of its vibrational spectrum is in excellent agreement with predictions based on ab initio potentials, although the lowest vibrational levels exhibit strong perturbative mixing with the triplet 2 3 Π u state. The detection method reported here, with minor variations, should be effective for the entire potential well of the X state. In this work no transitions are observed from vibrational levels above v = 118, but this turns out to be a limitation not of the detection method but rather of the photoassociative formation scheme, due to re-excitation of the highest- v levels by the same photoassociation laser that produces them.