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Journal of Quantitative Spectroscopy and Radiative Transfer

Resonance enhanced two-photon ionization spectrum of ultracold 85Rb133Cs molecules in (2)1Π1←X1Σ+ transitions

Zhonghua Ji, Ting Gong, Yanting Zhao, Chuanliang Li, Liantuan Xiao, Suotang Jia

Published Jul 13, 2020• 3 citations
Publisher
DOI
10.1016/j.jqsrt.2020.107215

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We investigate the production of cold 85Rb133Cs molecules in the lowest vibronic level of the ground electronic state via the B1Π1 short-range state. The photoassociation (PA) spectra of the B1Π1 state, including newly observed transition to 2 vibronic levels, are obtained by high sensitivity time-of-flight mass spectrometry. Based on these PA spectra, the harmonic and anharmonic constants of vibronic states are obtained, resulting in predicted vibronic energies with an uncertainty of 1–2 cm−1. The B1Π1 (v = 3) state is found to have the maximum production rate for ground-state molecules with a value of 3(1) × 104 s−1, which is 3 times larger than the value via the previously studied 23Π0+ (v = 10, J = 0) state with two-photon cascade decay. The populations of J = 0, 1, and 2 rotational levels of X1Σ+ (v = 0) state molecules formed via the B1Π1 (v = 3, J = 1) state are measured to be around 20%, 40%, and 20%. To quantify the coupling strength between the B1Π1 (v = 3) state and X1Σ+ (v = 0) state, the transition dipole moment between them is measured to be 7.2(2) × 10−3ea0, which is also 3 times larger than the value between the 23Π0+(v=10) state and X1Σ+ (v = 0) state, meaning the B1Π1 (v = 3) state has a stronger coupling with the X1Σ+ (v = 0) state. Our detailed measurements provide relevant parameters for investigation on direct stimulated Raman adiabatic passage transfer between the atomic scattering state and molecular bound state for 85Rb133Cs molecules.

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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.

Journal of Physics B Atomic Molecular and Optical Physics•Sep 25, 2006•52 citations
We investigate the production of cold 85Rb133Cs molecules in the lowest vibronic level of the ground electronic state via the B1Π1 short-range state. The photoassociation (PA) spectra of the B1Π1 state, including newly observed transition to 2 vibronic levels, are obtained by high sensitivity time-of-flight mass spectrometry. Based on these PA spectra, the harmonic and anharmonic constants of vibronic states are obtained, resulting in predicted vibronic energies with an uncertainty of 1–2 cm−1. The B1Π1 (v = 3) state is found to have the maximum production rate for ground-state molecules with a value of 3(1) × 104 s−1, which is 3 times larger than the value via the previously studied 23Π0+ (v = 10, J = 0) state with two-photon cascade decay. The populations of J = 0, 1, and 2 rotational levels of X1Σ+ (v = 0) state molecules formed via the B1Π1 (v = 3, J = 1) state are measured to be around 20%, 40%, and 20%. To quantify the coupling strength between the B1Π1 (v = 3) state and X1Σ+ (v = 0) state, the transition dipole moment between them is measured to be 7.2(2) × 10−3ea0, which is also 3 times larger than the value between the 23Π0+(v=10) state and X1Σ+ (v = 0) state, meaning the B1Π1 (v = 3) state has a stronger coupling with the X1Σ+ (v = 0) state. Our detailed measurements provide relevant parameters for investigation on direct stimulated Raman adiabatic passage transfer between the atomic scattering state and molecular bound state for 85Rb133Cs molecules.
One- and two-color resonance-enhanced two-photon ionization (RETPI) is used to detect ultracold ground-state RbCs molecules which are formed via short-range photoassociation from laser-cooled atoms. The transition from the X1Σ+(v = 0) state to the 21Π(v = 10) state of ultracold RbCs molecules shows the consistence of one- and two-color RETPI. A multi-photon photoionization rate model is introduced to interpret the dependence of molecular ion intensity on photoionized laser energy, and can be used to verify the photoionization scheme. This photoionization rate model can be expanded to multi-color photoionization for all kinds of atoms and molecules, which is a powerful method of determining the photoionization scheme.
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.