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Journal of the Physical Society of Japan

Line Shape Analysis of Ultracold Heteronuclear Molecular Photoassociation Spectroscopy by Resonance-Enhanced Two-Photon Ionization

Jinpeng Yuan, Zhonghua Ji, Yanting Zhao, Yan Yang, Yonggang Yang, Liantuan Xiao, Suotang Jia

Published Jul 12, 2013• 1 citation
Publisher

Abstract

Resonance-enhanced two-photon ionization (RETPI) is a powerful tool in ultracold molecular photoassociation spectroscopy measurement. Using the RETPI, the line shape of ultracold RbCs molecular photoassociation spectroscopy, which contains intensity and full width at half maximum, is measured and analyzed systematically with varied photoassociation laser intensity and ionization laser energy. The saturation of photoassociation spectroscopy at a high ionization laser energy is observed and the suppression phenomenon is observed at high photoassociation laser intensity. The saturation intensity of RbCs molecular photoassociation, the linewidths of excited state molecules in different rovibrational levels at zero photoassociation laser intensity, and two-photon ionization efficiency have been derived from the line shape of photoassociation spectroscopy. The line shape analysis of photoassociation spectroscopy is important for precision spectroscopic analysis.

DOI
10.7566/jpsj.82.084301

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Resonance-enhanced two-photon ionization (RETPI) is a powerful tool in ultracold molecular photoassociation spectroscopy measurement. Using the RETPI, the line shape of ultracold RbCs molecular photoassociation spectroscopy, which contains intensity and full width at half maximum, is measured and analyzed systematically with varied photoassociation laser intensity and ionization laser energy. The saturation of photoassociation spectroscopy at a high ionization laser energy is observed and the suppression phenomenon is observed at high photoassociation laser intensity. The saturation intensity of RbCs molecular photoassociation, the linewidths of excited state molecules in different rovibrational levels at zero photoassociation laser intensity, and two-photon ionization efficiency have been derived from the line shape of photoassociation spectroscopy. The line shape analysis of photoassociation spectroscopy is important for precision spectroscopic analysis.
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 have investigated photoassociative formation of RbCs molecules in the ${(2)}^{\phantom{\rule{0.16em}{0ex}}3}\phantom{\rule{-0.16em}{0ex}}\ensuremath{\Pi}$ excited state correlated to v=8v=8v=8, (5)0+(5){0}^{+}(5)0+ vibrational level in detail. The metastable ground-state RbCs molecules formed by spontaneous decay are ionized by pulsed dye laser through resonance-enhanced two-photon ionization. A rate equation of the photoionization process is introduced to explain the dependence of RbCs+{}^{+}+ molecular ion intensity on the ionization laser intensity. The saturation effect of molecular ion intensity appears as the photoassociation laser intensity increases. The rotational constant and centrifugal distortion constant are derived to be 0.01304 cm${}^{\ensuremath{-}1}$ and 0.000015 cm${}^{\ensuremath{-}1}$ from the photoassociation spectrum with a high sensitivity, respectively. The measured electric dipole moment of the observed $(2){\phantom{\rule{0.16em}{0ex}}}^{3}\phantom{\rule{-0.16em}{0ex}}\ensuremath{\Pi}$ state RbCs molecules is 4.7(6) D by Stark effect in static electric field.
We derive ultracold atom-atom photoassociation line shapes valid for intense light fields and investigate laser power effects in sodium and rubidium photoassociation to the purely long-range ${0}_{g}^{\ensuremath{-}}$ symmetry state. We consider intensities up to a few hundreds W/cm2,{\mathrm{W}/\mathrm{c}\mathrm{m}}^{2},W/cm2, a strongly saturating intensity for typical transitions of experimental interest. For these intensities the ${0}_{g}^{\ensuremath{-}}$ rotational spectrum is still well resolved; however, it is essential to couple the photoassociation resonance to both s- and d-wave ground-state channels. A low-energy d-wave shape resonance can have a profound effect on the line shape. Understanding the line shape is essential for precision spectroscopic analysis and could improve the extraction of ground-state scattering properties such as scattering lengths.
Ultracold polar RbCs molecules are produced via photoassociation in a laser-cooled mixture of 85 Rb and 133 Cs atoms. The a 3 Σ + state molecules which decay from electronically excited (2)0 − state RbCs molecules are detected by resonance-enhanced two-photon ionization. The new rovibrational levels ( v = 189, 190) in the (2)0 − state are also observed, which exist in theory and have not been observed in experiments yet. The corresponding rotational constants are measured by photoassociation spectroscopy, which are consistent with theoretical calculations using a nonrigid rotor model.
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We present spectroscopic studies of ultracold LiRb molecules using ionization detection. The molecules are created by cooling and trapping Li and Rb atoms in overlapping magneto-optical traps (MOTs) and using light resonant with a free-bound transition to create weakly bound excited state molecules in a process known as photoassociation (PA). We explore weakly bound vibrational levels of LiRb with PA spectroscopy using ionization detection and, where possible, compare our results with earlier measurements performed in our lab using trap-loss spectroscopy. In addition, we also probe vibrational levels of the ground triplet electronic state and excited electronic states using resonantly enhanced multiphoton ionization (REMPI) spectroscopy. We identify several vibrational levels of the α3Σ+, (3)3ΠΩ and (4)3Σ + states and compare our observations with theoretical calculations. As LiRb is one of the least studied heteronuclear diatomic molecules, these studies are aimed towards exploring the molecular structure. The spectroscopic work is also in line with the long-term project goals of transferring ultracold LiRb molecules into the lowest rotational and vibrational levels of the ground singlet electronic state. Molecules in this rovibronic ground state possess a large electric dipole moment, which is essential for application of ultracold molecules in various quantum computation schemes. The rovibronic ground state will also be an ideal starting point for investigating molecular entangled states.