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Experimental Studies of LiRb: Spectroscopy and Ultracold Molecule Formation by Photoassociation

Sourav Dutta

Published Jan 1, 2013• 4 citations
OpenAlex

Abstract

Heteronuclear polar molecules have recently attracted enormous attention owing to their ground state having a large electric dipole moment. The long range anisotropic dipole-dipole interaction in such systems is the basis for a variety of applications including quantum computing, precision measurements, ultracold chemistry and quantum simulations. Heteronuclear bi-alkali molecules, only a small subset of polar molecules, have received special attention mainly because the constituent alkali atoms are easy to laser cool and can be relatively easily associated to form molecules at ultracold temperatures. Our choice, the LiRb molecule, is motivated by the relatively high dipole moment (4.1 Debye) of the LiRb molecule in its rovibronic ground state. In this thesis, we study the LiRb molecule using laser spectroscopy and report, for the first time, the production of ultracold LiRb molecules by photoassociation (PA). The LiRb molecule is the least studied among all bi-alkali molecules and the first spectroscopic measurements on hot vapor phase LiRb molecules were reported only in 2011. We describe these measurements and their significance in chapter 2, after a brief introduction to the field of ultracold polar molecules in chapter 1. In chapter 3, we discuss our apparatus for simultaneous cooling and trapping of Li and Rb atoms in a dual-species magneto-optical trap (MOT) and report the measurement of interspecies collision-induced losses. In chapter 4, we describe the production of ultracold LiRb molecules in excited electronic states by photoassociation (PA). We report the measurements of the C6 coefficients for the Li (2s 2S1/2) + Rb (5p 2P1/2) and the Li (2s 2S1/2) + Rb (5p 2P3/2) asymptotes. We find a molecule formation rate (PLiRb) as high as 3.5x107 s-1 and a PA rate coefficient (KPA) as high as 1.3x10-10 cm3/s, the highest among heteronuclear bi-alkali molecules. In chapter 5, we discuss results on two-photon PA and we conclude, in chapter 6, with a road roadmap of future experiments for the production and detection of ultracold LiRb molecules in their rovibronic ground state.

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Photoassociation of ultracold LiRb * molecules: Observation of high efficiency and unitarity-limited rate saturation

Sourav Dutta, John Lorenz, Adeel Altaf +2 more

We report the production of ultracold heteronuclear $^{7}\mathrm{Li}^{85}\mathrm{Rb}$ molecules in excited electronic states by photoassociation (PA) of ultracold $^{7}\mathrm{Li}$ and $^{85}\mathrm{Rb}$ atoms. PA is performed in a dual-species $^{7}\mathrm{Li}$-$^{85}\mathrm{Rb}$ magneto-optical trap (MOT) and the PA resonances are detected using trap loss spectroscopy. We identify several strong PA resonances below the Li (2$s$ ${}^{2}$${S}_{1/2}$) + Rb (5$p$ ${}^{2}{P}_{3/2}$) asymptote and experimentally determine the long range ${C}_{6}$ dispersion coefficients. We find a molecule formation rate (${P}_{\mathrm{LiRb}}$) of 3.5 \ifmmode\times\else\texttimes\fi{} 10${}^{7}$ s${}^{\ensuremath{-}1}$ and a PA rate coefficient (${K}_{\mathrm{PA}}$) of 1.3 \ifmmode\times\else\texttimes\fi{} 10${}^{\ensuremath{-}10}$ cm${}^{3}$/s, the highest among heteronuclear bi-alkali-metal molecules. At large PA laser intensity we observe the saturation of the PA rate coefficient (${K}_{\mathrm{PA}}$) close to the theoretical value at the unitarity limit.

arXiv:1311.6297•Physical Review A•Feb 19, 2014•39 citations

Spectroscopy of ultracold LiRb molecules using ionization detection

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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.

•Jan 1, 2014•2 citations

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Production of ultracold heteronuclear KRb molecules

Dajun Wang

This thesis describes the spectroscopy work on ultracold 39K 85Rb molecules as part of our effort towards producing ground-state ultracold polar molecules. ^ The starting points of our experiment are laser cooled and trapped K and Rb atoms in dual-species MOTs and the molecule formation method is photoassociation (PA). A fraction of the PA-produced excited-state molecules can spontaneously emit to the two lowest electronic states, the X 1Σ + state and the a 3Σ + state, to form high vibrational level molecules. In order to develop a population transfer scheme to make deeply bound molecules, we have studied the spectroscopy of KRb in several steps. Besides the PA step, we have also carried out a state-selective detection experiment to study the population distribution of the high vibrational level molecules formed via spontaneous emission. The detection method is pulsed-laser based ion time-of-flight mass spectroscopy. Due to the linewidth limitations of the pulsed laser, this detection method can only resolve vibrational structures. A cw laser induced ion depletion spectroscopy technique has been developed in order to obtain rotational resolution. Using this ion depletion method, we have studied a possible stimulated Raman transfer scheme via the 3 1Σ+ state. To this end, we have obtained all the spectroscopic information required to produce deeply bound KRb molecules in a single vibrational and rotational level. ^ Several other spectroscopic studies using the high vibrational level ultracold molecules are also discussed. ^

•Jan 1, 2007•0 citations

Structure, formation, and interactions of ultracold polar molecules

Johannes Deiglmayr

In this thesis properties of ultracold alkali dimers are studied both theoretically and experimentally. In the first, theoretical, part, the prospects for the formation of ultracold LiCs dimers in deeply bound vibrational levels using photoassociation (PA) are investigated. Furthermore a previous systematic investigation of the structure of all alkali dimers is extended by the ab initio calculation of static dipole polarizabilities. An extensive comparison with other published results supports the reliability of the chosen method. Based on these results an experimental scheme for the creation of an sample of oriented ultracold dipolar molecules is developed. In the second, experimental part the formation of LiCs ground state molecules by PA is investigated. PA spectroscopy is used to improve the accuracy of the potential energy curve for the B1P and the value of the dissociation energy of the X1S+ state significantly. The rovibrational distribution of ground state molecules is probed in a combination of resonance-enhanced multi-photon ionization and depletion spectroscopy. A simple scheme is found to form ultracold polar LiCs molecules in the absolute ground state X1S+,v''=0,J''=0. In a quasi-electrostatic trap created by a CO2 laser, LiCs molecules are formed and stored. A lifetime of 24(3)s, limited by collisions with background gas, is observed and rate coefficients for inelastic collisions between LiCs in high vibrational states and Cs atoms are determined. The long storage time facilitates the observation of radiative decay of polar molecules towards lower vibrational levels.

•Jan 1, 2009•2 citations
Heteronuclear polar molecules have recently attracted enormous attention owing to their ground state having a large electric dipole moment. The long range anisotropic dipole-dipole interaction in such systems is the basis for a variety of applications including quantum computing, precision measurements, ultracold chemistry and quantum simulations. Heteronuclear bi-alkali molecules, only a small subset of polar molecules, have received special attention mainly because the constituent alkali atoms are easy to laser cool and can be relatively easily associated to form molecules at ultracold temperatures. Our choice, the LiRb molecule, is motivated by the relatively high dipole moment (4.1 Debye) of the LiRb molecule in its rovibronic ground state. In this thesis, we study the LiRb molecule using laser spectroscopy and report, for the first time, the production of ultracold LiRb molecules by photoassociation (PA). The LiRb molecule is the least studied among all bi-alkali molecules and the first spectroscopic measurements on hot vapor phase LiRb molecules were reported only in 2011. We describe these measurements and their significance in chapter 2, after a brief introduction to the field of ultracold polar molecules in chapter 1. In chapter 3, we discuss our apparatus for simultaneous cooling and trapping of Li and Rb atoms in a dual-species magneto-optical trap (MOT) and report the measurement of interspecies collision-induced losses. In chapter 4, we describe the production of ultracold LiRb molecules in excited electronic states by photoassociation (PA). We report the measurements of the C6 coefficients for the Li (2s 2S1/2) + Rb (5p 2P1/2) and the Li (2s 2S1/2) + Rb (5p 2P3/2) asymptotes. We find a molecule formation rate (PLiRb) as high as 3.5x107 s-1 and a PA rate coefficient (KPA) as high as 1.3x10-10 cm3/s, the highest among heteronuclear bi-alkali molecules. In chapter 5, we discuss results on two-photon PA and we conclude, in chapter 6, with a road roadmap of future experiments for the production and detection of ultracold LiRb molecules in their rovibronic ground state.
We report the production of ultracold heteronuclear 7Li85Rb^{7}\mathrm{Li}^{85}\mathrm{Rb}7Li85Rb molecules in excited electronic states by photoassociation (PA) of ultracold 7Li^{7}\mathrm{Li}7Li and 85Rb^{85}\mathrm{Rb}85Rb atoms. PA is performed in a dual-species 7Li^{7}\mathrm{Li}7Li-85Rb^{85}\mathrm{Rb}85Rb magneto-optical trap (MOT) and the PA resonances are detected using trap loss spectroscopy. We identify several strong PA resonances below the Li (2sss 2{}^{2}2S1/2{S}_{1/2}S1/2​) + Rb (5ppp 2P3/2{}^{2}{P}_{3/2}2P3/2​) asymptote and experimentally determine the long range C6{C}_{6}C6​ dispersion coefficients. We find a molecule formation rate (PLiRb{P}_{\mathrm{LiRb}}PLiRb​) of 3.5 \ifmmode\times\else\texttimes\fi{} 107{}^{7}7 s${}^{\ensuremath{-}1}$ and a PA rate coefficient (KPA{K}_{\mathrm{PA}}KPA​) of 1.3 \ifmmode\times\else\texttimes\fi{} 10${}^{\ensuremath{-}10}$ cm3{}^{3}3/s, the highest among heteronuclear bi-alkali-metal molecules. At large PA laser intensity we observe the saturation of the PA rate coefficient (KPA{K}_{\mathrm{PA}}KPA​) close to the theoretical value at the unitarity limit.
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.
We report the production of ultracold 7 Li 85 Rb molecules by photoassociation (PA) below the Li (2 s 2 S 1/2 ) + Rb(5 p 2 P 1/2 ) asymptote. We perform PA spectroscopy in a dual-species 7 Li- 85 Rb magneto-optical trap (MOT) and detect the PA resonances using trap loss spectroscopy. We observe several strong PA resonances corresponding to the last few bound states, assign the lines and derive the long-range C 6 dispersion coefficients for the Li (2 s 2 S 1/2 ) + Rb(5 p 2 P 1/2 ) asymptote. We also report an excited-state molecule formation rate of and a PA rate coefficient of , which are both among the highest observed for heteronuclear bi-alkali molecules. These suggest that PA is a promising route for the creation of ultracold ground-state LiRb molecules.
This thesis describes the spectroscopy work on ultracold 39K 85Rb molecules as part of our effort towards producing ground-state ultracold polar molecules. ^ The starting points of our experiment are laser cooled and trapped K and Rb atoms in dual-species MOTs and the molecule formation method is photoassociation (PA). A fraction of the PA-produced excited-state molecules can spontaneously emit to the two lowest electronic states, the X 1Σ + state and the a 3Σ + state, to form high vibrational level molecules. In order to develop a population transfer scheme to make deeply bound molecules, we have studied the spectroscopy of KRb in several steps. Besides the PA step, we have also carried out a state-selective detection experiment to study the population distribution of the high vibrational level molecules formed via spontaneous emission. The detection method is pulsed-laser based ion time-of-flight mass spectroscopy. Due to the linewidth limitations of the pulsed laser, this detection method can only resolve vibrational structures. A cw laser induced ion depletion spectroscopy technique has been developed in order to obtain rotational resolution. Using this ion depletion method, we have studied a possible stimulated Raman transfer scheme via the 3 1Σ+ state. To this end, we have obtained all the spectroscopic information required to produce deeply bound KRb molecules in a single vibrational and rotational level. ^ Several other spectroscopic studies using the high vibrational level ultracold molecules are also discussed. ^
In this thesis properties of ultracold alkali dimers are studied both theoretically and experimentally. In the first, theoretical, part, the prospects for the formation of ultracold LiCs dimers in deeply bound vibrational levels using photoassociation (PA) are investigated. Furthermore a previous systematic investigation of the structure of all alkali dimers is extended by the ab initio calculation of static dipole polarizabilities. An extensive comparison with other published results supports the reliability of the chosen method. Based on these results an experimental scheme for the creation of an sample of oriented ultracold dipolar molecules is developed. In the second, experimental part the formation of LiCs ground state molecules by PA is investigated. PA spectroscopy is used to improve the accuracy of the potential energy curve for the B1P and the value of the dissociation energy of the X1S+ state significantly. The rovibrational distribution of ground state molecules is probed in a combination of resonance-enhanced multi-photon ionization and depletion spectroscopy. A simple scheme is found to form ultracold polar LiCs molecules in the absolute ground state X1S+,v''=0,J''=0. In a quasi-electrostatic trap created by a CO2 laser, LiCs molecules are formed and stored. A lifetime of 24(3)s, limited by collisions with background gas, is observed and rate coefficients for inelastic collisions between LiCs in high vibrational states and Cs atoms are determined. The long storage time facilitates the observation of radiative decay of polar molecules towards lower vibrational levels.