Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review A

Accuracy of molecular data in the understanding of ultracold collisions

Olivier Dulieu, Paul S. Julienne, J. Weiner

Published Jan 1, 1994• 15 citations
Publisher

Abstract

We show through close-coupled quantum-scattering calculations that the cross section for fine-structure-changing collisions between excited $^{2}$${\mathit{P}}_{3/2}$ and ground $^{2}$${\mathit{S}}_{1/2}$ A atoms of the same species, where A=Rb or Cs, is very sensitive to the molecular potentials and spin-orbit matrix elements of the alkali-metal-dimer species. Spectroscopic studies of these species are needed to extract accurate parameters. New high-resolution photoassociation spectroscopy of trapped atoms could be used for this purpose.

DOI
10.1103/physreva.49.607

Related papers

Cold collisions of ground- and excited-state alkali-metal atoms

Paul S. Julienne, J. Vigué

This paper examines two collisional mechanisms by which cold alkali-metal atoms can escape from a neutral-atom trap, due to collison of excited- and ground-state atoms. One is fine-structure-changing collisions, by which the atoms are heated by the amount of the fine-structure splitting. The other produces hot ground-state atoms following emission of a red-shifted photon during the course of a collision. A rate expression is obtained that applies to both normal and ultracold temperatures (1 mK). This expression assumes a canonical distribution of initial states, low-intensity excitation, and a semiclassical treatment of the survival probability relative to excited-state decay during the long time of the ultracold collision, and uses fine-structure-changing probabilities found by quantum scattering calculations. The known properties of the attractive molecular states of the alkaline-metal dimers are used to identify and calculate the probabilities for the specific mechanisms. We conclude that the earlier semiclassical analysis by Dashevskaya [Opt. Spectrosk. 46, 423 (1979)] of the fine-structure-changing mechanisms for the various alkali-metal species is qualitatively correct. We present quantum-mechanical calculations of the rate coefficient for fine-structure-changing collisions between ground- and excited-state Cs atoms from 1000 K to 100 \ensuremath{\mu}K. Collision-rate coefficients for the trap-loss processes are calculated for pairs of Li, Na, K, Rb, and Cs atoms at low temperature. There is a wide variation of predicted loss rate among alkali-metal species from the fastest for K and the slowest for Li. Retardation corrections to molecular lifetimes must be taken into account to predict the correct rate coefficients for Na, K, and Rb. Good agreement is obtained with the observed trap loss rate in a Cs trap.

Physical Review A•Oct 1, 1991•183 citations

Photoassociative molecular spectroscopy for atomic radiative lifetimes

Nadia Bouloufa-Maafa, A. Crubellier, Olivier Dulieu

When the atoms of a dimer remain most of the time very far apart, in so-called long-range molecular states, their mutual interaction is ruled by plain atomic properties. The high-resolution spectroscopic study of some molecular excited states populated by photoassociation of cold atoms (photoassociative spectroscopy) gives a good illustration of this property. It provides accurate determinations of atomic radiative lifetimes, which are known to be sensitive tests for atomic calculations. A number of such analyses have been performed up to now, for all stable alkali atoms and for some other atomic species (Ca, Sr, Yb). A systematic review of these determinations is attempted here, with special attention paid to accuracy issues.

arXiv:0902.2846•Physica Scripta•May 1, 2009•22 citations

Experimental Investigation of Ultracold Atom-Molecule Collisions

Peter Frøhlich Staanum, Stephan Kraft, Jörg Lange +2 more

Ultracold collisions between Cs atoms and ${\mathrm{Cs}}_{2}$ dimers in the electronic ground state are observed in an optically trapped gas of atoms and molecules. The ${\mathrm{Cs}}_{2}$ molecules are formed in the triplet ground state by cw photoassociation through the outer well of the ${0}_{g}^{\ensuremath{-}}({P}_{3/2})$ excited electronic state. Inelastic atom-molecule collisions converting internal excitation into kinetic energy lead to a loss of ${\mathrm{Cs}}_{2}$ molecules from the dipole trap. Rate coefficients are determined for collisions involving Cs atoms in either the $F=3$ or $F=4$ hyperfine ground state, and ${\mathrm{Cs}}_{2}$ molecules in either highly vibrationally excited states (${v}^{\ensuremath{'}}=32--47$) or in low vibrational states (${v}^{\ensuremath{'}}=4--6$) of the $a\text{ }^{3}\ensuremath{\Sigma}_{u}^{+}$ triplet ground state. The rate coefficients $\ensuremath{\beta}\ensuremath{\sim}{10}^{\ensuremath{-}10}\text{ }\text{ }{\mathrm{cm}}^{3}/\mathrm{s}$ are found to be largely independent of the vibrational and rotational excitation indicating unitary limited cross sections.

arXiv:physics/0509123•Physical Review Letters•Jan 19, 2006•145 citations

Triatomic Photoassociation in an Ultracold Atom–Molecule Collision

Ahmed A. Elkamshishy, Chris H. Greene

Ultracold collisions of neutral atoms and molecules have been of great interest since experimental advances enabled the cooling and trapping of such species. This study develops a simplified theoretical treatment of a low-energy collision between an alkali atom and a diatomic molecule accompanied by absorption of a photon from an external electromagnetic field. The long-range interaction between the two species is treated, including the atomic spin–orbit interaction. The long-range potential energy curves for the triatomic complex are calculated in realistic detail, while effects of the short-range behavior are mimicked by applying different boundary conditions at the van der Waals length. For neutral colliding species, the leading interaction term is the dipole–dipole interaction. In the case of nonpolar dimers like Cs 2, the second leading term is the quadrupole–quadrupole interaction. However, there is also a strong dipole–quadrupole interaction for dimers with a large permanent dipole moment such as NaCs, making the dipole–quadrupole interaction the second leading term for an atom colliding with a polar dimer. Our applications of the simplified treatment show a higher density of trimer states for a polar dimer compared to the case of a nonpolar dimer like Cs 2 . This is a consequence of the strong quadrupole–dipole coupling between the atom and the dimer dipole moment.

arXiv:2207.02092•The Journal of Physical Chemistry A•Dec 30, 2022•8 citations

High-Precision Calculations of Dispersion Coefficients, Static Dipole Polarizabilities, and Atom-Wall Interaction Constants for Alkali-Metal Atoms

Andrei Derevianko, W. R. Johnson, Marianna S. Safronova +1 more

The van der Waals coefficients for the alkali-metal atoms from Na to Fr interacting in their ground states are calculated using relativistic ab initio methods. The accuracy of the calculations is estimated by also evaluating atomic static electric-dipole polarizabilities and coefficients for the interaction of the atoms with a perfectly conducting wall. The results are in excellent agreement with the latest data from studies of magnetic field induced Feshbach resonances in ultracold collisions of Na and of Rb atoms. For Cs we provide critically needed data for ultracold collision studies.

arXiv:physics/9812028•Physical Review Letters•May 3, 1999•365 citations

Coupled singlet-triplet analysis of two-color cold-atom photoassociation spectra

J. M. M. J. Vogels, R. S. Freeland, Chin‐Chun Tsai +2 more

We describe a method that is well suited to analysis of the bound states of the alkali-metal dimers near their dissociation limit. The method combines inverse perturbation theory, coupled-channel bound-state theory, and the accumulated phase method to treat the short-range part of the molecular potentials. We apply this method to analyze the bound-state energies measured in a two-color photoassociation experiment in an ultracold ${}^{85}\mathrm{Rb}$ gas. This analysis yields information on the interactions between ultracold ${}^{85}\mathrm{Rb}$ atoms that is important to the understanding of ultracold Rb collisions and Bose-Einstein condensation.

Physical Review A•Mar 8, 2000•23 citations
We show through close-coupled quantum-scattering calculations that the cross section for fine-structure-changing collisions between excited ^{2}$${\mathit{P}}_{3/2} and ground ^{2}$${\mathit{S}}_{1/2} A atoms of the same species, where A=Rb or Cs, is very sensitive to the molecular potentials and spin-orbit matrix elements of the alkali-metal-dimer species. Spectroscopic studies of these species are needed to extract accurate parameters. New high-resolution photoassociation spectroscopy of trapped atoms could be used for this purpose.
This paper examines two collisional mechanisms by which cold alkali-metal atoms can escape from a neutral-atom trap, due to collison of excited- and ground-state atoms. One is fine-structure-changing collisions, by which the atoms are heated by the amount of the fine-structure splitting. The other produces hot ground-state atoms following emission of a red-shifted photon during the course of a collision. A rate expression is obtained that applies to both normal and ultracold temperatures (1 mK). This expression assumes a canonical distribution of initial states, low-intensity excitation, and a semiclassical treatment of the survival probability relative to excited-state decay during the long time of the ultracold collision, and uses fine-structure-changing probabilities found by quantum scattering calculations. The known properties of the attractive molecular states of the alkaline-metal dimers are used to identify and calculate the probabilities for the specific mechanisms. We conclude that the earlier semiclassical analysis by Dashevskaya [Opt. Spectrosk. 46, 423 (1979)] of the fine-structure-changing mechanisms for the various alkali-metal species is qualitatively correct. We present quantum-mechanical calculations of the rate coefficient for fine-structure-changing collisions between ground- and excited-state Cs atoms from 1000 K to 100 \ensuremath{\mu}K. Collision-rate coefficients for the trap-loss processes are calculated for pairs of Li, Na, K, Rb, and Cs atoms at low temperature. There is a wide variation of predicted loss rate among alkali-metal species from the fastest for K and the slowest for Li. Retardation corrections to molecular lifetimes must be taken into account to predict the correct rate coefficients for Na, K, and Rb. Good agreement is obtained with the observed trap loss rate in a Cs trap.
When the atoms of a dimer remain most of the time very far apart, in so-called long-range molecular states, their mutual interaction is ruled by plain atomic properties. The high-resolution spectroscopic study of some molecular excited states populated by photoassociation of cold atoms (photoassociative spectroscopy) gives a good illustration of this property. It provides accurate determinations of atomic radiative lifetimes, which are known to be sensitive tests for atomic calculations. A number of such analyses have been performed up to now, for all stable alkali atoms and for some other atomic species (Ca, Sr, Yb). A systematic review of these determinations is attempted here, with special attention paid to accuracy issues.
Ultracold collisions between Cs atoms and Cs2{\mathrm{Cs}}_{2}Cs2​ dimers in the electronic ground state are observed in an optically trapped gas of atoms and molecules. The Cs2{\mathrm{Cs}}_{2}Cs2​ molecules are formed in the triplet ground state by cw photoassociation through the outer well of the ${0}_{g}^{\ensuremath{-}}({P}_{3/2})$ excited electronic state. Inelastic atom-molecule collisions converting internal excitation into kinetic energy lead to a loss of Cs2{\mathrm{Cs}}_{2}Cs2​ molecules from the dipole trap. Rate coefficients are determined for collisions involving Cs atoms in either the F=3F=3F=3 or F=4F=4F=4 hyperfine ground state, and Cs2{\mathrm{Cs}}_{2}Cs2​ molecules in either highly vibrationally excited states (${v}^{\ensuremath{'}}=32--47$) or in low vibrational states (${v}^{\ensuremath{'}}=4--6$) of the $a\text{ }^{3}\ensuremath{\Sigma}_{u}^{+}$ triplet ground state. The rate coefficients $\ensuremath{\beta}\ensuremath{\sim}{10}^{\ensuremath{-}10}\text{ }\text{ }{\mathrm{cm}}^{3}/\mathrm{s}$ are found to be largely independent of the vibrational and rotational excitation indicating unitary limited cross sections.
Ultracold collisions of neutral atoms and molecules have been of great interest since experimental advances enabled the cooling and trapping of such species. This study develops a simplified theoretical treatment of a low-energy collision between an alkali atom and a diatomic molecule accompanied by absorption of a photon from an external electromagnetic field. The long-range interaction between the two species is treated, including the atomic spin–orbit interaction. The long-range potential energy curves for the triatomic complex are calculated in realistic detail, while effects of the short-range behavior are mimicked by applying different boundary conditions at the van der Waals length. For neutral colliding species, the leading interaction term is the dipole–dipole interaction. In the case of nonpolar dimers like Cs 2, the second leading term is the quadrupole–quadrupole interaction. However, there is also a strong dipole–quadrupole interaction for dimers with a large permanent dipole moment such as NaCs, making the dipole–quadrupole interaction the second leading term for an atom colliding with a polar dimer. Our applications of the simplified treatment show a higher density of trimer states for a polar dimer compared to the case of a nonpolar dimer like Cs 2 . This is a consequence of the strong quadrupole–dipole coupling between the atom and the dimer dipole moment.
The van der Waals coefficients for the alkali-metal atoms from Na to Fr interacting in their ground states are calculated using relativistic ab initio methods. The accuracy of the calculations is estimated by also evaluating atomic static electric-dipole polarizabilities and coefficients for the interaction of the atoms with a perfectly conducting wall. The results are in excellent agreement with the latest data from studies of magnetic field induced Feshbach resonances in ultracold collisions of Na and of Rb atoms. For Cs we provide critically needed data for ultracold collision studies.
We describe a method that is well suited to analysis of the bound states of the alkali-metal dimers near their dissociation limit. The method combines inverse perturbation theory, coupled-channel bound-state theory, and the accumulated phase method to treat the short-range part of the molecular potentials. We apply this method to analyze the bound-state energies measured in a two-color photoassociation experiment in an ultracold 85Rb{}^{85}\mathrm{Rb}85Rb gas. This analysis yields information on the interactions between ultracold 85Rb{}^{85}\mathrm{Rb}85Rb atoms that is important to the understanding of ultracold Rb collisions and Bose-Einstein condensation.