Physical Review A

Cold magnetically trapped 2Dg scandium atoms. II. Scattering dynamics

Tijs Karman, Gerrit C. Groenenboom

Published Nov 5, 2014• 6 citations

Abstract

The binary collision dynamics of ${}^{2}{D}_{g,3/2}$ ground state scandium atoms is studied from first principles. We employ 30 coupled diabatic ab initio potentials in a coupled-channels study of the scattering dynamics of cold and ultracold scandium atoms in external magnetic fields. Due to the long-ranged magnetic dipolar interaction, the field dependence of the cross section does not follow the threshold laws derived by Volpi and Bohn [Phys. Rev. A 65, 052712 (2002)]. In the field-free case, the near-threshold cross section is independent of the collision energy, and hence the cross section does not follow the well-established Wigner threshold laws. The observed threshold behavior is explained in the Born approximation. For energies above $1\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}$, inelastic collisions are driven by the anisotropic nonrelativistic electronic interaction. For energies below $100\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}$, the ratio of elastic-to-inelastic collisions is likely to be favorable for evaporative cooling. Both anisotropy in the long-range interaction and in the short-range potential contribute to large cross sections for inelastic collisions at higher energies and lead to a small ratio of elastic-to-inelastic collisions. This is in agreement with the large rates for Zeeman relaxation of submerged-shell atoms observed experimentally. The effect of the uncertainty in the ab initio potential is sampled by scaling the reduced mass and is found to have little influence on the conclusions drawn from this work.

DOI: 10.1103/physreva.90.052702

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Cold magnetically trapped 2Dg scandium atoms. I. Interaction potential

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Physical Review A

Cold magnetically trapped 2Dg scandium atoms. II. Scattering dynamics

Tijs Karman, Gerrit C. Groenenboom

Published Nov 5, 2014• 6 citations

Publisher

Abstract

The binary collision dynamics of

{}^{2}{D}_{g,3/2}

ground state scandium atoms is studied from first principles. We employ 30 coupled diabatic ab initio potentials in a coupled-channels study of the scattering dynamics of cold and ultracold scandium atoms in external magnetic fields. Due to the long-ranged magnetic dipolar interaction, the field dependence of the cross section does not follow the threshold laws derived by Volpi and Bohn [Phys. Rev. A 65, 052712 (2002)]. In the field-free case, the near-threshold cross section is independent of the collision energy, and hence the cross section does not follow the well-established Wigner threshold laws. The observed threshold behavior is explained in the Born approximation. For energies above

1\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}

, inelastic collisions are driven by the anisotropic nonrelativistic electronic interaction. For energies below

100\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}

, the ratio of elastic-to-inelastic collisions is likely to be favorable for evaporative cooling. Both anisotropy in the long-range interaction and in the short-range potential contribute to large cross sections for inelastic collisions at higher energies and lead to a small ratio of elastic-to-inelastic collisions. This is in agreement with the large rates for Zeeman relaxation of submerged-shell atoms observed experimentally. The effect of the uncertainty in the ab initio potential is sampled by scaling the reduced mass and is found to have little influence on the conclusions drawn from this work.

DOI: 10.1103/physreva.90.052702

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Dipolar collisions in cooling and trapping of paramagnetic atoms

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The long-range van der Waals (vdW) interactions between atoms are calculated, for Cr, by including accurate transition frequencies, discrete dipole matrix elements, and photoionization continuum oscillator strengths, and for Rb, using published dynamic polarizabilities. The vdW coefficients for Cr-Cr and Rb-Cr are obtained. In the cold collision regime, I investigate the influence of angular momentum shape resonances on the elastic and inelastic (loss channel) rate coefficients, and when the Zeeman relaxation, resulting in the loss of atoms from the trap, dominates elastic collision. Dipolar collisions are crucial to achieving quantum degeneracy. Magnetically tuned Fano-Feshbach closed-channel resonances are used to obtain zero-energy scattering lengths in comparison with observation of trap loss. In bosonic chromium collisions, resonances appear due only to dipolar interaction. 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The collisions of different isotopes of maximally spin-polarized chromium atoms (52Cr and 53Cr), alkali-metal atom (Rb) - chromium atom, and magnetically trapped hydroxide (OH) with cold supersonic helium beam are considered in this thesis. Spin-changing cross sections and rate constants in Cr-Cr isotopic collision in the presence of a magnetic field are calculated by propagating a set of multichannel equations in the field. The coupling between dipole-dipole allowed and hyperfine channels are included. The short range electrostatic interactions between atoms and atom-molecule are represented with highly-accurate Born-Oppenheimer (BO) potential energy curves. Due to the large spin multiplicity in Cr-Cr and Rb-Cr interactions, more than the usual singlet and triplet channels are obtained. The long-range van der Waals (vdW) interactions between atoms are calculated, for Cr, by including accurate transition frequencies, discrete dipole matrix elements, and photoionization continuum oscillator strengths, and for Rb, using published dynamic polarizabilities. The vdW coefficients for Cr-Cr and Rb-Cr are obtained. In the cold collision regime, I investigate the influence of angular momentum shape resonances on the elastic and inelastic (loss channel) rate coefficients, and when the Zeeman relaxation, resulting in the loss of atoms from the trap, dominates elastic collision. Dipolar collisions are crucial to achieving quantum degeneracy. Magnetically tuned Fano-Feshbach closed-channel resonances are used to obtain zero-energy scattering lengths in comparison with observation of trap loss. In bosonic chromium collisions, resonances appear due only to dipolar interaction. 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Jan 1, 20111 citation

Cold magnetically trapped 2Dg scandium atoms. I. Interaction potential

Tijs Karman, Xi Chu, Gerrit C. Groenenboom

We present a first principles description of the interaction of two ground-state scandium atoms. Scandium has a ${{}^{2}D}_{g}$ ground state. Thirty molecular states correlate to the lowest dissociation limit of the dimer. In the short range, potential energy curves are calculated using second-order $n$ -electron valence state perturbation theory. The first-order long-range interaction is calculated at the complete active space self-consistent field level. We determine the second-order long-range dispersion interaction from atomic dynamic polarizabilities at imaginary frequencies. These polarizabilities are calculated using time-dependent density functional theory. We merge the short-range approach with the long-range model to obtain a physical description of the 30 potential energy curves correlating to the ${{}^{2}D}_{g}+{{}^{2}D}_{g}$ limit. Diabatic potentials are presented that can be used in quantum scattering calculations, in order to study Zeeman relaxation of ultracold scandium atoms.We present a first principles description of the interaction of two ground-state scandium atoms. Scandium has a ${{}^{2}D}_{g}$ ground state. Thirty molecular states correlate to the lowest dissociation limit of the dimer. In the short range, potential energy curves are calculated using second-order $n$-electron valence state perturbation theory. The first-order long-range interaction is calculated at the complete active space self-consistent field level. We determine the second-order long-range dispersion interaction from atomic dynamic polarizabilities at imaginary frequencies. These polarizabilities are calculated using time-dependent density functional theory. We merge the short-range approach with the long-range model to obtain a physical description of the 30 potential energy curves correlating to the ${{}^{2}D}_{g}+{{}^{2}D}_{g}$ limit. Diabatic potentials are presented that can be used in quantum scattering calculations, in order to study Zeeman relaxation of ultracold scandium atoms.

Physical Review ANov 5, 201410 citations

Ab initiostudy of Tm-He interactions and dynamics in a magnetic trap

Alexei A. Buchachenko, Grzegorz Chałasiński, Małgorzata M. Szczęśniak +1 more

The dynamics of magnetic relaxation of Tm atoms in cold helium gas is investigated using ab initio interaction potentials between $\mathrm{Tm}(^{2}F)$ and He atoms. The interaction of $\mathrm{Tm}(^{2}F)$ with He gives rise to four adiabatic potentials of ${\ensuremath{\Sigma}}^{+}$, $\ensuremath{\Pi}$, $\ensuremath{\Delta}$, and $\ensuremath{\Phi}$ symmetries, which are found to be degenerate to within $0.1\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ at all interatomic distances larger than $R=5.4\phantom{\rule{0.3em}{0ex}}\mathrm{\AA{}}$ . The small splitting between the interaction potentials leads to suppression of Zeeman transitions in Tm-He collisions. Our quantum scattering calculations yield a small rate constant of $1.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$ for Zeeman relaxation of the $\mathrm{Tm}(^{2}F_{7∕2})$ atoms in the maximally stretched $M=7∕2$ sublevel at the temperature $0.8\phantom{\rule{0.3em}{0ex}}\mathrm{K}$ , in reasonable agreement with the measured value $(5.0\ifmmode\pm\else\textpm\fi{}2.1)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$. The sensitivity of Zeeman-relaxation cross sections to details of the interaction potentials is examined. To our knowledge, this is one of only two comparisons of ab initio quantum scattering calculations with experimental measurements of inelastic collisions at subkelvin temperatures near one Kelvin. Our work thus demonstrates the feasibility of describing cold collisions from first principles.The dynamics of magnetic relaxation of Tm atoms in cold helium gas is investigated using ab initio interaction potentials between $\mathrm{Tm}(^{2}F)$ and He atoms. The interaction of $\mathrm{Tm}(^{2}F)$ with He gives rise to four adiabatic potentials of ${\ensuremath{\Sigma}}^{+}$, $\ensuremath{\Pi}$, $\ensuremath{\Delta}$, and $\ensuremath{\Phi}$ symmetries, which are found to be degenerate to within $0.1\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ at all interatomic distances larger than $R=5.4\phantom{\rule{0.3em}{0ex}}\mathrm{\AA{}}$. The small splitting between the interaction potentials leads to suppression of Zeeman transitions in Tm-He collisions. Our quantum scattering calculations yield a small rate constant of $1.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$ for Zeeman relaxation of the $\mathrm{Tm}(^{2}F_{7∕2})$ atoms in the maximally stretched $M=7∕2$ sublevel at the temperature $0.8\phantom{\rule{0.3em}{0ex}}\mathrm{K}$, in reasonable agreement with the measured value $(5.0\ifmmode\pm\else\textpm\fi{}2.1)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$. The sensitivity of Zeeman-relaxation cross sections to details of the interaction potentials is examined. To our knowledge, this is one of only two comparisons of ab initio quantum scattering calculations with experimental measurements of inelastic collisions at subkelvin temperatures near one Kelvin. Our work thus demonstrates the feasibility of describing cold collisions from first principles.

Physical Review AAug 2, 200615 citations

Cold and ultracold NH–NH collisions: The field-free case

Liesbeth M. C. Janssen, Piotr Szymon Żuchowski, Ad van der Avoird +2 more

We present elastic and inelastic spin-changing cross sections for cold and ultracold NH(X (3)Σ(-)) + NH(X (3)Σ(-)) collisions, obtained from full quantum scattering calculations on an accurate ab initio quintet potential-energy surface. Although we consider only collisions in zero field, we focus on the cross sections relevant for magnetic trapping experiments. It is shown that evaporative cooling of both fermionic (14)NH and bosonic (15)NH is likely to be successful for hyperfine states that allow s-wave collisions. The calculated cross sections are very sensitive to the details of the interaction potential, due to the presence of (quasi)bound state resonances. The remaining inaccuracy of the ab initio potential-energy surface therefore gives rise to an uncertainty in the numerical cross-section values. However, based on a sampling of the uncertainty range of the ab initio calculations, we conclude that the exact potential is likely to be such that the elastic-to-inelastic cross-section ratio is sufficiently large to achieve efficient evaporative cooling. This likelihood is only weakly dependent on the size of the channel basis set used in the scattering calculations.We present elastic and inelastic spin-changing cross sections for cold and ultracold NH(X (3)Σ(-)) + NH(X (3)Σ(-)) collisions, obtained from full quantum scattering calculations on an accurate ab initio quintet potential-energy surface. Although we consider only collisions in zero field, we focus on the cross sections relevant for magnetic trapping experiments. It is shown that evaporative cooling of both fermionic (14)NH and bosonic (15)NH is likely to be successful for hyperfine states that allow s-wave collisions. The calculated cross sections are very sensitive to the details of the interaction potential, due to the presence of (quasi)bound state resonances. The remaining inaccuracy of the ab initio potential-energy surface therefore gives rise to an uncertainty in the numerical cross-section values. However, based on a sampling of the uncertainty range of the ab initio calculations, we conclude that the exact potential is likely to be such that the elastic-to-inelastic cross-section ratio is sufficiently large to achieve efficient evaporative cooling. This likelihood is only weakly dependent on the size of the channel basis set used in the scattering calculations.

arXiv:1012.0804The Journal of Chemical PhysicsMar 28, 201125 citations

Ultracold O2 + O2 collisions in a magnetic field: On the role of the potential energy surface

Jesús Pérez‐Ríos, José Campos-Martı́nez, Marta I. Hernández

The collision dynamics of (17)O(2)((3)Σ(g)(-)) + (17)O(2)((3)Σ(g)(-)) in the presence of a magnetic field is studied within the close-coupling formalism in the range between 10 nK and 50 mK. A recent global ab initio potential energy surface (PES) is employed and its effect on the dynamics is analyzed and compared with previous calculations where an experimentally derived PES was used [T. V. Tscherbul et al., New J. Phys 134, 055021 (2009)]. Compared to the results using the older PES, magnetic-field dependence of the low-field-seeking state in the ultracold regime is characterized by a very large background scattering length, a(bg), and cross sections exhibit broader and more pronounced Feshbach resonances. The marked resonance structure is somewhat surprising considering the influence of inelastic scattering but it can be explained by resorting to the analytical van der Waals theory, where the short-range amplitude of the entrance channel wavefunction is enhanced by the large a(bg). This strong sensitivity to the short range of the ab initio PES persists up to relatively high energies (10 mK). After this study and despite quantitative predictions are very difficult, it can be concluded that the ratio between elastic and spin relaxation scattering is generally small, except for magnetic fields which are either low or close to an asymmetric Fano-type resonance. Some general trends found here, such as a large density of quasibound states and a propensity toward large scattering lengths, could be also characteristic of other anisotropic molecule-molecule systems.The collision dynamics of (17)O(2)((3)Σ(g)(-)) + (17)O(2)((3)Σ(g)(-)) in the presence of a magnetic field is studied within the close-coupling formalism in the range between 10 nK and 50 mK. A recent global ab initio potential energy surface (PES) is employed and its effect on the dynamics is analyzed and compared with previous calculations where an experimentally derived PES was used [T. V. Tscherbul et al., New J. Phys 134, 055021 (2009)]. Compared to the results using the older PES, magnetic-field dependence of the low-field-seeking state in the ultracold regime is characterized by a very large background scattering length, a(bg), and cross sections exhibit broader and more pronounced Feshbach resonances. The marked resonance structure is somewhat surprising considering the influence of inelastic scattering but it can be explained by resorting to the analytical van der Waals theory, where the short-range amplitude of the entrance channel wavefunction is enhanced by the large a(bg). This strong sensitivity to the short range of the ab initio PES persists up to relatively high energies (10 mK). After this study and despite quantitative predictions are very difficult, it can be concluded that the ratio between elastic and spin relaxation scattering is generally small, except for magnetic fields which are either low or close to an asymmetric Fano-type resonance. Some general trends found here, such as a large density of quasibound states and a propensity toward large scattering lengths, could be also characteristic of other anisotropic molecule-molecule systems.

arXiv:1102.0883The Journal of Chemical PhysicsMar 28, 201122 citations

Low-temperature collisions of NH(X3Σ−) molecules with He atoms in a magnetic field: Anab initiostudy

Roman V. Krems, H. R. Sadeghpour, A. Dalgarno +3 more

Ab initio calculations of cross sections and rate constants for elastic scattering and Zeeman relaxation in collisions of $\mathrm{NH}(X{}^{3}{\ensuremath{\Sigma}}^{\ensuremath{-}})$ molecules with ${}^{3}\mathrm{He}$ atoms in a magnetic field are presented and the mechanism for Zeeman transitions in ground-state ${}^{3}\ensuremath{\Sigma}$ molecules is established. The potential surface for He-NH interaction is obtained using all-electron coupled-cluster calculations with single, double, and noniterative triple excitations in a basis set augmented by bond functions. The ratio of the rates for elastic energy transfer and Zeeman relaxation in NH- ${}^{3}\mathrm{He}$ collisions exceeds ${10}^{5}$ at temperatures between $0.5$ and 1 K.Ab initio calculations of cross sections and rate constants for elastic scattering and Zeeman relaxation in collisions of $\mathrm{NH}(X{}^{3}{\ensuremath{\Sigma}}^{\ensuremath{-}})$ molecules with ${}^{3}\mathrm{He}$ atoms in a magnetic field are presented and the mechanism for Zeeman transitions in ground-state ${}^{3}\ensuremath{\Sigma}$ molecules is established. The potential surface for He-NH interaction is obtained using all-electron coupled-cluster calculations with single, double, and noniterative triple excitations in a basis set augmented by bond functions. The ratio of the rates for elastic energy transfer and Zeeman relaxation in NH-${}^{3}\mathrm{He}$ collisions exceeds ${10}^{5}$ at temperatures between $0.5$ and 1 K.

Physical Review ANov 12, 200372 citations

The binary collision dynamics of

{}^{2}{D}_{g,3/2}

1\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}

, inelastic collisions are driven by the anisotropic nonrelativistic electronic interaction. For energies below

100\phantom{\rule{4pt}{0ex}}\ensuremath{\mu}\mathrm{K}

We present a first principles description of the interaction of two ground-state scandium atoms. Scandium has a

{{}^{2}D}_{g}

ground state. Thirty molecular states correlate to the lowest dissociation limit of the dimer. In the short range, potential energy curves are calculated using second-order

n

-electron valence state perturbation theory. The first-order long-range interaction is calculated at the complete active space self-consistent field level. We determine the second-order long-range dispersion interaction from atomic dynamic polarizabilities at imaginary frequencies. These polarizabilities are calculated using time-dependent density functional theory. We merge the short-range approach with the long-range model to obtain a physical description of the 30 potential energy curves correlating to the

{{}^{2}D}_{g}+{{}^{2}D}_{g}

limit. Diabatic potentials are presented that can be used in quantum scattering calculations, in order to study Zeeman relaxation of ultracold scandium atoms.

The dynamics of magnetic relaxation of Tm atoms in cold helium gas is investigated using ab initio interaction potentials between

\mathrm{Tm}(^{2}F)

and He atoms. The interaction of

\mathrm{Tm}(^{2}F)

with He gives rise to four adiabatic potentials of ${\ensuremath{\Sigma}}^{+}$, $\ensuremath{\Pi}$, $\ensuremath{\Delta}$, and $\ensuremath{\Phi}$ symmetries, which are found to be degenerate to within $0.1\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$ at all interatomic distances larger than

R=5.4\phantom{\rule{0.3em}{0ex}}\mathrm{\AA{}}

. The small splitting between the interaction potentials leads to suppression of Zeeman transitions in Tm-He collisions. Our quantum scattering calculations yield a small rate constant of $1.5\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$ for Zeeman relaxation of the

\mathrm{Tm}(^{2}F_{7∕2})

atoms in the maximally stretched

M=7∕2

sublevel at the temperature

0.8\phantom{\rule{0.3em}{0ex}}\mathrm{K}

, in reasonable agreement with the measured value $(5.0\ifmmode\pm\else\textpm\fi{}2.1)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}15}\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{3}\phantom{\rule{0.2em}{0ex}}{\mathrm{s}}^{\ensuremath{-}1}$. The sensitivity of Zeeman-relaxation cross sections to details of the interaction potentials is examined. To our knowledge, this is one of only two comparisons of ab initio quantum scattering calculations with experimental measurements of inelastic collisions at subkelvin temperatures near one Kelvin. Our work thus demonstrates the feasibility of describing cold collisions from first principles.

Ab initio calculations of cross sections and rate constants for elastic scattering and Zeeman relaxation in collisions of $\mathrm{NH}(X{}^{3}{\ensuremath{\Sigma}}^{\ensuremath{-}})$ molecules with

{}^{3}\mathrm{He}

atoms in a magnetic field are presented and the mechanism for Zeeman transitions in ground-state ${}^{3}\ensuremath{\Sigma}$ molecules is established. The potential surface for He-NH interaction is obtained using all-electron coupled-cluster calculations with single, double, and noniterative triple excitations in a basis set augmented by bond functions. The ratio of the rates for elastic energy transfer and Zeeman relaxation in NH-

{}^{3}\mathrm{He}

collisions exceeds

{10}^{5}

at temperatures between

0.5

and 1 K.