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arXiv:1007.0469 · Physical Review A

Collisional properties of cold spin-polarized nitrogen gas: Theory, experiment, and prospects as a sympathetic coolant for trapped atoms and molecules

Timur V. Tscherbul, Jacek A. Kłos, A. Dalgarno, Bernard Zygelman, Zoran Miroslav Pavlovic, Matthew T. Hummon, Hsin-I Lu, Edem Tsikata, John M. Doyle

Published Oct 26, 2010• 14 citations
arXivHTMLPDF

Abstract

We report a combined experimental and theoretical study of collision-induced dipolar relaxation in a cold spin-polarized gas of atomic nitrogen (N). We use buffer gas cooling to create trapped samples of $^{14}\mathrm{N}$ and $^{15}\mathrm{N}$ atoms with densities $(5\ifmmode\pm\else\textpm\fi{}2)\ifmmode\times\else\texttimes\fi{}{10}^{12} {\mathrm{cm}}^{\ensuremath{-}3}$ and measure their magnetic relaxation rates at milli-Kelvin temperatures. These measurements, together with rigorous quantum scattering calculations based on accurate ab initio interaction potentials for the ${}^{7}{\ensuremath{\Sigma}}_{u}^{+}$ electronic state of ${\mathrm{N}}_{2}$ demonstrate that dipolar relaxation in $\mathrm{N}+\mathrm{N}$ collisions occurs at a slow rate of $~{10}^{\ensuremath{-}13} {\mathrm{cm}}^{3}$/s over a wide range of temperatures (1 mK to 1 K) and magnetic fields (10 mT to 2 T). The calculated dipolar relaxation rates are insensitive to small variations of the interaction potential and to the magnitude of the spin-exchange interaction, enabling the accurate calibration of the measured N atom density. We find consistency between the calculated and experimentally determined rates. Our results suggest that N atoms are promising candidates for future experiments on sympathetic cooling of molecules.

DOI
10.1103/physreva.82.042718

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We report a combined experimental and theoretical study of collision-induced dipolar relaxation in a cold spin-polarized gas of atomic nitrogen (N). We use buffer gas cooling to create trapped samples of 14N^{14}\mathrm{N}14N and 15N^{15}\mathrm{N}15N atoms with densities (5\ifmmode±\else\textpm\fi2)\ifmmode×\else\texttimes\fi1012cm\ensuremath−3(5\ifmmode\pm\else\textpm\fi{}2)\ifmmode\times\else\texttimes\fi{}{10}^{12} {\mathrm{cm}}^{\ensuremath{-}3}(5\ifmmode±\else\textpm\fi2)\ifmmode×\else\texttimes\fi1012cm\ensuremath−3 and measure their magnetic relaxation rates at milli-Kelvin temperatures. These measurements, together with rigorous quantum scattering calculations based on accurate ab initio interaction potentials for the 7\ensuremathΣu+{}^{7}{\ensuremath{\Sigma}}_{u}^{+}7\ensuremathΣu+​ electronic state of N2{\mathrm{N}}_{2}N2​ demonstrate that dipolar relaxation in N+N\mathrm{N}+\mathrm{N}N+N collisions occurs at a slow rate of  10\ensuremath−13cm3~{10}^{\ensuremath{-}13} {\mathrm{cm}}^{3} 10\ensuremath−13cm3/s over a wide range of temperatures (1 mK to 1 K) and magnetic fields (10 mT to 2 T). The calculated dipolar relaxation rates are insensitive to small variations of the interaction potential and to the magnitude of the spin-exchange interaction, enabling the accurate calibration of the measured N atom density. We find consistency between the calculated and experimentally determined rates. Our results suggest that N atoms are promising candidates for future experiments on sympathetic cooling of molecules.
The prospects of sympathetic cooling of polar molecules with magnetically cotrapped alkali-metal atoms are generally considered poor due to strongly anisotropic atom-molecule interactions leading to large spin relaxation rates. Using rigorous quantum scattering calculations based on ab initio interaction potentials, we show that inelastic spin relaxation in low-temperature collisions of CaH(${}^{2}\ensuremath{\Sigma}$) molecules with Li and Mg atoms occurs at a slow rate despite the strongly anisotropic interactions. This unexpected result, which we rationalize using multichannel quantum-defect theory, opens up the possibility of sympathetic cooling of polar ${}^{2}\ensuremath{\Sigma}$ molecules with alkali-metal atoms in a magnetic trap and with alkaline-earth-metal atoms in an optical dipole trap.
We present a rigorous theoretical study of low-temperature collisions of polyatomic molecular radicals with (1)S(0) atoms in the presence of an external magnetic field. Accurate quantum scattering calculations based on ab initio and scaled interaction potentials show that collision-induced spin relaxation of the prototypical organic molecule CH(2)(X(3)B(1)) (methylene) and nine other triatomic radicals in cold (3)He gas occurs at a slow rate, demonstrating that cryogenic buffer-gas cooling and magnetic trapping of these molecules is feasible with current technology. Our calculations further suggest that it may be possible to create ultracold gases of polyatomic molecules by sympathetic cooling with alkaline-earth atoms in a magnetic trap.
We present an experimental and theoretical study of atom-molecule collisions in a mixture of cold, trapped N atoms and NH molecules at a temperature of $\ensuremath{\sim}600\text{ }\text{ }\mathrm{mK}$. We measure a small N+NH\mathrm{N}+\mathrm{NH}N+NH trap loss rate coefficient of ${k}_{\mathrm{loss}}^{(\mathrm{N}+\mathrm{NH})}=9(5)(3)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}13}\text{ }\text{ }{\mathrm{cm}}^{3}\text{ }{\mathrm{s}}^{\ensuremath{-}1}$. Accurate quantum scattering calculations based on ab initio interaction potentials are in agreement with experiment and indicate the magnetic dipole interaction to be the dominant loss mechanism. Our theory further indicates the ratio of N+NH\mathrm{N}+\mathrm{NH}N+NH elastic-to-inelastic collisions remains large (>100>100>100) into the mK regime.
We present a combined experimental and theoretical study of angular momentum depolarization in cold collisions of 2P^{2}P2P atoms in the presence of an external magnetic field. We show that collision-induced Zeeman relaxation of Ga(2P1/2)\text{Ga}({^{2}P}_{1/2})Ga(2P1/2​) and In(2P1/2)\text{In}({^{2}P}_{1/2})In(2P1/2​) atoms in cold 4He^{4}\text{H}\text{e}4He gas is dramatically suppressed compared to atoms in 2P3/2{^{2}P}_{3/2}2P3/2​ states. Using rigorous quantum-scattering calculations based on ab initio interaction potentials, we demonstrate that Zeeman transitions in collisions of atoms in 2P1/2{^{2}P}_{1/2}2P1/2​ electronic states occur via couplings to the 2P3/2{^{2}P}_{3/2}2P3/2​ state induced by the anisotropy of the interaction potential. Our results suggest the feasibility of sympathetic cooling and magnetic trapping of 2P1/2{^{2}P}_{1/2}2P1/2​-state atoms, such as halogens, thereby opening up exciting areas of research in precision spectroscopy and cold-controlled chemistry.
In this dissertation, I present ab initio theoretical results on cold and ultra-cold collision of atomic and molecular systems with magnetic and electric dipole moments. 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. The interplay between hyperfine and dipolar resonances in mixed-species Cr-Cr and Rb-Cr collisions is studied. In Rb-Cr, it is found that the molecule has broken symmetry and therefore contains a large permanent electric dipole moment in the ground state. A recent collisional experiment at JILA of a supersonic helium beam with a magnetically trapped OH radical found the onset of a quantum threshold in the total OH loss rate. Using ab initio BO energy surfaces, I calculated the spin-changing collisions which removed OH from the trap. Only after including the effect of the trapping potential on the collision dynamics, some agreement with observation was found. ^
Cold molecules promise to reveal a rich set of novel collision dynamics in the low-energy regime. By combining for the first time the techniques of Stark deceleration, magnetic trapping, and cryogenic buffer gas cooling, we present the first experimental observation of cold collisions between two different species of state-selected neutral polar molecules. This has enabled an absolute measurement of the total trap loss cross sections between OH and ND(3) at a mean collision energy of 3.6 cm(-1) (5 K). Due to the dipolar interaction, the total cross section increases upon application of an external polarizing electric field. Cross sections computed from ab initio potential energy surfaces are in agreement with the measured value at zero external electric field. The theory presented here represents the first such analysis of collisions between a (2)Π radical and a closed-shell polyatomic molecule.