We develop a rigorous quantum mechanical theory for collisions of polyatomic molecular radicals with S-state atoms in the presence of an external magnetic field. The theory is based on a fully uncoupled space-fixed basis set representation of the mul
tichannel scattering wavefunction. Explicit expressions are presented for the matrix elements of the scattering Hamiltonian for spin-1/2 and spin-1 polyatomic molecular radicals interacting with structureless targets. The theory is applied to calculate the cross sections and thermal rate constants for spin relaxation in low-temperature collisions of the prototypical organic molecule methylene [CH2(X)] with He atoms. To this end, two highly accurate three-dimensional potential energy surfaces (PESs) of the He-CH2(X) complex are developed using the state-of-the-art CCSD(T) method and large basis sets. Both PESs exhibit shallow minima and are weakly anisotropic. Our calculations show that spin relaxation in collisions of CH2, CHD, and CD2 molecules with He atoms occurs at a much slower rate than elastic scattering over a large range of temperatures (1 uK -- 1 K) and magnetic fields (0.01 - 1 T), suggesting excellent prospects for cryogenic helium buffer-gas cooling of ground-state ortho-CH2(X) molecules in a magnetic trap. Furthermore, we find that ortho-CH2 undergoes collision-induced spin relaxation much more slowly than para-CH2, which indicates that magnetic trapping can be used to separate nuclear spin isomers of open-shell polyatomic molecules.
A rigorous quantum theory of atomic collisions in the presence of radio frequency (rf) magnetic fields is developed and applied to elucidate the effects of combined dc and rf magnetic fields on elastic scattering in ultracold collisions of Rb atoms.
We show that rf fields can be used to induce Feshbach resonances, which can be tuned by varying the amplitude and frequency of the rf field. The rf-induced Feshbach resonances occur also in collisions of atoms in low-field-seeking states at moderate rf field strengths easily available in atom chip experiments, which opens up the world of tunable interactions to magnetically trappable atomic quantum gases.
We present an accurate quantum mechanical study of molecule-molecule collisions in the presence of a magnetic field. The work focusses on the analysis of elastic scattering and spin relaxation in collisions of O2(3Sigma_g) molecules at cold (~0.1 K)
and ultracold (~10^{-6} K) temperatures. Our calculations show that magnetic spin relaxation in molecule-molecule collisions is extremely efficient except at magnetic fields below 1 mT. The rate constant for spin relaxation at T=0.1 K and a magnetic field of 0.1 T is found to be as large as 6.1 x 10^{-11} cm3/s. The magnetic field dependence of elastic and inelastic scattering cross sections at ultracold temperatures is dominated by a manifold of Feshbach resonances with the density of ~100 resonances per Tesla for collisions of molecules in the absolute ground state. This suggests that the scattering length of ultracold molecules in the absolute ground state can be effectively tuned in a very wide range of magnetic fields. Our calculations demonstrate that the number and properties of the magnetic Feshbach resonances are dramatically different for molecules in the absolute ground and excited spin states. The density of Feshbach resonances for molecule-molecule scattering in the low-field-seeking Zeeman state is reduced by a factor of 10.
We use accurate quantum mechanical calculations to analyze the effects of parallel electric and magnetic fields on collision dynamics of OH(2Pi) molecules. It is demonstrated that spin relaxation in 3He-OH collisions at temperatures below 0.01 K can
be effectively suppressed by moderate electric fields of order 10 kV/cm. We show that electric fields can be used to manipulate Feshbach resonances in collisions of cold molecules. Our results can be verified in experiments with OH molecules in Stark decelerated molecular beams and electromagnetic traps.
