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Register a new userMagnetic field modification of ultracold molecule-molecule collisions
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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.
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Understanding ultracold collisions involving molecules is of fundamental importance for current experiments, where inelastic collisions typically limit the lifetime of molecular ensembles in optical traps. Here we present a broad study of optically trapped ultracold RbCs molecules in collisions with one another, in reactive collisions with Rb atoms, and in nonreactive collisions with Cs atoms. For experiments with RbCs alone, we show that by modulating the intensity of the optical trap, such that the molecules spend 75% of each modulation cycle in the dark, we partially suppress collisional loss of the molecules. This is evidence for optical excitation of molecule pairs mediated via sticky collisions. We find that the suppression is less effective for molecules not prepared in the spin-stretched hyperfine ground state. This may be due either to longer lifetimes for complexes or to laser-free decay pathways. For atom-molecule mixtures, RbCs+Rb and RbCs+Cs, we demonstrate that the rate of collisional loss of molecules scales linearly with the density of atoms. This indicates that, in both cases, the loss of molecules is rate-limited by two-body atom-molecule processes. For both mixtures, we measure loss rates that are below the thermally averaged universal limit.
We investigate collisional loss in an ultracold mixture of $^{40}$K$^{87}$Rb molecules and $^{87}$Rb atoms, where chemical reactions between the two species are energetically forbidden. Through direct detection of the KRb$_{2}^{*}$ intermediate complexes formed from atom-molecule collisions, we show that a $1064$ nm laser source used for optical trapping of the sample can efficiently deplete the complex population via photo-excitation, an effect which can explain the universal two-body loss observed in the mixture. By monitoring the time-evolution of the KRb$_{2}^{*}$ population after a sudden reduction in the $1064$ nm laser intensity, we measure the lifetime of the complex ($0.39(6)$ ms), as well as the photo-excitation rate for $1064$ nm light ($0.50(3)$ $mu$s$^{-1}($kW/cm$^{2})^{-1}$). The observed lifetime is ${sim}10^{5}$ times longer than recent estimates based on the Rice-Ramsperger-Kassel-Marcus statistical theory, which calls for new insight to explain such a dramatic discrepancy.
Highly accurate variational calculations, based on a few-parameter, physically adequate trial function, are carried out for the hydrogen molecule hh in inclined configuration, where the molecular axis forms an angle $theta$ with respect to the direction of a uniform constant magnetic field ${bf B}$, for $B=0,, 0.1,, 0.175$ and $0.2,$a.u. Three inclinations $theta=0^circ,,45^circ,,90^circ$ are studied in detail with emphasis to the ground state $1_g$. Diamagnetic and paramagnetic susceptibilities are calculated (for $theta=45^circ$ for the first time), they are in agreement with the experimental data and with other calculations. For $B=0,, 0.1$ and $0.2,$a.u. potential energy curves $E$ vs $R$ are built for each inclination, they are interpolated by simple, two-point Pade approximant $Pade[2/6](R)$ with accuracy of not less than 4 significant digits. Spectra of rovibrational states are calculated for the first time. It was found that the optimal configuration of the ground state for $B leq B_{cr}=0.178,$a.u. corresponds always to the parallel configuration, $theta=0$, thus, it is a $^1Sigma_g$ state. The state $1_g$ remains bound for any magnetic field, becoming metastable for $B > B_{cr}$, while for $B_{cr} < B < 12$,a.u. the ground state corresponds to two isolated hydrogen atoms with parallel spins.
The stereochemical properties of the ultracold ground state OH molecule in the presence of electric and magnetic fields are currently of considerable interest. For example, relevant quantities such as molecular alignment and orientation, calculated numerically by using large basis sets, have lately appeared in the literature. In this work, based on our recent exact solution to an effective eight-dimensional matrix Hamiltonian for the molecular ground state, we present analytic expressions for the stereochemical properties of OH. Our results require the solution of algebraic equations only, agree well with the aforementioned fully numerical calculations, provide compact expressions for simple field geometries, allow ready access to relatively unexplored parameter space, and yield straightforwardly higher moments of the molecular axis distribution.
In this article we present a concrete proposal for spin squeezing the ultracold ground state polar paramagnetic molecule OH, a system currently under fine control in the laboratory. In contrast to existing work, we consider a single, non-interacting molecule with angular momentum greater than $1/2$. Starting from an experimentally relevant effective Hamiltonian, we identify a parameter regime where different combinations of static electric and magnetic fields can be used to realize the single-axis twisting Hamiltonian of Kitagawa and Ueda [M. Kitagawa and M. Ueda, Phys. Rev. A 47, 5138 (1993)], the uniform field Hamiltonian proposed by Law et al. [C. K. Law, H. T Ng and P. T. Leung, Phys. Rev. A 63, 055601 (2001)], and a model of field propagation in a Kerr medium considered by Agarwal and Puri [G. S. Agarwal and R. R. Puri, Phys. Rev. A 39, 2969 (1989)]. To support our conclusions, we provide analytical expressions as well as numerical calculations, including optimization of field strengths and accounting for the effects of field misalignment. Our results have consequences for applications such as precision spectroscopy, techniques such as magnetometry, and stereochemical effects such as the orientation-to-alignment transition.
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