Nuclear spin relaxation in cold atom-molecule collisions

TL;DR

This paper develops a quantum dynamical model to study nuclear spin relaxation in cold atom-molecule collisions, revealing slow relaxation in the ground state and temperature-dependent rates, with implications for quantum control.

Contribution

The authors introduce a rigorous coupled-channel methodology that includes rotational, nuclear spin, and magnetic field effects in atom-molecule collision dynamics.

Findings

Nuclear spin relaxation in the ground state is extremely slow.

Transition rates between N=1 nuclear spin states are higher due to spin-rotation coupling.

Relaxation times decrease rapidly with increasing temperature.

Abstract

We explore the quantum dynamics of nuclear spin relaxation in cold collisions of $^1\Sigma^+$ molecules with structureless atoms in an external magnetic field. To this end, we develop a rigorous coupled-channel methodology, which accounts for rotational and nuclear spin degrees of freedom of $^1\Sigma^+$ molecules, their interaction with an external magnetic field, as well as for anisotropic atom-molecule interactions. We apply the methodology to study collisional relaxation of the nuclear spin sublevels of $^{13}$CO molecules immersed in a cold buffer gas of $^4$He atoms. We find that nuclear spin relaxation in the ground rotational manifold of CO occurs extremely slowly due to the absence of direct couplings between the nuclear spin sublevels. The rates of collisional transitions between the $N=1$ nuclear spin states of CO are generally much higher due to the direct nuclear spin-rotation coupling between the states. These transitions obey selection rules, which depend on the values of space-fixed projections of rotational and nuclear spin angular momenta for the initial and final molecular states. For some initial states, we also observe a strong magnetic field dependence, which can be understood using the first Born approximation. We use our calculated nuclear spin relaxation rates to investigate the thermalization of a single nuclear spin state of CO$(N=0)$ immersed in a cold buffer gas of He. The calculated nuclear spin relaxation times ($T_1\simeq 0.5$ s at $T=1$ K) display a steep temperature dependence decreasing rapidly at elevated temperatures due to the increased population of rotationally excited states, which undergo nuclear spin relaxation at a much faster rate. Thus, long relaxation times of $N=0$ nuclear spin states in cold collisions with buffer gas atoms can only be maintained at sufficiently low temperatures ($kT\ll 2B_e$), where $B_e$ is the rotational constant.