Highly Spin-Polarized Molecules via Collisional Microwave Pumping.

We propose a general technique to produce cold spin-polarized molecules in the electronic states of Σ symmetry, in which rotationally excited levels are first populated by coherent microwave excitation, and then allowed to spin flip and relax via collisional quenching, which populates a single final spin state. The steady-state spin polarization is maximized in the regime, where collisional slip-flipping transitions in the ground rotational manifold (N=0) are suppressed by a factor of ≥10 compared to those in the first rotationally excited manifold (N=1), as generally expected for Σ-state molecules at temperatures below the rotational spacing between the N=0 and N=1 manifolds. We theoretically demonstrate the high selectivity of the technique for ^{13}C^{16}O molecules immersed in a cold buffer gas of helium atoms, achieving a high degree (≥95%) of nuclear spin polarization at 1 K.