molecules*

Resonant scattering of optically state-prepared and aligned molecules in the cold regime allows the most detailed interrogation and control of bimolecular collisions. This technique has recently been applied to collisions of two aligned ortho-D₂ molecules prepared in the j=2 rotational level of the v=2 vibrational manifold using the Stark-induced adiabatic Raman passage technique. Here, we develop the theoretical formalism for describing four-vector correlations in collisions of two aligned molecules and apply our approach to state-prepared D₂(v=2,j=2)+ D₂(v=2,j=2)→D₂(v=2,j=2)+ D₂(v=2,j=0) collisions, making possible the simulations of the experimental results from first principles. Key features of the experimental angular distributions are reproduced and attributed primarily to a partial wave resonance with orbital angular momentum l=4.