In summary, we demonstrated that the molecular orientation with O An as the coordinate origin provides the most faithful representation of the LG(OI) OR tensor using a standard LG approach. Although other choices of origin and orientation are possible, O An is more natural because it is close to the COM of the molecule and it can be obtained with a simple analytical procedure. Furthermore, this choice of orientation is transferable across methods so it can be computed at a lower level where the implementation of LG(OI) is simple, and used for standard LG calculations at higher levels of theory.