  We report two schemes to generate perfect anisotropy in the photoelectron
angular distribution of a randomly oriented ensemble of polyatomic molecules.
In order to exert full control over the anisotropy of photoelectron emission,
we exploit interferences between single-photon pathways and a manifold of
resonantly-enhanced two-photon pathways. These are shown to outperform
non-sequential $(\omega,2\omega)$ bichromatic phase control for the example of
CHFClBr molecules. We are able to optimize pulses that yield anisotropic
photoelectron emission thanks to a very efficient calculation of photoelectron
momentum distributions. This is accomplished by combining elements of quantum
chemistry, variational scattering theory, and time-dependent perturbation
theory.
