  We propose and computationally study a method for simultaneously orienting
the angular momentum of asymmetric top molecules along: 1) a laboratory-fixed
direction; 2) the molecular intermediate moment of inertia axis; 3) the laser
field wavevector. For this purpose we utilize a coherent control scheme in
which a tailored-pulse optical centrifuge populates rotational states with well
defined projections of the total angular momentum onto molecular axes.
Appropriately time-shaped optical centrifuge pulses can leave the rotational
wavepacket in peculiar rotational coherences which lead to a good degree of
3-dimensional transient alignment, with an arbitrary molecular axis pointing
along the laser pulse propagation direction. As an example, we demonstrate how
to generate highly resilient rotational quantum states of D2S in which the
molecule rotates mainly about its intermediate inertia axis, such that its
electric dipole moment is permanently aligned along the propagation direction
of the laser pulse. Applications might include accessing less obscured
information in various photo-electron imaging experiments.
