We computationally demonstrate a new method for coherently controlling the rotation-axis direction in asymmetric top molecules . The new scheme utilises an optical centrifuge, which is a linearly polarised light pulse that performs accelerated rotation about the direction of its propagation. A nearly arbitrary rotational wavepacket can be created with appropriately chosen electric-field strengths and the rotating field’s acceleration rate. As an example, we show how to create highly resilient rotational states of deuterium sulphide (D2S), in which the molecule rotates about the intermediate inertia axis, such that its electric dipole moment is aligned along the laser’s propagation axis. Photo-ionisation from these tailored wavepackets can give direct access to the dynamics in the molecular-frame. A newly developed CHIRALEX computer code can be used to model photo-ionisation from arbitrary rotational wavepackets with arbitrary pulses. We are currently utilising CHIRALEX to study the interaction of chiral molecules with chiral electromagnetic pulses, to capture the dynamical nature of chirality at the attosecond time-scales.
References  Emil J. Zak, Andrey Yachmenev, and Jochen Kuepper; Controlling rotation in the molecular frame with an optical centrifuge, Phys. Rev. Research 3, 023188 (2021)