Controlling rotation in the molecular frame with an optical centrifuge

We computationally demonstrate a new method for coherently controlling the rotation-axis direction in asymmetric top molecules with an optical centrifuge. Appropriately chosen electric-field strengths and centrifuge's acceleration rate allow to generate nearly arbitrary rotational wavepacket. For D$_2$S 2H-imidazole (C$_3$H$_4$N$_2$) we created wavepackets at large values of quantum number $J$ desired projections total angular momentum onto two molecules' principal axes inertia. One application is three-dimensional alignment molecular axis aligned along laser's wave vector, which important imaging yet not accessible standard approaches. The simultaneous orientation laboratory frame could also be used robust control scattering experiments.