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 the centrifuge's acceleration rate allow to generate a nearly arbitrary rotational wave packet. For dihydrogen sulfide $\left({\text{D}}_2\text{S}\right)$ and 2H-imidazole $\left({\text{C}}_3{\text{H}}_4{\text{N}}_2\right)$, we created wave packets at large values of the rotational quantum number $J$ with the desired projections of the total angular momentum onto two of the molecules' principal axes of inertia. One application of the new method is three-dimensional alignment with a molecular axis aligned along the laser's wave vector, which is important for the three-dimensional imaging of molecules yet not accessible in standard approaches. The simultaneous orientation of the angular momentum in the laboratory frame and in the molecular frame could also be used in robust control of scattering experiments.

• Received 8 September 2020
• Revised 28 April 2021
• Accepted 4 May 2021

DOI:https://doi.org/10.1103/PhysRevResearch.3.023188

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Published by the American Physical Society