New publication on coherent control of molecular superrotors in Journal of Physical Chemistry Letters

11 July, 2018

Our new publication "Coherent Control of the Rotation Axis of Molecular Superrotors" has been published in The Journal of Physical Chemistry Letters.

Controlling ultrafast rotational motion has seen tremendous progress in recent years thanks to the development of innovative techniques in strong-field laser physics. The ability to efficiently produce molecules in highly excited rotational states, known as molecular superrotors, has revealed unexpected behavior and made superrotors interesting quantities for studies of scattering, spectroscopy, and dynamics. Recently, theoretical research in the CMI group has demonstrated a novel type of coherent control involving molecular superrotors.

Using an optical centrifuge, which is a corkscrew shaped laser pulse capable of spinning molecules into high angular momentum states, we have shown that by modifying the pulse envelope, an asymmetric-top molecule can be made to rotate about two entirely different molecular axes in a stable and controlled manner. This is achieved by exciting the molecule along different pathways of rotational states, ultimately leading to rotation about different axes. Such a scheme to control the angular momentum alignment of a molecule will be useful in studies of molecule-molecule or molecule-surface scattering, particularly due to the large amounts of energy associated with superrotors, which can even be controlled by changing the duration of the optical centrifuge pulse.

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