Laser control of molecular rotation: Expanding the utility of an optical centrifuge.

Since its invention in 1999, the optical centrifuge has become a powerful tool for controlling molecular rotation and studying molecular dynamics and molecular properties at extreme levels of rotational excitation. This technique has been applied to a variety of molecular species, from simple linear molecules to symmetric and asymmetric tops, to molecular ions and chiral enantiomers. Properties of isolated ultrafast rotating molecules, the so-called molecular superrotors, have been investigated, as well as their collisions with one another and the interaction with external fields. The ability of an optical centrifuge to spin a particular molecule of interest depends on both the molecular structure and the parameters of the centrifuge laser pulse. An interplay between these two factors dictates the utility of an optical centrifuge in any specific application. Here, we discuss the strategy of assessing and adjusting the properties of the centrifuge to those of the molecular rotors and describe two practical examples of optical centrifuges with very different characteristics, implemented experimentally in our laboratory.