The optical centrifuge technique that spins up molecules is modified to align molecules into highly excited rotational states, where it is demonstrated that the created alignment has a long lifetime against collisions with other molecules.
We use an optical centrifuge to align asymmetric top SO_{2} molecules by adiabatically spinning their most polarizable O-O axis. The effective centrifugal potential in the rotating frame confines the sulfur atoms to the plane of the laser-induced rotation, leading to the planar molecular alignment that persists after the molecules are released from the centrifuge. The periodic appearance of the full three-dimensional alignment, typically observed only with linear and symmetric top molecules, is also detected. Together with strong in-plane centrifugal forces, which bend the molecules by up to 10 deg, permanent field-free alignment offers new ways of controlling molecules with laser light.
The control of ultrafast molecular rotational motion has benefited from the development of innovative techniques in strong-field laser physics. Here, we theoretically demonstrate a novel type of coherent control by inducing rotation of an asymmetric-top molecule about two different molecular axes. An optical centrifuge is applied to the hydrogen sulfide (H 2 S) molecule to create a molecular superrotor, an object performing ultrafast rotation about a well-defined axis. Using two distinct pulse envelopes for the optical centrifuge, we show that H 2 S can be excited along separate pathways of rotational states. This leads to stable rotation about two entirely different molecular axes while ensuring rotation is about the propagation direction of the centrifuge, i.e., the laboratory-fixed Z -axis. The presented scheme to control the angular momentum alignment of a molecule will, for instance, be useful in studies of molecule–molecule or molecule–surface scattering, especially due to the large amounts of energy associated with superrotors, which can even be controlled by changing the duration of the optical centrifuge pulse.
We experimentally demonstrate that the rotation of molecules embedded in helium nanodroplets can be controlled with an optical centrifuge, allowing for the study of molecular dynamics inside the strongly interacting many-body environment of superfluid helium at variable levels of rotational excitation. By doping the droplets with dimers of nitric oxide, (NO)_{2}, and measuring the degree of their centrifuge-induced alignment as a function of time, we show both the forced in-field rotation of molecules in a continuous range of frequencies, as well as the field-free resonant rotation with a long nanosecond-scale decay. The ability to control and monitor the rotational dynamics of molecular rotors inside the superfluid medium may shed new light on superfluidity and the interaction of superfluids with defects at the atomic level.