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Bulletin of the American Physical Society

Control of Rotational Energy and Angular Momentum Orientation with an Optical Centrifuge

Hannah M. Ogden, Matthew J. Murray, Amy S. Mullin

Published Jun 9, 2017• 0 citations
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We experimentally demonstrate a controlled transfer of angular momentum to roton pairs in superfluid helium. The control is executed with an optical centrifuge and detected with coherent time- and frequency-resolved Raman scattering. We show that the sign of the Raman shift, and hence the orientation of the angular momentum transferred from the laser field to the rotons, is dictated by the centrifuge. The magnitude of the shift reflects the two-roton energy and indicates that the centrifuge-induced roton pairs are far from the equilibrium with the quantum bath. The observed decay of the coherent Raman signal suggests that the decoherence is governed by the scattering on thermal rotons and phonons. The demonstrated method offers ways of examining microscopic origins of superfluidity by controlling collective excitations in superfluids.

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Coherent Control of the Rotation Axis of Molecular Superrotors

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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.

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Dynamics of molecular superrotors in an external magnetic field

Aleksey Korobenko, Valery Milner

Abstract We excite diatomic oxygen and nitrogen to high rotational states with an optical centrifuge and study their dynamics in an external magnetic field. Ion imaging is employed to directly visualize, and follow in time, the rotation plane of the molecular superrotors. The two different mechanisms of interaction between the magnetic field and the molecular angular momentum in paramagnetic oxygen and non-magnetic nitrogen lead to qualitatively different behaviour. In nitrogen, we observe the precession of the molecular angular momentum around the field vector. In oxygen, strong spin–rotation coupling results in faster and richer dynamics, encompassing the splitting of the rotation plane into three separate components. As the centrifuged molecules evolve with no significant dispersion of the molecular wave function, the observed magnetic interaction presents an efficient mechanism for controlling the plane of molecular rotation.

arXiv:1504.01432•Journal of Physics B Atomic Molecular and Optical Physics•Jul 15, 2015•16 citations
We experimentally demonstrate a controlled transfer of angular momentum to roton pairs in superfluid helium. The control is executed with an optical centrifuge and detected with coherent time- and frequency-resolved Raman scattering. We show that the sign of the Raman shift, and hence the orientation of the angular momentum transferred from the laser field to the rotons, is dictated by the centrifuge. The magnitude of the shift reflects the two-roton energy and indicates that the centrifuge-induced roton pairs are far from the equilibrium with the quantum bath. The observed decay of the coherent Raman signal suggests that the decoherence is governed by the scattering on thermal rotons and phonons. The demonstrated method offers ways of examining microscopic origins of superfluidity by controlling collective excitations in superfluids.
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.
Abstract We excite diatomic oxygen and nitrogen to high rotational states with an optical centrifuge and study their dynamics in an external magnetic field. Ion imaging is employed to directly visualize, and follow in time, the rotation plane of the molecular superrotors. The two different mechanisms of interaction between the magnetic field and the molecular angular momentum in paramagnetic oxygen and non-magnetic nitrogen lead to qualitatively different behaviour. In nitrogen, we observe the precession of the molecular angular momentum around the field vector. In oxygen, strong spin–rotation coupling results in faster and richer dynamics, encompassing the splitting of the rotation plane into three separate components. As the centrifuged molecules evolve with no significant dispersion of the molecular wave function, the observed magnetic interaction presents an efficient mechanism for controlling the plane of molecular rotation.