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arXiv:2509.02913 · Physical Review Letters

Control of Molecular Rotation in Helium Nanodroplets with an Optical Centrifuge

Ian MacPhail-Bartley, Alexander A. Milner, Frank Stienkemeier, Valery Milner

Published Dec 1, 2025• 2 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1103/5jnj-97vs

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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.
An optical centrifuge is a laser pulse which enables controlled rotational excitation of molecules. Centrifuged molecules rotating with well-defined angular frequencies are ideal candidates to probe many-body quantum systems at the nanoscale. Because the interaction with the quantum environment increases the effective moment of inertia of the embedded molecular probes, the required rotational acceleration of the optical centrifuge must be lowered to accommodate adiabatic spinning. We demonstrate a design of an optical centrifuge, based on the method of spectral focusing, which enables extremely low, down to zero, rotational accelerations. We discuss the potential of using such constant-frequency centrifuge to investigate molecular rotation inside helium nanodroplets.
A macroscopic manifestation of superfluidity is that objects moving through liquid helium experience negligible friction below the Landau critical velocity. How this frictionless motion breaks down at the nanoscale remains an open question. Molecules embedded in helium nanodroplets represent a well-controlled system for studying this breakdown, yet none has reached the regime of strong dissipative coupling, when energy transfer from the molecule to the superfluid dominates the observed dynamics. Molecular rotation, induced by short laser pulses, offer a suitable probe to reach rotational energies in the range of the roton gap, where superfluid helium supports a large number of elementary excitations. However, the solvation shell around a rotating molecule caps the energy reachable by a free rotor after impulsive excitation well below the roton excitation energy. Here we show that continuous driving with an ultraslow optical centrifuge overcomes this limitation: the strong field dresses the molecule into pendular states whose energies fall within the spectrum of the collective excitations of the superfluid, placing the system in the strong-dissipation regime. The resulting rapid thermalization locks the molecule to the rotating field until the rotation-induced level splittings overtake the thermalization rate, beyond which the molecular alignment is progressively lost. Our approach offers a direct measurement of the molecule-bath coupling in a quantum fluid.
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Helium nanodroplets are considered ideal model systems to explore quantum hydrodynamics in self-contained, isolated superfluids. However, exploring the dynamic properties of individual droplets is experimentally challenging. In this work, we used single-shot femtosecond x-ray coherent diffractive imaging to investigate the rotation of single, isolated superfluid helium-4 droplets containing ~10(8) to 10(11) atoms. The formation of quantum vortex lattices inside the droplets is confirmed by observing characteristic Bragg patterns from xenon clusters trapped in the vortex cores. The vortex densities are up to five orders of magnitude larger than those observed in bulk liquid helium. The droplets exhibit large centrifugal deformations but retain axially symmetric shapes at angular velocities well beyond the stability range of viscous classical droplets.
Molecules embedded in superfluids provide an experimentally controllable platform for investigating impurity physics. Here, we investigate a driven molecule rotating in a superfluid environment, including helium and Bose--Einstein condensates, at rotation frequencies similar to the bath dynamics. Within the experimentally relevant platform of an optical centrifuge, we show that the rotor remains localized up to a characteristic harmonic frequency that can realistically exceed the excitation energies of the bath, enabling access to ultrafast rotating impurities. In the co-rotating frame, the bath excitations experience a rotational Doppler shift, generating angular-momentum-resolved resonances absent in equilibrium angulon theory. We identify a dissipative rotational sound barrier at which the molecule resonantly emits bath excitations and undergoes strong angular momentum exchange with the surrounding medium. Overall, we establish the dynamical phase diagram of the driven rotor in a quantum solvent and introduce a generic platform for investigating fast driven rotating impurities in quantum many-body systems.
The first minimum appearing in molecular rotational constants as a function of helium droplet size has been previously associated with the onset of superfluidity in these finite systems. We investigate this relationship by bosonic density functional theory calculations of classical molecular rotors (OCS, N2O, CO, and HCN) interacting with the surrounding helium. The calculated rotational constants are in fair agreement with the existing experimental data, demonstrating the applicability of the theoretical model. Inspection of the spatial evolution of the global phase and density shows the increase in the rotational constant after the first minimum correlates with continuous coverage of the molecule by helium and the appearance of angular phase coherence rather than completion of the first solvent shell. We assign the observed phenomenon to quantum phase transition between a localized state and one-dimensional superfluid, which represents the onset of rotational superfluidity in small helium droplets.