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arXiv:2608.27030

Crossing the Rotational Sound Barrier in a Quantum Solvent

Baptiste Coquinot, Giacomo Bighin, Mikhail Lemeshko, Ragheed Alhyder

cond-mat.quant-gascond-mat.mes-hallcond-mat.supr-conquant-phSubmitted Aug 27, 2026• Announced Aug 28, 2026• 0 citations
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Abstract

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.

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•Jan 1, 2020•0 citations
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.
We develop a microscopic theory describing a quantum impurity whose rotational degree of freedom is coupled to a many-particle bath. We approach the problem by introducing the concept of an "angulon"-a quantum rotor dressed by a quantum field-and reveal its quasiparticle properties using a combination of variational and diagrammatic techniques. Our theory predicts renormalization of the impurity rotational structure, such as that observed in experiments with molecules in superfluid helium droplets, in terms of a rotational Lamb shift induced by the many-particle environment. Furthermore, we discover a rich many-body-induced fine structure, emerging in rotational spectra due to a redistribution of angular momentum within the quantum many-body system.
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.
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.
We investigate a molecular quantum rotor in a two-dimensional Bose-Einstein condensate. The focus is on studying the angulon quasiparticle concept in the crossover from few- to many-body physics. To this end, we formulate the problem in real space and solve it with a mean-field approach in the frame co-rotating with the impurity. We show that the system starts to feature angulon characteristics when the size of the bosonic cloud is large enough to screen the rotor. More importantly, we demonstrate the departure from the angulon picture for large system sizes or large angular momenta where the properties of the system are determined by collective excitations of the Bose gas.
We investigate the in- and out-of-equilibrium phenomena of a rotational impurity—specifically, a linear molecule—coupled to a nonconventional environment, a helium nanodroplet. By employing a Lee-Low-Pines-like transformation combined with a multireference configuration approach, we self-consistently account for the molecule's backaction on the superfluid bath and accurately capture the complex entanglement between the molecule's rotational degrees of freedom and the bath excitations. Our findings reveal that in the ground state, the impurity induces a density defect in the superfluid bath, giving rise to two novel types of excited states: (a) attractive angulon states, analogous to bound states in photonic crystals and Yu-Shiba-Rusinov bound states in superconductors, localized within the density defect region, and (b) long-lived repulsive angulon states in dilute environments. Rotational spectroscopy demonstrates a crossover from repulsive to attractive angulon states as the bath density increases. This work paves the way for exploring novel nonequilibrium phenomena of quantum impurities in interacting environments.
The oft-quoted dictum by Arthur Schawlow: ``A diatomic molecule has one atom too many'' has been disavowed. Inspired by the possibility to experimentally manipulate and enhance chemical reactivity in helium nanodroplets, we investigate the rotation of coupled cold molecules in the presence of a many-body environment. In this thesis, we introduce new variational approaches to quantum impurities and apply them to the Fröhlich polaron - a quasiparticle formed out of an electron (or other point-like impurity) in a polar medium, and to the angulon - a quasiparticle formed out of a rotating molecule in a bosonic bath. With this theoretical toolbox, we reveal the self-localization transition for the angulon quasiparticle. We show that, unlike for polarons, self-localization of angulons occurs at finite impurity-bath coupling already at the mean-field level. The transition is accompanied by the spherical-symmetry breaking of the angulon ground state and a discontinuity in the first derivative of the ground-state energy. Moreover, the type of symmetry breaking is dictated by the symmetry of the microscopic impurity-bath interaction, which leads to a number of distinct self-localized states. For the system containing multiple impurities, by analogy with the bipolaron, we introduce the biangulon quasiparticle describing two rotating molecules that align with respect to each other due to the effective attractive interaction mediated by the excitations of the bath. We study this system from the strong-coupling regime to the weak molecule-bath interaction regime. We show that the molecules tend to have a strong alignment in the ground state, the biangulon shows shifted angulon instabilities and an additional spectral instability, where resonant angular momentum transfer between the molecules and the bath takes place. Finally, we introduce a diagonalization scheme that allows us to describe the transition from two separated angulons to a biangulon as a function of the distance between the two molecules.