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arXiv:2501.16066 · The Journal of Chemical Physics

Environment-limited transfer of angular momentum in Bose liquids

Alberto Cappellaro, Giacomo Bighin, Igor N. Cherepanov, Mikhail Lemeshko

Published Feb 18, 2025• 0 citations
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Abstract

Impurity motion in a many-body environment has been a central issue in the field of low-temperature physics for decades. In bosonic quantum fluids, the onset of a drag force experienced by point-like objects is due to collective environment excitations, driven by the exchange of linear momentum between the impurity and the many-body bath. In this work we consider a rotating impurity, with the aim of exploring how angular momentum is exchanged with the surrounding bosonic environment. In order to elucidate these issues, we employ a quasiparticle approach based on the angulon theory, which allows us to effectively deal with the non-trivial algebra of quantized angular momentum in the presence of a many-body environment. We uncover how impurity dressing by environmental excitations can establish an exchange channel, whose effectiveness crucially depends on the initial state of the impurity. Remarkably, we find that there is a critical value of initial angular momentum, above which this channel effectively freezes.

DOI
10.1063/5.0253451

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Impurity motion in a many-body environment has been a central issue in the field of low-temperature physics for decades. In bosonic quantum fluids, the onset of a drag force experienced by point-like objects is due to collective environment excitations, driven by the exchange of linear momentum between the impurity and the many-body bath. In this work we consider a rotating impurity, with the aim of exploring how angular momentum is exchanged with the surrounding bosonic environment. In order to elucidate these issues, we employ a quasiparticle approach based on the angulon theory, which allows us to effectively deal with the non-trivial algebra of quantized angular momentum in the presence of a many-body environment. We uncover how impurity dressing by environmental excitations can establish an exchange channel, whose effectiveness crucially depends on the initial state of the impurity. Remarkably, we find that there is a critical value of initial angular momentum, above which this channel effectively freezes.
The angulon, a quasiparticle formed by a quantum rotor dressed by the excitations of a many-body bath, can be used to describe an impurity rotating in a fluid or solid environment. Here, we propose a coherent state ansatz in the co-rotating frame, which provides a comprehensive theoretical description of angulons. We reveal the quasiparticle properties, such as energies, quasiparticle weights, and spectral functions, and show that our ansatz yields a persistent decrease in the impurity's rotational constant due to many-body dressing, which is consistent with experimental observations. From our study, a picture of the angulon emerges as an effective spin interacting with a magnetic field that is self-consistently generated by the molecule's rotation. Moreover, we discuss rotational spectroscopy, which focuses on the response of rotating molecules to a laser perturbation in the linear response regime. Importantly, we take into account initial-state interactions that have been neglected in prior studies and reveal their impact on the excitation spectrum. To examine the angulon instability regime, we use a single-excitation ansatz and obtain results consistent with experiments, in which a broadening of spectral lines is observed while phonon wings remain highly suppressed due to initial-state interactions.
Feynman diagrams represent one of the most powerful techniques of modern many-particle theory. Applying such diagrammatic techniques to many-body processes involving angular momentum is, however, substantially challenging. Here, the authors introduce a diagrammatic approach to the angulon quasiparticle, which consists of an orbital quantum impurity -- such as a molecule or electron -- exchanging angular momentum with a bath of bosons (superfluid, lattice phonons). The new approach fuses the Feynman diagrams of solid-state physics with the angular momentum diagrams previously used in atomic and nuclear structure calculations.
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.
During the past 70 years, the quantum theory of angular momentum has been successfully applied to describing the properties of nuclei, atoms, and molecules, and their interactions with each other as well as with external fields.Because of the properties of quantum rotations, the angular-momentum algebra can be of tremendous complexity even for a few interacting particles, such as valence electrons of an atom, not to mention larger many-particle systems.In this work, we study an example of the latter: a rotating quantum impurity coupled to a many-body bosonic bath.In the regime of strong impurity-bath couplings, the problem involves the addition of an infinite number of angular momenta, which renders it intractable using currently available techniques.Here, we introduce a novel canonical transformation that allows us to eliminate the complex angular-momentum algebra from such a class of many-body problems.In addition, the transformation exposes the problem's constants of motion, and renders it solvable exactly in the limit of a slowly rotating impurity.We exemplify the technique by showing that there exists a critical rotational speed at which the impurity suddenly acquires one quantum of angular momentum from the many-particle bath.Such an instability is accompanied by the deformation of the phonon density in the frame rotating along with the impurity.
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.
It is a common knowledge that an effective interaction of a quantum impurity with an electromagnetic field can be screened by surrounding charge carriers, whether mobile or static. Here we demonstrate that very strong, "anomalous" screening can take place in the presence of a neutral, weakly polarizable environment, due to an exchange of orbital angular momentum between the impurity and the bath. Furthermore, we show that it is possible to generalize all phenomena related to isolated impurities in an external field to the case when a many-body environment is present, by casting the problem in terms of the angulon quasiparticle. As a result, the relevant observables such as the effective Rabi frequency, geometric phase, and impurity spatial alignment are straightforward to evaluate in terms of a single parameter: the angular-momentum-dependent screening factor.