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arXiv:2605.17835

Coherent spectroscopy of collective excitations in superfluid helium far from equilibrium

Gabriel Voith, Alexander A. Milner, Michael J. Desrochers, Philip C. E. Stamp, Valery Milner

cond-mat.othercond-mat.quant-gasquant-phSubmitted May 18, 2026• Announced May 19, 2026• 0 citations• Revised Jun 21, 2026 (v2)
v1 · May 18, 2026v2 · Jun 21, 2026v3 · Aug 31, 2026
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Abstract

Ultrafast dynamics of collective excitations in superfluids remains largely unexplored beyond the roton region of the Landau excitation spectrum, despite the importance of such dynamics for understanding nonequilibrium processes in these systems. Here, we employ ultrafast coherent control with sequences of femtosecond pulses to perform spectroscopy of multiple quasiparticles in superfluid helium far from equilibrium. By measuring the time-resolved optical birefringence, we track the nonequilibrium dynamics of quasiparticle pairs associated with rotons, maxons and the Pitaevskii plateau region. The spectral lineshape of the roton peak is explained by an ab initio theoretical analysis of the roton-roton interaction. We also reveal strong energy shifts and short lifetimes of both maxon and Pitaevskii-plateau pairs, as well as an influence of the quasiparticle effective mass on the phase of their coherent response to laser pulses. These results demonstrate the ability to extract previously inaccessible information about collective excitations in a strongly interacting quantum fluid by probing its nonequilibrium dynamics on picosecond and sub-picosecond timescales.

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•Nov 28, 2022•1 citation
Ultrafast dynamics of collective excitations in superfluids remains largely unexplored beyond the roton region of the Landau excitation spectrum, despite the importance of such dynamics for understanding nonequilibrium processes in these systems. Here, we employ ultrafast coherent control with sequences of femtosecond pulses to perform spectroscopy of multiple quasiparticles in superfluid helium far from equilibrium. By measuring the time-resolved optical birefringence, we track the nonequilibrium dynamics of quasiparticle pairs associated with rotons, maxons and the Pitaevskii plateau region. The spectral lineshape of the roton peak is explained by an ab initio theoretical analysis of the roton-roton interaction. We also reveal strong energy shifts and short lifetimes of both maxon and Pitaevskii-plateau pairs, as well as an influence of the quasiparticle effective mass on the phase of their coherent response to laser pulses. These results demonstrate the ability to extract previously inaccessible information about collective excitations in a strongly interacting quantum fluid by probing its nonequilibrium dynamics on picosecond and sub-picosecond timescales.
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.
Dilute quantum gases offer a controllable platform for investigating quantum liquids, such as superfluid helium, in which correlations and fluctuations are encoded in the form of a quasiparticle energy (i.e., roton-maxon) dispersion. An approach to extracting the roton-maxon spectrum of a Bose-Einstein condensate is theoretically developed: the method relies on using an external one-dimensional optical lattice that effectively controls the response of the system, giving access to its elementary excitations.
The paradoxes and disparities in the contemporary microscopic theory of superfluid helium (He–II) are discussed along with possible ways of resolving them by taking pair correlations of He4 atoms into consideration. It is shown that most paradoxes are associated with the commonly accepted initial assumption concerning the dominating role of single-particle Bose condensate (SPBC) in the quantum microstructure of the superfluid component ρs. The existence of intensive SPBC leads to a strong hybridization of the elementary excitation branches and to a common dispersion law for all boson branches, which is identified with the quasiparticle spectrum E(p) observed experimentally from slow neutron scattering in liquid helium. However, the stability of this spectrum during a transition through the λ-point and the large value of the gap in the vicinity of the “rotonic” minimum contradict both the Landau theoretical criterion of superfluidity and the small value of experimentally measured critical velocity. At the same time, a strong interaction between particles in the Bose liquid He4 strongly suppresses the SPBC which amounts to less than 1% of all He4 atoms and hence cannot be the main constituent of the superfluid component, unlike the case of a weakly nonideal Bose gas. Moreover, for a quite strong attraction between particles in a certain region of the momentum space, bound pairs of bosons can be formed in the superfluid Bose liquid, and a coherent pair condensate (CPC) analogous to the Cooper pair condensate in superconductors may appear. Such a strong CPC may completely suppress the weak SPBC. In this case, the one-particle spectrum ε(p) of elementary excitations does not hybridize with the collective (two-particle) spectrum and does not appear in the structure of the dynamic form factor S(p,ε), i.e., does not coincide with the spectrum measured from neutron scattering. The dispersion of one-particle spectrum is defined by the momentum dependence of the pair order parameter Ψ̃(p) and may have a minimum or a point of inflection at p≠0. This peculiarity in the one-particle spectrum of a Bose liquid with CPC but without SPBC vanishes together with Ψ̃(p) at the temperature Tc=Tλ of the phase transition from the superfluid to the normal state (unlike the rotonic minimum in the collective spectrum), while the corresponding critical velocity vc=min[ε(p)/p] vanishes at the λ-point in accordance with the Landau criterion and the experimental data. The assumption that the strong “Cooper-like” CPC is responsible for the quantum structure of the superfluid component ρs is confirmed indirectly by the successful application of the Justrow approximation (based on strong pair correlations) for describing the properties of liquid He4 and quantum liquid mixtures He3–4He on one hand, and by an anomalously large effective mass of He3 impurity atoms in He4, which is approximately equal to total mass of He3 and He4 atoms, thus pointing to the existence of helium atoms in superfluid liquid He–II. The value of the superfluid velocity circulation quantum in the Onsager–Feynman vortices in a Bose liquid with CPC but without SPBC is discussed as well as the critical velocities of superfluid He4 in ultrathin films and channels in which the creation and motion of quantum vortices are ruled out, and the quasiparticle spectrum undergoes dimensional quantization.
Interactions between particles in quantum many-body systems play a crucial role in determining the electric, magnetic, optical, and thermal properties of the system. The recent progress in the laser-pulse technique has enabled the manipulations and measurements of physical properties on ultrafast timescales. Here we propose a method for the direct and ultrafast probing of quantum many-body interaction through coherent two-dimensional (2D) spectroscopy. Using a two-band fermionic Hubbard model for the minimum two-site lattice system, we find that the 2D spectrum of a noninteracting system contains only diagonal peaks; the interparticle interaction manifests itself in the emergence of off-diagonal peaks in the 2D spectrum before all the peaks coalesce into a single diagonal peak as the system approaches the strongly interacting limit. The evolution of the 2D spectrum as a function of the time delay between the second and third laser pulses can provide important information on the ultrafast time variation of the interaction.
Excitons-polaritons of semiconductor microcavities are quasiparticles originating from the dressing of optical cavity photons by the interactions between quantum well electron-hole pairs. In planar geometry, their belonging to the family of quantum fluids has been many times demonstrated through the observation of macroscopic coherence phenomena, such as superfluidity and Bose-Einstein condensation. Like ultracold atoms, polaritons support on their surface a set of collective excitations, the Bogoliubov modes, whose spectrum encompasses the key information to describe the dynamics of quantum fluids. In this thesis, we present a wide variety of results concerning the detection and control of such modes in different configurations. Thanks to the development of a new high-resolution coherent spectroscopy method, we carried out a detailed study of the spectrum of polariton collective excitations. In particular, we highlighted the effects of the driven-dissipative nature of the system on the fundamental dynamics of the fluid, by investigating the interplay between the Bogoliubov modes and the polariton bistability under coherent pumping. This was the opportunity to reveal, in addition to the well-known phonon-type excitations, precursors of dynamical instability and the so-called ghost branch. Moreover, we studied the behavior of out-of-equilibrium phase transitions: first, via the effect of the system dimension on the bistability and, second, with the onset of a Goldstone mode, as a result of a spontaneous symmetry breaking in a parametric oscillation regime. Finally, we designed a pumping geometry that directly controls the instability modes between dark solitons of a pair guided by an intensity channel, leading to the formation of vortex-antivortex streets in the density.