Attractive and repulsive angulons in superfluid environments

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.