Equilibrium and non-equilibrium phases of microwave-dressed polar molecules beyond rotational symmetries

Abstract

Recent experiments on molecular droplets have opened a new frontier of self-organization in strongly dipolar quantum matter. Microwave-dressing of polar molecules permits to tune both the strength and the angular structure of long-range interactions, potentially promoting a rich spectrum of quantum phases, from superfluid droplets with varying geometry and insulating or supersolid droplet arrays to strongly correlated crystals of individual molecules. Using path-integral Monte Carlo simulations of large molecular ensembles, we demonstrate that experimentally observed droplet arrays emerge as a metastable non-equilibrium state from the quenching of a gas-droplet phase transition under entirely broken rotational symmetry of the microwave-induced interaction potential. We moreover find that a crystalline phase of molecules, predicted for antidipolar interactions, is absent under conditions of recent experiments. This is traced back to the lack of angular symmetry in currently employed microwave-dressing, which qualitatively reshapes the many-body energy landscape and cannot be captured by effective scalar interaction parameters. Our results provide the first direct comparison of ab initio simulations and experiments and establish interaction anisotropy as a key aspect of molecular quantum gases.