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arXiv:2609.05344

How dipolar interactions structure molecular droplets

Wiiliam Freitas, Panagiotis Giannakeas, Jan M. Rost

cond-mat.quant-gasquant-phSubmitted Sep 4, 2026• Announced Sep 7, 2026• 0 citations
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Abstract

We investigate how dipolar interactions between microwave-shielded polar molecules structure the self-bound droplets formed under variation of the interaction strength. We identify the transition from droplets to crystals as a finite-size first order transition. With droplet-ring states and transitional supersolid states we predict additional structure in the crystal and droplet phases, respectively. To describe this strongly correlated regime, and in particular the reconfiguration of quantum ground states, we design a variational Monte Carlo framework based on neural quantum states. It is especially suitable to describe ground states and almost degenerate states with very different configurations. Moreover, one can easily determine the superfluid fraction. Our results reveal the sequence of finite-size structures through which dipolar interactions reorganize molecular droplets into crystals.

Comments
7 pages, 8 figures

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We investigate how dipolar interactions between microwave-shielded polar molecules structure the self-bound droplets formed under variation of the interaction strength. We identify the transition from droplets to crystals as a finite-size first order transition. With droplet-ring states and transitional supersolid states we predict additional structure in the crystal and droplet phases, respectively. To describe this strongly correlated regime, and in particular the reconfiguration of quantum ground states, we design a variational Monte Carlo framework based on neural quantum states. It is especially suitable to describe ground states and almost degenerate states with very different configurations. Moreover, one can easily determine the superfluid fraction. Our results reveal the sequence of finite-size structures through which dipolar interactions reorganize molecular droplets into crystals.
We investigate the physics of ultracold dipolar molecules using path-integral quantum Monte Carlo simulations, and construct the complete phase diagram extending from weak to strong interactions and from small to mesoscopic particle numbers. Our calculations predict the formation of self-bound quantum droplets at interaction strengths lower than previous estimates for molecular condensates. Strikingly, we observe that, for stronger interactions, the oblate quantum droplet transitions to a two-dimensional sheet or superfluid membrane with a thickness of a single molecule. As interactions are increased further the system continually loses superfluidity while correlations develop, and is eventually found to undergo a transition to a crystalline monolayer that remains self-bound without external confinement. The spontaneous formation of such two-dimensional phases from a three-dimensional quantum gas is traced back to the peculiar anisotropic form of the dipole-dipole interaction generated by microwave dressing of rotational molecular states. For sufficiently large particle numbers, crystallization takes place for comparably low interaction strengths that do not promote two-body bound states and should thus be observable in ongoing experiments without limitations from three-body recombination.
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.
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Recent experiments with degenerate molecular gases dressed by elliptically polarized microwave fields have enabled new control of dipolar interactions via engineered anisotropy. We reveal a symmetry structure of the dipolar interaction that generates degeneracies among the interaction parameters, enabling a classification of spatial symmetries and equilibrium shapes of the gases. Exploiting these symmetries, we analyze solutions including beyond-mean-field quantum fluctuations in the dilute gas regime and develop a complementary variational theory. We map out the phase diagram of self-bound droplets and characterize their widths, energies, and densities.
We propose a novel scheme to realize the supersolid phase in ultracold gases of microwave-shielded polar molecules by engineering an additional anisotropy in inter-molecular dipolar interaction via an elliptically polarized microwave. It is shown through quantum Monte-Carlo calculations that the interplay of the anisotropies between the interaction and trapping potential gives rise to rich quantum phases. Particularly, it is found that the supersolid phase emerges in the parameter regime accessible to current experiments. Our study paves the way for exploring the properties of supersolid phases in ultracold gases of polar molecules.
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