Lawrence Berkeley National Laboratory

Quantum fluid droplets made of helium-3 (³He) or helium-4 (⁴He) isotopes have long been considered as ideal cryogenic nanolabs, enabling unique ultracold chemistry and spectroscopy applications. The droplets were believed to provide a homogeneous environment in which dopant atoms and molecules could move and react almost as in free space but at temperatures close to absolute zero. Here, we report ultrafast x-ray diffraction experiments on xenon-doped ³He and ⁴He nanodroplets, demonstrating that the unavoidable rotational excitation of isolated droplets leads to highly anisotropic and inhomogeneous interactions between the host matrix and enclosed dopants. Superfluid ⁴He droplets are laced with quantum vortices that trap the embedded particles, leading to the formation of filament-shaped clusters. In comparison, dopants in ³He droplets gather in diffuse, ring-shaped structures along the equator. The shapes of droplets carrying filaments or rings are direct evidence that rotational excitation is the root cause for the inhomogeneous dopant distributions.