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Science

Shapes and vorticities of superfluid helium nanodroplets

Luis F. Gomez, Ken Ferguson, James Patrick Cryan, Camila Bacellar, Rico Mayro P. Tanyag, Curtis F. Jones, Sebastian Schorb, Denis Anielski, A. Belkacem, Charles Bernando, Rebecca Boll, John D. Bozek, S. Carron, Gang Chen, Tjark Delmas, Lars Englert, Sascha W. Epp, Benjamin Erk, L. Foucar, Robert Hartmann, Alexander Hexemer, Martin Huth, Justin Kwok, Stephen R. Leone, H. Jonathan, Filipe R. N. C. Maia, Erik Malmerberg, Stefano Marchesini, Daniel M. Neumark, Billy K. Poon, James S. Prell, Daniel Rolles, Benedikt Rudek, Artem Rudenko, Martin T. Seifrid, Katrin R. Siefermann, Felix P. Sturm, Michele L. Swiggers, J. Ullrich, Fabian Weise, Petrus H. Zwart, Christoph Bostedt, Oliver Geßner, Andrey F. Vilesov

Published Aug 21, 2014• 230 citations
Publisher

Abstract

Helium nanodroplets are considered ideal model systems to explore quantum hydrodynamics in self-contained, isolated superfluids. However, exploring the dynamic properties of individual droplets is experimentally challenging. In this work, we used single-shot femtosecond x-ray coherent diffractive imaging to investigate the rotation of single, isolated superfluid helium-4 droplets containing ~10(8) to 10(11) atoms. The formation of quantum vortex lattices inside the droplets is confirmed by observing characteristic Bragg patterns from xenon clusters trapped in the vortex cores. The vortex densities are up to five orders of magnitude larger than those observed in bulk liquid helium. The droplets exhibit large centrifugal deformations but retain axially symmetric shapes at angular velocities well beyond the stability range of viscous classical droplets.

DOI
10.1126/science.1252395

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Helium nanodroplets are considered ideal model systems to explore quantum hydrodynamics in self-contained, isolated superfluids. However, exploring the dynamic properties of individual droplets is experimentally challenging. In this work, we used single-shot femtosecond x-ray coherent diffractive imaging to investigate the rotation of single, isolated superfluid helium-4 droplets containing ~10(8) to 10(11) atoms. The formation of quantum vortex lattices inside the droplets is confirmed by observing characteristic Bragg patterns from xenon clusters trapped in the vortex cores. The vortex densities are up to five orders of magnitude larger than those observed in bulk liquid helium. The droplets exhibit large centrifugal deformations but retain axially symmetric shapes at angular velocities well beyond the stability range of viscous classical droplets.
Helium nanodroplets are considered ideal model systems to explore quantum hydrodynamics in self-contained, isolated superfluids. Rotation of a superfluid droplet is manifested as a collection of quantum vortices. Here, the authors use single-shot femtosecond X-ray coherent diffractive imaging to investigate the shapes and vorticity of rotating superfluid 4{}^{4}4He droplets. They find that most of the diffraction contours exhibit noticeable ellipticity. A smaller but still significant number of distorted diffraction contours are marked by regions of high intensity concentrated along the direction of the long axis in the diffraction image, indicating the presence of extremely deformed 4{}^{4}4He droplets. Forward modeling of the diffraction images shows that the shapes of superfluid 4{}^{4}4He droplets are very similar to their classical counterparts. In particular, the existence of both axially symmetric (oblate) and, for higher angular momenta, two-lobed (triaxial prolate) droplets is revealed. The latter shapes are strongly deformed compared to the spheroidal bodies that are expected for smaller rotational speeds. The observed shapes provide direct access to the droplet angular momenta, angular velocities, and estimated number of quantum vortices inside the droplets.
Superfluid helium nanodroplets are an ideal environment for the formation of metastable, self-organized dopant nanostructures. However, the presence of vortices often hinders their formation. Here, we demonstrate the generation of vortex-free helium nanodroplets and explore the size range in which they can be produced. From x-ray diffraction images of xenon-doped droplets, we identify that single compact structures, assigned to vortex-free aggregation, prevail up to 10810^8108 atoms per droplet. This finding builds the basis for exploring the assembly of far-from-equilibrium nanostructures at low temperatures.
A significant fraction of superfluid helium nanodroplets produced in a free-jet expansion has been observed to gain high angular momentum resulting in large centrifugal deformation. We measured single-shot diffraction patterns of individual rotating helium nanodroplets up to large scattering angles using intense extreme ultraviolet light pulses from the FERMI free-electron laser. Distinct asymmetric features in the wide-angle diffraction patterns enable the unique and systematic identification of the three-dimensional droplet shapes. The analysis of a large data set allows us to follow the evolution from axisymmetric oblate to triaxial prolate and two-lobed droplets. We find that the shapes of spinning superfluid helium droplets exhibit the same stages as classical rotating droplets while the previously reported metastable, oblate shapes of quantum droplets are not observed. Our three-dimensional analysis represents a valuable landmark for clarifying the interrelation between morphology and superfluidity on the nanometer scale.
Superfluid helium nanodroplets are an ideal environment for the formation of metastable, self-organized dopant nanostructures. However, the presence of vortices often hinders their formation. Here, we demonstrate the generation of vortex-free helium nanodroplets and explore the size range in which they can be produced. From x-ray diffraction images of xenon-doped droplets, we identify that single compact structures, assigned to vortex-free aggregation, prevail up to 10^{8} atoms per droplet. This finding builds the basis for exploring the assembly of far-from-equilibrium nanostructures at low temperatures.
Free superfluid helium droplets constitute a versatile medium for a diverse range of experiments in physics and chemistry that extend from studies of the fundamental laws of superfluid motion to the synthesis of novel nanomaterials. In particular, the emergence of quantum vortices in rotating helium droplets is one of the most dramatic hallmarks of superfluidity and gives detailed access to the wave function describing the quantum liquid. This review provides an introduction to quantum vorticity in helium droplets, followed by a historical account of experiments on vortex visualization in bulk superfluid helium and a more detailed discussion of recent advances in the study of the rotational motion of isolated, nano- to micrometer-scale superfluid helium droplets. Ultrafast X-ray and extreme ultraviolet scattering techniques enabled by X-ray free-electron lasers and high-order harmonic generation in particular have facilitated the in situ detection of droplet shapes and the imaging of vortex structures inside individual, isolated droplets. New applications of helium droplets ranging from studies of quantum phase separations to mechanisms of low-temperature aggregation are discussed.
Single He nanodroplets doped with Xe atoms are studied via ultrafast coherent x-ray diffraction imaging. The diffraction images show that rotating He nanodroplets about 200 nm in diameter contain a small number of symmetrically arranged quantum vortices decorated with Xe clusters. Unexpected large distances of the vortices from the droplet center ($\ensuremath{\approx}0.7\text{--}0.8$ droplet radii) are explained by a significant contribution of the Xe dopants to the total angular momentum of the droplets and a stabilization of widely spaced vortex configurations by the trapped Xe clusters.