Three-Dimensional Shapes of Spinning Helium Nanodroplets

A significant fraction of superfluid helium nanodroplets produced in a free-jet expansion have 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 dataset 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

Orientation, rotation and solvation of ions in helium nanodroplets

Helium nanodroplets are liquid, finite size, nanoscale helium clusters that have been employed since the 1990s as a matrix for high-resolution spectroscopy of molecules. Spectroscopic studies of ionic species inside helium droplets were not however realised until 2010, even though the potential information about their structure is of special interest since they are fundamental reaction intermediates in biochemistry. Additionally, the interaction of these species with the helium environment can be determined from these experiments, which is interesting from a fundamental point of view. To determine structural information and study product selectivity, we proposed using high electric fields to orient the molecular ions in helium nanodroplets. Pendular state spectroscopy of neutral polar molecules in helium nanodroplets in the presence of electric fields has previously given satisfactory results to achieve molecular orientation, allowing one to distinguish biomolecular isomers. Our first experiments validated the technique for neutral aniline since the polarisation difference ratios, which express the degree of orientation, obtained from the NH2-stretch transitions were well-reproduced by calculations. On the other hand, the measured degree of orientation of cationic aniline is noticeably smaller than calculations show. Even so, the variation of the degree of orientation with electric field lets us conclude that orientation of the ions in helium droplets was observed. The results of several experiments performed to investigate the possible effects influencing the apparent orientation of the cations did not lead to any straightforward explanation. Our study therefore shows that orientation of molecular ions indeed seems possible and leads the way to possible future experiments. To examine the formation of ionic-alkali solvation complexes in helium droplets upon photoionisation of the alkali, sodium, and understand the helium-dopant interaction we have performed ion spectroscopy. We found that several scenarios are possible after ionisation including dissociation, solvation and complete solvent evaporation depending on the ionisation process, droplet size and number of water ligands considered. Direct ionisation of sodium leads to solvation in the droplet, collision with the water molecules and formation of the ionic complexes if the droplet size is sufficiently large. For these conditions, rovibrational spectroscopy of Na(OH2)+ was performed to obtain the A rotational constant in helium droplets and thus determine if the dopant-helium interaction affects the moment of inertia. From the results, we could confirm the latter but could not deduce the extent to which this was the case. This study shows how the spectral information of the solvated ions is useful to understand complexation dynamics in helium droplets and acquire further understanding about the dopant-helium interaction

Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets

We explore the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump–probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation with near-infrared laser pulses. After a variable time delay of up to 800 ps, we image the subsequent dynamics using intense extreme ultraviolet pulses from the FERMI free-electron laser. The recorded scattering images exhibit complex intensity fluctuations that are categorized based on their characteristic features. Systematic simulations of wide-angle diffraction patterns are performed, which can qualitatively explain the observed features by employing model shapes with both randomly distributed as well as structured, symmetric distortions. This points to a connection between the dynamics and the positions of the dopants in the droplets. In particular, the structured fluctuations might be governed by an underlying array of quantized vortices in the superfluid droplet as has been observed in previous small-angle diffraction experiments. Our results provide a basis for further investigations of dopant–droplet interactions and associated heating mechanisms.ISSN:1367-263

Diffraction imaging of light induced dynamics in xenon-doped helium nanodroplets

We have explored the light induced dynamics in superfluid helium nanodroplets with wide-angle scattering in a pump-probe measurement scheme. The droplets are doped with xenon atoms to facilitate the ignition of a nanoplasma through irradiation with near-infrared laser pulses. After a variable time delay of up to 800 ps, we image the subsequent dynamics using intense extreme ultraviolet pulses from the FERMI free-electron laser. The recorded scattering images exhibit complex intensity fluctuations that are categorized based on their characteristic features. Systematic simulations of wide-angle diffraction patterns are performed, which can qualitatively explain the observed features by employing model shapes with both randomly distributed as well as structured, symmetric distortions. This points to a connection between the dynamics and the positions of the dopants in the droplets. In particular, the structured fluctuations might be governed by an underlying array of quantized vortices in the superfluid droplet as has been observed in previous small-angle diffraction experiments. Our results provide a basis for further investigations of dopant-droplet interactions and associated heating mechanisms

SARS-CoV-2 vaccination modelling for safe surgery to save lives: data from an international prospective cohort study

Background: Preoperative SARS-CoV-2 vaccination could support safer elective surgery. Vaccine numbers are limited so this study aimed to inform their prioritization by modelling. Methods: The primary outcome was the number needed to vaccinate (NNV) to prevent one COVID-19-related death in 1 year. NNVs were based on postoperative SARS-CoV-2 rates and mortality in an international cohort study (surgical patients), and community SARS-CoV-2 incidence and case fatality data (general population). NNV estimates were stratified by age (18-49, 50-69, 70 or more years) and type of surgery. Best- and worst-case scenarios were used to describe uncertainty. Results: NNVs were more favourable in surgical patients than the general population. The most favourable NNVs were in patients aged 70 years or more needing cancer surgery (351; best case 196, worst case 816) or non-cancer surgery (733; best case 407, worst case 1664). Both exceeded the NNV in the general population (1840; best case 1196, worst case 3066). NNVs for surgical patients remained favourable at a range of SARS-CoV-2 incidence rates in sensitivity analysis modelling. Globally, prioritizing preoperative vaccination of patients needing elective surgery ahead of the general population could prevent an additional 58 687 (best case 115 007, worst case 20 177) COVID-19-related deaths in 1 year. Conclusion: As global roll out of SARS-CoV-2 vaccination proceeds, patients needing elective surgery should be prioritized ahead of the general population