X‑ray Coherent Diffractive Imaging of Large Helium Nanodroplets Doped with Small Molecules

Journal Article · Mon Dec 22 00:00:00 EST 2025 · Journal of Physical Chemistry A

DOI:https://doi.org/10.1021/acs.jpca.5c07766· OSTI ID:3012942

Feinberg, AlexandraJ; Singh, Amandeep; Saladrigas, Catherine A; Stein, Landin; Verma, Deepak; O’Connell-Lopez, Sean M O; Erukala, Swetha; Toulson, Benjamin W; Borgwardt, Mario; Shivaram, Niranjan H; Lin, Ming-Fu; Al Haddad, Andre; Jäger, Wolfgang; Bostedt, Christoph; Walter, Peter; Gessner, Oliver; Vilesov, Andrey F

We report the first X-ray coherent diffractive imaging experiment on molecule-doped helium nanodroplets. It complements previous work, where we reported single-shot X-ray coherent diffractive imaging studies of Xe dopant clusters formed in 4He and 3He droplets. These noble gas clusters were used to visualize the impact of rotational excitation of the droplets on the spatial distribution of atomic dopants within the droplets, and to study the differences and connections between quantum and classical droplet rotational motion. Here, we expand our studies to the molecular dopants CF4, CHF3, CH3CN, and SF6, imaged with 1.5 keV photons. We find multiple Bragg spots in the diffraction patterns of molecule-doped droplets with radii of approximately 600 nm, which provide evidence that molecules form elongated clusters with preferential alignment along the angular momentum axis of the 4He droplets, in agreement with our previous results on the aggregation of Xe clusters on quantum vortices. Real-space reconstructions of molecular dopant cluster density profiles are obtained for droplets with smaller radii of approximately 300 nm. The diffuse images suggest the formation of low-density, potentially porous, molecular clusters upon aggregation at T = 0.4 K in 4He droplets. In the normal fluid 3He droplets, molecules aggregate into loose clusters on the droplets' equator, similar to previous observations for Xe atoms. Time-of-flight mass spectra reveal that the doped helium nanodroplet moieties fragment extensively into constituent atomic ions, producing only a small fraction of molecular fragment ions. The findings are discussed in the context of previously proposed schemes to use He droplets as potential tamper materials for ultrafast X-ray imaging experiments.

• Research Organization: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
• Sponsoring Organization: US Department of Energy; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB) (SC-CSGB)
• Grant/Contract Number: AC02-05CH11231
• OSTI ID: 3012942
• Journal Information: Journal of Physical Chemistry A, Journal Name: Journal of Physical Chemistry A Journal Issue: 1 Vol. 130
• Country of Publication: United States
• Language: English