Abstract
We have recorded the diffraction patterns from individual xenon clusters irradiated with intense extreme ultraviolet pulses to investigate the influence of light-induced electronic changes on the scattering response. The clusters were irradiated with short wavelength pulses in the wavelength regime of different 4d inner-shell resonances of neutral and ionic xenon, resulting in distinctly different optical properties from areas in the clusters with lower or higher charge states. The data show the emergence of a transient structure with a spatial extension of tens of nanometers within the otherwise homogeneous sample. Simulations indicate that ionization and nanoplasma formation result in a light-induced outer shell in the cluster with a strongly altered refractive index. The presented resonant scattering approach enables imaging of ultrafast electron dynamics on their natural timescale.
Highlights
Intense femtosecond short-wavelength pulses from free-electron lasers (FELs) open new avenues to investigate transient states and ultrafast processes with unprecedented spatial and temporal resolution.[1,2,3,4] One prominent example is ultrafast x-ray diffraction methods such as femtosecond Coherent Diffraction Imaging (CDI), which have enabled the structure determination of individual nonperiodic nanoscale objects.[5]
The encoded structural information can be retrieved via phase retrieval methods[8] or forward simulations,[9] which allowed for the structural characterization of such fragile objects as single viruses,[10,11] aerosols,[12,13]
Via pump-probe techniques, laser-induced processes in individual nanoparticles can be studied in a timeresolved manner with unprecedented spatiotemporal resolution.[18,19,20,21,22]. Such studies are pivotal for understanding and mitigating the damage dynamics from ionization, plasma formation, and particle explosion, which limit the achievable resolution in CDI experiments.[7,23]
Summary
Intense femtosecond short-wavelength pulses from free-electron lasers (FELs) open new avenues to investigate transient states and ultrafast processes with unprecedented spatial and temporal resolution.[1,2,3,4] One prominent example is ultrafast x-ray diffraction methods such as femtosecond Coherent Diffraction Imaging (CDI), which have enabled the structure determination of individual nonperiodic nanoscale objects.[5] The elastically scattered photons of a single-shot exposure form an interference pattern containing a snapshot of the object before it is quickly destroyed due to the large amount of deposited energy.[6,7] The encoded structural information can be retrieved via phase retrieval methods[8] or forward simulations,[9] which allowed for the structural characterization of such fragile objects as single viruses,[10,11] aerosols,[12,13]. Scitation.org/journal/sdy atomic clusters,[9,14,15] and even superfluid helium nanodroplets containing quantum vortices.[16,17] Via pump-probe techniques, laser-induced processes in individual nanoparticles can be studied in a timeresolved manner with unprecedented spatiotemporal resolution.[18,19,20,21,22] Such studies are pivotal for understanding and mitigating the damage dynamics from ionization, plasma formation, and particle explosion, which limit the achievable resolution in CDI experiments.[7,23]
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