Abstract
X-ray free-electron lasers (XFELs) deliver ultrashort coherent laser pulses in the X-ray spectral regime, enabling novel investigations into the structure of individual nanoscale samples. In this work, we demonstrate how single-shot small-angle X-ray scattering (SAXS) measurements combined with fluorescence and ion time-of-flight (TOF) spectroscopy can be used to obtain size- and structure-selective evaluation of the light-matter interaction processes on the nanoscale. We recorded the SAXS images of single xenon clusters using XFEL pulses provided by the SPring-8 Angstrom compact free-electron laser (SACLA). The XFEL fluences and the radii of the clusters at the reaction point were evaluated and the ion TOF spectra and fluorescence spectra were sorted accordingly. We found that the XFEL fluence and cluster size extracted from the diffraction patterns showed a clear correlation with the fluorescence and ion TOF spectra. Our results demonstrate the effectiveness of the multispectroscopic approach for exploring laser–matter interaction in the X-ray regime without the influence of the size distribution of samples and the fluence distribution of the incident XFEL pulses.
Highlights
The development of free-electron lasers (FEL) has enabled novel studies into the structure and dynamics of various forms of matter under extreme conditions, ranging from atoms and molecules [1,2,3,4]to condensed matter [5,6,7]
The hit rate determined by the ratio of observed small-angle X-ray scattering (SAXS) signals in the octal multiport charge-coupled device (MPCCD) sensor to the total number of FEL shots was less than 0.1%
These results indicate that X-ray free-electron lasers (XFELs)–cluster interaction can be studied more accurately using size- and fluence-selective measurements, i.e., by eliminating the washout of characteristics of single targets due to their size distribution and laser profile [18,22,33,34]
Summary
The development of free-electron lasers (FEL) has enabled novel studies into the structure and dynamics of various forms of matter under extreme conditions, ranging from atoms and molecules [1,2,3,4]to condensed matter [5,6,7]. The development of free-electron lasers (FEL) has enabled novel studies into the structure and dynamics of various forms of matter under extreme conditions, ranging from atoms and molecules [1,2,3,4]. Atomic clusters are an ideal model system for this research Their size is tunable and they are isolated systems with bulk density. Experimental studies started with ion spectrometry, from which, unexpected energetic ion emissions, even in the short wavelength (extreme ultraviolet to X-ray) regime, were reported [9]. This stimulated discussion regarding the dynamics in clusters based on the spectra obtained by averaging over the ensemble of shots of the incident laser pulses. Pioneering works [18,22,33,34] revealed that the properties of individual particles are concealed by the accumulation of spectra due to the laser profile and to the size distribution and structural isomers of clusters originating from the generation methods
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