X-ray crystallography has traditionally been limited to the study of the groundstate structure of molecules and solids. 2À ], performed at helium temperatures with synchrotron radiation. The shortening of the PtÐPt bond by 0.28 (9) A Ê upon excitation is compatible with the proposed mechanism involving promotion of a PtÐPt antibonding d'* electron to a weakly bonding p orbital. The contraction is accompanied by a 3 molecular rotation. The time-resolved diffraction technique described here is applicable to reversible light-driven processes in the crystalline solid state.
X-ray emission spectroscopy (XES) is a powerful element-selective tool to analyze the oxidation states of atoms in complex compounds, determine their electronic configuration, and identify unknown compounds in challenging environments. Until now the low efficiency of wavelength-dispersive X-ray spectrometer technology has limited the use of XES, especially in combination with weaker laboratory X-ray sources. More efficient energy-dispersive detectors have either insufficient energy resolution because of the statistical limits described by Fano or too low counting rates to be of practical use. This paper updates an approach to high-resolution X-ray emission spectroscopy that uses a microcalorimeter detector array of superconducting transition-edge sensors (TESs). TES arrays are discussed and compared with conventional methods, and shown under which circumstances they are superior. It is also shown that a TES array can be integrated into a table-top time-resolved X-ray source and a soft X-ray synchrotron beamline to perform emission spectroscopy with good chemical sensitivity over a very wide range of energies.
A plasma source free from characteristic emission lines is described, based on laser irradiation of a water jet in a helium atmosphere. Various key aspects of the laser interaction are presented along with practical characterization of the observed isotropic approximately 4-10 keV x-ray emissions, measurements of which indicate subpicosecond duration. Observations are consistent with a vacuum heating plasma mechanism at the helium-water interface and indicate strong potential for in-house ultrafast chemical structure dynamics application when coupled to contemporary detector developments.
Examinations of bremsstrahlung and energetic electron beams from a novel laser plasma source motivate and assist characterization of a backthinned, backilluminated direct detection x-ray charge-coupled device (CCD), a topology that is uncommon in hard x-ray work. Behavior toward pseudomonochromatic ((55)Fe) and multichromatic ((241)Am) sources is briefly reviewed under optimized noise conditions. Results collectively establish the previously unknown functional depth structure. Several modes of usage are illustrated in approximately 4-20 keV x-ray laser plasma source investigations, where the significance of the characterization is briefly discussed. The spectral redistribution associated with this CCD topology is unfavorable, yet appropriate analysis ensures that sufficient spectral information remains for quantitative determination of broadband x-ray flux and spectra in essentially single laser shot measurements. The energy dependence of nascent electron cloud radii in silicon is determined using broadband x-rays from the laser plasma source, turning the narrow depletion depth to advantage. Finally, the characterization is used to quantify recent x-ray spectral explorations of the water jet laser plasma source operating under aspirator vacuum. These results will have key value for establishment of laboratory based ultrafast extended x-ray absorption fine structure experiments using microbolometric detectors.
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