Relativistic and resonant effects in the ionization of heavy atoms by ultra-intense hard X-rays.

An accurate description of the interaction of intense hard X-ray pulses with heavy atoms, which is crucial for many applications of free-electron lasers, represents a hitherto unresolved challenge for theory because of the enormous number of electronic configurations and relativistic effects, which need to be taken into account. Here we report results on multiple ionization of xenon atoms by ultra-intense (about 1019 W/cm2) femtosecond X-ray pulses at photon energies from 5.5 to 8.3 keV and present a theoretical model capable of reproducing the experimental data in the entire energy range. Our analysis shows that the interplay of resonant and relativistic effects results in strongly structured charge state distributions, which reflect resonant positions of relativistically shifted electronic levels of highly charged ions created during the X-ray pulse. The theoretical approach described here provides a basis for accurate modeling of radiation damage in hard X-ray imaging experiments on targets with high-Z constituents.

Development of high-repetition-rate laser pump/x-ray probe methodologies for synchrotron facilities.

We describe our implementation of a high repetition rate (54 kHz-6.5 MHz), high power (>10 W), laser system at the 7ID beamline at the Advanced Photon Source for laser pump/x-ray probe studies of optically driven molecular processes. Laser pulses at 1.06 µm wavelength and variable duration (10 or 130 ps) are synchronized to the storage ring rf signal to a precision of ~250 fs rms. Frequency doubling and tripling of the laser radiation using nonlinear optical techniques have been applied to generate 532 and 355 nm light. We demonstrate that by combining a microfocused x-ray probe with focused optical laser radiation the requisite fluence (with <10 µJ/pulse) for efficient optical excitation can be readily achieved with a compact and commercial laser system at megahertz repetition rates. We present results showing the time-evolution of near-edge x-ray spectra of a well-studied, laser-excited metalloporphyrin, Ni(II)-tetramesitylporphyrin. The use of high repetition rate, short pulse lasers as pump sources will dramatically enhance the duty cycle and efficiency in data acquisition and hence capabilities for laser-pump/x-ray probe studies of ultrafast structural dynamics at synchrotron sources.