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

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10 Author(s)
March, Anne Marie ; X-ray Science Division, Advanced Photon Source, Argonne National Laboratory, 9700 S. Cass Ave., Argonne, Illinois 60439, USA ; Stickrath, Andrew ; Doumy, Gilles ; Kanter, Elliot P.
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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.

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Review of Scientific Instruments  (Volume:82 ,  Issue: 7 )