Solution phase high repetition rate laser pump x-ray probe picosecond hard x-ray spectroscopy at the Stanford Synchrotron Radiation Lightsource.

We present a dedicated end-station for solution phase high repetition rate (MHz) picosecond hard x-ray spectroscopy at beamline 15-2 of the Stanford Synchrotron Radiation Lightsource. A high-power ultrafast ytterbium-doped fiber laser is used to photoexcite the samples at a repetition rate of 640 kHz, while the data acquisition operates at the 1.28 MHz repetition rate of the storage ring recording data in an alternating on-off mode. The time-resolved x-ray measurements are enabled via gating the x-ray detectors with the 20 mA/70 ps camshaft bunch of SPEAR3, a mode available during the routine operations of the Stanford Synchrotron Radiation Lightsource. As a benchmark study, aiming to demonstrate the advantageous capabilities of this end-station, we have conducted picosecond Fe K-edge x-ray absorption spectroscopy on aqueous [FeII(phen)3]2+, a prototypical spin crossover complex that undergoes light-induced excited spin state trapping forming an electronic excited state with a 0.6-0.7 ns lifetime. In addition, we report transient Fe Kß main line and valence-to-core x-ray emission spectra, showing a unique detection sensitivity and an excellent agreement with model spectra and density functional theory calculations, respectively. Notably, the achieved signal-to-noise ratio, the overall performance, and the routine availability of the developed end-station have enabled a systematic time-resolved science program using the monochromatic beam at the Stanford Synchrotron Radiation Lightsource.

Generation of picosecond electron bunches in storage rings.

Approaches to generating short X-ray pulses in synchrotron light sources are discussed. In particular, the method of using a superconducting harmonic cavity to generate simultaneously long and short bunches in storage rings and the approach of injecting short bunches from a linac injector into a storage ring for multi-turn circulation are emphasized. If multi-cell superconducting RF (SRF) cavities with frequencies of ∼1.5 GHz can be employed in storage rings, it would be possible to generate stable, high-flux, short-pulse X-ray beams with pulse lengths of 1-10 ps (FWHM) in present or future storage rings. However, substantial challenges exist in adapting today's high-gradient SRF cavities for high-current storage ring operation. Another approach to generating short X-ray pulses in a storage ring is injecting short-pulse electron bunches from a high-repetition-rate linac injector for circulation. Its performance is limited by the microbunching instability due to coherent synchrotron radiation. Tracking studies are carried out to evaluate its performance. Challenges and operational considerations for this mode are considered.