X-rays only when you want them: Optimized pump-probe experiments using pseudo-single-bunch operation

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Abstract

Laser pump-X-ray probe experiments require control over the X-ray pulse pattern and timing. Here, the first use of pseudo-single-bunch mode at the Advanced Light Source in picosecond time-resolved X-ray absorption experiments on solutions and solids is reported. In this mode the X-ray repetition rate is fully adjustable from single shot to 500kHz, allowing it to be matched to typical laser excitation pulse rates. Suppressing undesired X-ray pulses considerably reduces detector noise and improves signal to noise in time-resolved experiments. In addition, dose-induced sample damage is considerably reduced, easing experimental setup and allowing the investigation of less robust samples. Single-shot X-ray exposures of a streak camera detector using a conventional non-gated charge-coupled device (CCD) camera are also demonstrated.

Figures

  • Figure 1 Top: orbit of the multi-bunch train and the kicked camshaft bunch in the storage ring. The kicker magnet periodically moves the camshaft into a different orbit. Bottom: the X-ray beam emitted from the multi-bunches is blocked by a horizontal slit, also called the vertical beam-defining aperture, while X-rays generated by the kicked camshaft pulse are displaced vertically and pass through.
  • Figure 2 Schematics of the beamline optics at ALS beamline 6.0.2.
  • Figure 3 Fe L3-edge transmission spectra and pump–probe difference of solvated FeII polypyridyl measured using PSB-KAC (top). Four spectra were acquired (before/after time zero and with laser on/off), showing a small transient change that is better visible in the difference spectra (bottom). Negative delay indicates an X-ray measurement before the laser excites the sample.
  • Table 1 Comparison of noise of three detection schemes; the mean-square residual of the fit is tabulated.
  • Figure 4 Time dependence of transient spectral changes at 709 eV measured by three different detection modes, with exponential fit and residual. The spectra are stacked vertically for easier comparison. A constant pre-timezero offset was subtracted and the transient change normalized to unity for easier comparison. All spectra were acquired in sequence and using the same laser power and fluence. Analysis shows that noise is reduced by a factor of up to four using PSB-KAC.
  • Table 2 Orbit offsets and angles of the kicked camshaft bunch at beamline 6.0.2 for two displaced round trips.
  • Figure 5 Top left: beamline 6.0.2 in spectrograph mode using an X-ray streak camera detector. Right: energy- and time-dispersed images in multibunch and PSB-KAC mode. Bottom left: intensity profiles, vertically averaged over the areas outlined in blue on the right, showing the magnitude of the background signal: top, multi-bunch; bottom, PSBKAC. Note the difference in vertical scale.
  • Figure 6 X-ray pulse pattern downstream of the 4 kHz chopper measured by a fast photodiode during regular operation (left), with KAC-PSB active at 4 kHz (center), and with KAC-PSB active and slit displaced to block multi-bunch pulses and transmit one selected camshaft pulse (right).

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CITATION STYLE

APA

Hertlein, M. P., Scholl, A., Cordones, A. A., Lee, J. H., Engelhorn, K., Glover, T. E., … Robin, D. S. (2015). X-rays only when you want them: Optimized pump-probe experiments using pseudo-single-bunch operation. Journal of Synchrotron Radiation, 22, 729–735. https://doi.org/10.1107/S1600577515001770

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