Material Science, Chemistry, and Physics: Time-Resolved X-ray Scattering

Since its foundation, BioCARS has served time-resolved macromolecular crystallography community at the Advanced Photon Source. A recent upgrade of our 14-ID beamline increased the X-ray flux density by a factor of 100, improved pump-probe time-resolution to 100 ps, enabled us to use the widely-available 24-bunch mode of operation of the APS, and thus allows us to conduct time-resolved experiments for about 4000 hours per year (Graber et al., 2011). We also expanded our scientific reach beyond macromolecular crystallography to biological SAXS/WAXS. In addition, our upgraded technical capabilities have proved to be suitable to and attracted the attention of the time-resolved X-ray scattering community in the physical sciences.

Physical sciences user projects successfully conducted at 14-ID include photo-switching dynamics in spin-crossover molecular complexes (Collet et al, 2012), charge transfer and excited state structures in small molecules (Makal et al, 2012), X-ray pump optical probe cross-correlation study of GaAs (Durbin et al., 2012), time-resolved diffuse scattering to study the structural dynamics of photo-excited bismuth (Chen et al., 2013) etc.

14-ID capabilities for time-resolved science:

  • Picosecond and nanosecond lasers synchronized with X-ray pulses are available for pump-probe experiments (< 5ps rms timing jitter)
  • Single 100ps X-ray pulse isolation by an X-ray shutter system allows pump-probe time delays of arbitrary length (from 100 ps to ms, and longer)
  • 100ps pulse isolation is possible in both hybrid and 24-bunch modes of the APS storage ring
  • Both polychromatic (pink and white) and pulsed monochromatic (7-20 keV) X-ray beams are available
  • High X-ray flux per single 100ps X-ray pulse: 3 X 1010 photons/pulse (with two in-line undulators, polychromatic pulses, hybrid mode of the APS storage ring)
  • Two in-line undulators, U23 and U27; possible to modify the X-ray spectrum by offsetting the energies of the first harmonic for two undulators and/or tapering the undulator gaps
  • Pump-probe repetition rate: 40Hz to 1KHz
  • Detector readout rate: 10-100Hz with the new large area, high speed readout Rayonix detector (to be installed in March 2014)
  • Focusing: 20 (v) X 20 (h) µm2

References

  • Chen, J., Trigo, M., Fahy, S., Murray, E. D., Sheu, Y. M., Graber, T., Henning, R., Chien, Y. J., Uher, C., and Reis, D. A.  Time- and momentum-resolved probe of heat transport in photo-excited bismuth  Applied Physics Letters 102, 181903 (2013)
  • Collet, E., Moisan, N., Baldé, C., Bertoni, R., Trzop, E., Laulhé, C., Lorenc, M., Servol, M., Cailleau, H., Tissot, A., Boillot, M.-L., Graber, T., Henning, R., Coppens, P., and Cointe, M. B.-L.  Ultrafast spin-state photoswitching in a crystal and slower consecutive processes investigated by femtosecond optical spectroscopy and picosecond X-ray diffraction.  Phys Chem Chem Phys 14, 6185–6192 (2012)
  • Durbin, S. M., Clevenger, T., Graber, T., and Henning, R.  X-ray pump optical probe cross-correlation study of GaAs.  Nat Photon 6, 111–114 (2012)
  • Graber, T., Anderson, S., Brewer, H., Chen, Y.-S., Cho, H. S., Dashdorj, N., Henning, R. W., Kosheleva, I., Macha, G., Meron, M., Pahl, R., Ren, Z., Ruan, S., Schotte, F., Šrajer, V., Viccaro, P. J., Westferro, F., Anfinrud, P., and Moffat, K.  BioCARS: a synchrotron resource for time-resolved X-ray science.  J Synchrotron Rad 18, 658–670 (2011)
  • Makal, A., Benedict, J., Trzop, E., Sokolow, J., Fournier, B., Chen, Y., Kalinowski, J. A., Graber, T., Henning, R., and Coppens, P.  Restricted Photochemistry in the Molecular Solid State: Structural Changes on Photoexcitation of Cu(I) Phenanthroline Metal-to-Ligand Charge Transfer (MLCT) Complexes by Time-Resolved Diffraction.  J Phys Chem A 116, 3359–3365 (2012)

X-Ray Scattering Contacts

Robert Henning

Research Beamline Scientist
(630) 252-0446
henning@cars.uchicago.edu

Irina Kosheleva

Research Beamline Scientist
(630) 252-0467
ikoshelev@cars.uchicago.edu

Transmission of GaAs at 860 nm versus time after X-ray pump pulse

Data points are normalized to the transmitted intensity before X-ray excitation and are the average of 100 shots. Error bars are the standard deviation of 100 shots and are largely due to laser/X-ray pulse timing jitter. Dashed curve: Gaussian time profile of X-ray pulses. Solid curve: integral, which matches data at the transition region. Inset (top): scattering geometry, with GaAs surface at the intersection of the X-ray and laser beams. Inset (bottom): transmission at longer times, fit to an exponential decay with a lifetime of 1.1 ns. S.M. Durbin, T. Clevenger, T. Graber, R. Henning X-ray pump optical probe cross-correlation study of GaAs Nat. Photonics 6, 111-114 (2012)