W0091
A Time Resolved Crystallography Facility at ChemMatCARS.
T. Grabera and P. Coppensb
aThe Center for Advanced Radiation Sources, The
Univ. of Chicago, 5640 South Ellis Ave., Chicago, Illinois 60637,
bDept. of Chemistry, State Univ. of New York at Buffalo, Buffalo NY
14260-3000.
Undulators at high brilliance synchrotron x-ray facilities
such as the Advanced Photon Source (APS) provide intense highly collimated x-ray
beams which, when coupled with pump-probe crystallographic techniques, open new
possibilities to study transient chemical phenomena. The high spectral
brilliance of the source results in a very high photon flux density at the
sample, enabling high-resolution monochromatic time-resolved crystallographic
(TRC) measurements in the microsecond time domain. ChemMatCARS, a National
Synchrotron Resource for Chemistry and Materials Science, is presently
commissioning an undulator-based TRC capability at the APS for applications in
small molecule crystallography. In the time resolved experiments performed at
the facility, two CCD frames are taken consecutively covering the same angular
range. The first frame is taken with the pump-laser on while the second is taken
under dark conditions. The procedure continues much like a standard
crystallography measurement with the difference that two sets of data are
collected for a given sample. The relative change in integrated intensity of
each of the reflections is used to refine the change in molecular geometry upon
excitation. The heart of the system is a mechanical x-ray beam
chopper1 consisting of a brass wheel with slots machined around its
circumference. The wheel is spun at a high rate and depending on its rotational
speed and slot size, will produce differing x-ray-beam frequencies and pulse
widths. The temporal width of the chopped x-ray pulse and the repeat frequency
produced by the wheel are tailored to the lifetime of the molecule under study.
A description of the facility and its capabilities will be presented as well as
plans for the future.
1) W. F. Fullagar, G. Wu, C. Kim, L. Ribaud, G. Sagerman, and
P. Coppens, (2000) J. Synchrotron Radiation, 7 229-235