Synchrotron techniques in bio-physics

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Presentation transcript:

Synchrotron techniques in bio-physics Yulia Pushkar Department of Physics, Purdue University 1

Analyze electronic structure of molecules and proteins with high spatial and temporal resolution

Synchrotron

Synchrotrons of the World http://www.aps.anl.gov/About/Synchrotrons/index.html

Argonne National Laboratory

X-ray spectroscopy

Oxygenic photosynthesis Where do plants oxidize water? Mn4OxCa cluster Umena, Y. et al. Nature 2011

Objective: reproduce the efficiency of natural light-driven water splitting in a man made device. 4hn 2H2O O2 + 4H+ + 4e- Mn4CaOxCl

Question: why have we not yet achieved this objective? Possible answer: we still understand too little about the mechanism of water oxidation. Kok cycle was proposed in 1970 Liang et al. JACS 2000 Messinger et al. JACS, 2001 Pushkar et al. PNAS 2008

X-ray Absorption Spectroscopy of Mn4Ca cluster 1.8Å

Structural Changes in the Catalytic Cycle- S1, S2 and S3 Range-Extended Mn EXAFS S1 1) S1 to S2 no major changes in di-µ-oxo bridges 2) S2 to S3 - major structural changes in di-µ-oxo bridges

Photon-in-Photon-out spectroscopy 2p to 1s (K) Oxidation State 3p to 1s (K) Oxidation and spin state valence to 1s Ligands Information accessible: metal oxidation state, spin state, ligand environment Messinger et al. 2001 JACS; Pushkar et al. 2010 Angew. Chem.; Davis et al. J. Phys. Chem. Lett. 2012.

High resolution X-ray emission spectroscopy Point by point detection is not optimal for time resolved measurements monochromator Si(111), Si (221), Si(400) sample detector tunable analyzer ~ 1 eV X-ray beam Messinger et al. 2001 JACS; Pushkar et al. 2010 Angew. Chem.

Dispersive miniXES spectrometer Image on position sensitive detector: Davis et al. J. Phys. Chem. Lett. 2012

Laser pump X-ray probe Time-resolved XES analysis Will be used in analysis of PS II as well as artificial sun-light to fuel assemblies. MMCT in Mn-O-Ti chromophores will be studied. (Heinz Frei, Walter Weare)