TY  - JOUR
A1  - Mehrabi, Pedram
A1  - Schulz, Eike C.
A1  - Dsouza, Raison
A1  - Müller-Werkmeister, Henrike
A1  - Tellkamp, Friedjof
A1  - Miller, R. J. Dwayne
A1  - Pai, Emil F.
T1  - Time-resolved crystallography reveals allosteric communication aligned with molecular breathing
JF  - Science
N2  - A comprehensive understanding of protein function demands correlating structure and dynamic changes. Using time-resolved serial synchrotron crystallography, we visualized half-of-the-sites reactivity and correlated molecular-breathing motions in the enzyme fluoroacetate dehalogenase. Eighteen time points from 30 milliseconds to 30 seconds cover four turnover cycles of the irreversible reaction. They reveal sequential substrate binding, covalent-intermediate formation, setup of a hydrolytic water molecule, and product release. Small structural changes of the protein mold and variations in the number and placement of water molecules accompany the various chemical steps of catalysis. Triggered by enzyme-ligand interactions, these repetitive changes in the protein framework’s dynamics and entropy constitute crucial components of the catalytic machinery.
Y1  - 2019
U6  - https://doi.org/10.1126/science.aaw9904
SN  - 0036-8075
SN  - 1095-9203
VL  - 365
IS  - 6458
SP  - 1167
EP  - 1170
PB  - American Assoc. for the Advancement of Science
CY  - Washington
ER  -