TY - JOUR
T1 - Synchrotron X-ray diffraction investigation of the anomalous behavior of ice during freezing of aqueous systems
AU - Varshney, Dushyant B.
AU - Elliott, James A.
AU - Gatlin, Larry A.
AU - Kumar, Satyendra
AU - Suryanarayanan, Raj
AU - Shalaev, Evgenyi Y.
PY - 2009/5/7
Y1 - 2009/5/7
N2 - Simple aqueous systems, i.e., phosphate-glycine buffers and pure water, were studied at subambient temperatures by X-ray difractometry using a high-intensity synchrotron radiation source at the Advanced Photon Source of Argonne National Laboratory. Complex X-ray diffraction (XRD) patterns, with two or more poorly resolved peaks in place of each of the four diagnostic peaks of hexagonal ice, 100, 002, 101, and 102, referred as "splitting", were observed in the majority of cases. The splitting of up to 0.05 Å (d-spacing) was detected for 100, 002, and 101 peaks, whereas 102 peak was less affected. Deformation of the lattice of hexagonal ice, probably due to local stress created on the ice/ice or ice/container interface during water-to-ice transformation, is proposed as a possible mechanism for the observed splitting of XRD peaks. Using molecular modeling, it was estimated that the observed shifts in the peak positions are equivalent to applying a hydrostatic pressure of 2-3 kbars. The splitting can be used to quantify stresses during freezing, which could improve our understanding of the role of water-to-ice transformation on the destabilization of proteins and other biological systems.
AB - Simple aqueous systems, i.e., phosphate-glycine buffers and pure water, were studied at subambient temperatures by X-ray difractometry using a high-intensity synchrotron radiation source at the Advanced Photon Source of Argonne National Laboratory. Complex X-ray diffraction (XRD) patterns, with two or more poorly resolved peaks in place of each of the four diagnostic peaks of hexagonal ice, 100, 002, 101, and 102, referred as "splitting", were observed in the majority of cases. The splitting of up to 0.05 Å (d-spacing) was detected for 100, 002, and 101 peaks, whereas 102 peak was less affected. Deformation of the lattice of hexagonal ice, probably due to local stress created on the ice/ice or ice/container interface during water-to-ice transformation, is proposed as a possible mechanism for the observed splitting of XRD peaks. Using molecular modeling, it was estimated that the observed shifts in the peak positions are equivalent to applying a hydrostatic pressure of 2-3 kbars. The splitting can be used to quantify stresses during freezing, which could improve our understanding of the role of water-to-ice transformation on the destabilization of proteins and other biological systems.
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U2 - 10.1021/jp900404m
DO - 10.1021/jp900404m
M3 - Article
C2 - 19358549
AN - SCOPUS:66349137053
SN - 1520-6106
VL - 113
SP - 6177
EP - 6182
JO - Journal of Physical Chemistry B
JF - Journal of Physical Chemistry B
IS - 18
ER -