Experimental evidence of fragile-to-strong dynamic crossover in DNA hydration water.
We used high-resolution quasielastic neutron scattering spectroscopy to study the single-particle dynamics of water molecules on the surface of hydrated DNA samples. Both H(2)O and D(2)O hydrated samples were measured. The contribution of scattering from DNA is subtracted out by taking the difference of the signals between the two samples. The measurement was made at a series of temperatures from 270 down to 185 K. The relaxing-cage model was used to analyze the quasielastic spectra. This allowed us to extract a Q-independent average translational relaxation time <tau(T)> of water molecules as a function of temperature. We observe clear evidence of a fragile-to-strong dynamic crossover (FSC) at T(L)=222+/-2 K by plotting log<tau(T)> versus T. The coincidence of the dynamic transition temperature T(c) of DNA, signaling the onset of anharmonic molecular motion, and the FSC temperature T(L) of the hydration water suggests that the change of mobility of the hydration water molecules across T(L) drives the dynamic transition in DNA.
Chen
S-H
SH
Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA. sowhsin@mit.edu
Liu
L
L
Chu
X
X
Zhang
Y
Y
Fratini
E
E
Baglioni
P
P
Faraone
A
A
Mamontov
E
E
D004247:DNA / Q000737:chemistry*; D003903:Deuterium / Q000737:chemistry; D009113:Muramidase / Q000737:chemistry; D009502:Neutrons; D012542:Scattering, Radiation; D013057:Spectrum Analysis; D044366:Transition Temperature; D014867:Water / Q000737:chemistry*
D014867:Water; D004247:DNA; D003903:Deuterium; D009113:Muramidase