Experimental evidence of fragile-to-strong dynamic crossover in DNA hydration water

被引:109
作者
Chen, S. -H.
Liu, L.
Chu, X.
Zhang, Y.
Fratini, E.
Baglioni, P.
Faraone, A.
Mamontov, E.
机构
[1] MIT, Dept Nucl Sci & Engn, Cambridge, MA 02139 USA
[2] Univ Florence, Dept Chem, I-50019 Florence, Italy
[3] Univ Florence, CSGI, I-50019 Florence, Italy
[4] Univ Maryland, Dept Mat Sci & Engn, College Pk, MD 20742 USA
[5] Natl Inst Stand & Technol, Ctr Neutron Res, Gaithersburg, MD 20899 USA
基金
美国国家科学基金会;
关键词
D O I
10.1063/1.2372491
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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 H2O and D2O 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. (c) 2006 American Institute of Physics.
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页数:4
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