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

S. H. Chen; L. Liu; X. Chu; Y. Zhang; E. Fratini; P. Baglioni; A. Faraone; E. Mamontov

doi:10.1063/1.2372491

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

S. H. Chen, L. Liu, X. Chu, Y. Zhang, E. Fratini, P. Baglioni, A. Faraone, E. Mamontov

Chemical Spectroscopy

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117 Scopus citations

Abstract

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 H2 O and D2 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 〈 τT 〉 of water molecules as a function of temperature. We observe clear evidence of a fragile-to-strong dynamic crossover (FSC) at TL =222±2 K by plotting log〈 τT 〉 versus T. The coincidence of the dynamic transition temperature Tc of DNA, signaling the onset of anharmonic molecular motion, and the FSC temperature TL of the hydration water suggests that the change of mobility of the hydration water molecules across TL drives the dynamic transition in DNA.

Original language	English
Article number	171103
Journal	Journal of Chemical Physics
Volume	125
Issue number	17
DOIs	https://doi.org/10.1063/1.2372491
State	Published - 2006

Funding

The research at MIT is supported by DOE Grants No. DE-FG02-90ER45429 and No. 2113-MIT-DOE-591. Two of the authors (E.F. and P.B) acknowledge CSGI (Florence, Italy) for partial financial support. This work utilized facilities supported in part by the National Science Foundation under Agreement No. DMR-0086210. Technical support in measurements from V. Garcia-Sakai at NIST NCNR is greatly appreciated. We benefited from affiliation with EU-Marie-Curie Research and Training Network on Arrested Matter. Identification of commercial equipment and software does not imply recommendation or endorsement by the NIST, nor does it imply that the equipment identified is necessarily the best available for the purpose.

Funders	Funder number
CSGI
National Science Foundation
Directorate for Mathematical and Physical Sciences	0086210

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title = "Experimental evidence of fragile-to-strong dynamic crossover in DNA hydration water",

abstract = "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 H2 O and D2 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 〈 τT 〉 of water molecules as a function of temperature. We observe clear evidence of a fragile-to-strong dynamic crossover (FSC) at TL =222±2 K by plotting log〈 τT 〉 versus T. The coincidence of the dynamic transition temperature Tc of DNA, signaling the onset of anharmonic molecular motion, and the FSC temperature TL of the hydration water suggests that the change of mobility of the hydration water molecules across TL drives the dynamic transition in DNA.",

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AU - Chen, S. H.

AU - Liu, L.

AU - Chu, X.

AU - Zhang, Y.

AU - Fratini, E.

AU - Baglioni, P.

AU - Faraone, A.

AU - Mamontov, E.

PY - 2006

Y1 - 2006

N2 - 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 H2 O and D2 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 〈 τT 〉 of water molecules as a function of temperature. We observe clear evidence of a fragile-to-strong dynamic crossover (FSC) at TL =222±2 K by plotting log〈 τT 〉 versus T. The coincidence of the dynamic transition temperature Tc of DNA, signaling the onset of anharmonic molecular motion, and the FSC temperature TL of the hydration water suggests that the change of mobility of the hydration water molecules across TL drives the dynamic transition in DNA.

AB - 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 H2 O and D2 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 〈 τT 〉 of water molecules as a function of temperature. We observe clear evidence of a fragile-to-strong dynamic crossover (FSC) at TL =222±2 K by plotting log〈 τT 〉 versus T. The coincidence of the dynamic transition temperature Tc of DNA, signaling the onset of anharmonic molecular motion, and the FSC temperature TL of the hydration water suggests that the change of mobility of the hydration water molecules across TL drives the dynamic transition in DNA.

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

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