Chen S-H, Liu L, Chu X, Zhang Y, Fratini E, Baglioni P, Faraone A, Mamontov E
Department of Nuclear Science and Engineering, Massachusetts Institute of Technology, Cambridge, MA 02139, USA.
J Chem Phys. 2006 Nov 7;125(17):171103. doi: 10.1063/1.2372491.
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.
我们使用高分辨率准弹性中子散射光谱来研究水合DNA样品表面水分子的单粒子动力学。测量了H₂O和D₂O水合样品。通过取两个样品之间信号的差值,减去了DNA散射的贡献。在从270 K到185 K的一系列温度下进行了测量。使用弛豫笼模型来分析准弹性光谱。这使我们能够提取水分子与温度相关的与Q无关的平均平移弛豫时间<τ(T)>。通过绘制log<τ(T)>与T的关系图,我们观察到在T(L)=222±2 K处有明显的从脆弱到强烈的动力学转变(FSC)证据。DNA的动力学转变温度T(c)(标志着非谐分子运动的开始)与水合水的FSC温度T(L)的巧合表明,水合水分子在T(L)处迁移率的变化驱动了DNA中的动力学转变。