The Dynamic Response Function χT(Q,t) of Confined Supercooled Water and its Relation to the Dynamic Crossover Phenomenon

被引:5
作者
Chen, Sow-Hsin [1 ]
Zhang, Yang [1 ]
Lagi, Marco [1 ,2 ,3 ]
Chu, Xiangqiang [1 ]
Liu, Li [1 ,4 ]
Faraone, Antonio [1 ,5 ]
Fratini, Emiliano [2 ,3 ]
Baglioni, Piero [2 ,3 ]
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] Rensselaer Polytech Inst, Dept Mech Aerosp & Nucl Engn, Troy, NY 12180 USA
[5] NIST, Ctr Neutron Res, Gaithersburg, MD 20899 USA
来源
ZEITSCHRIFT FUR PHYSIKALISCHE CHEMIE-INTERNATIONAL JOURNAL OF RESEARCH IN PHYSICAL CHEMISTRY & CHEMICAL PHYSICS | 2010年 / 224卷 / 1-2期
关键词
Dynamic Response Function; Confined Supercooled Water; Dynamic Crossover Phenomenon; STRONG LIQUID TRANSITION; PROTEIN HYDRATION WATER; DIELECTRIC-RELAXATION; SIMULATIONS; TEMPERATURE; MODEL; SPECTROSCOPY; NANOTUBES; BEHAVIOR; DENSITY;
D O I
10.1524/zpch.2010.6095
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 have made a series of Quasi-Elastic Neutron Scattering (QENS) studies of supercooled water confined in 3-D and 1-D geometries, specifically, interstitial water in aged cement paste (3-D)and water confined in MCM-41-S and Double Wall Nano Tube DWNT (1-D). In addition, we also include the cases of hydration water oil protein surface and other biopolymer surfaces (Pseudo 2-D). By analyzing the QENS spectra using Relaxing Cage Model (RCM), we are able to extract accurately the self-intermediate scattering function of hydrogen atoms F-H(Q,t), at low-Q as a function of temperature T, showing an a-relaxation process at long time. We can then construct the Dynamic Response Function chi(T)(Q,t) = -dF(H)(Q,t)/dT. chi(T)(Q,t) as a function of t at constant Q shows a single peak at the characteristic alpha-relaxation time <tau >, the amplitude of which grows as we approach the dynamic crossover temperature T-L observed before in each of these geometries. However, the peak height of chi(T)(Q,t) decreases after passing the crossover temperature T-L. We make all argument to relate the occurrence of the extremum of the peak height in chi(T) to the existence of the dynamic crossover temperature in each of these cases.
引用
收藏
页码:109 / 131
页数:23
相关论文
共 70 条
  • [1] ON TEMPERATURE DEPENDENCE OF COOPERATIVE RELAXATION PROPERTIES IN GLASS-FORMING LIQUIDS
    ADAM, G
    GIBBS, JH
    [J]. JOURNAL OF CHEMICAL PHYSICS, 1965, 43 (01) : 139 - &
  • [2] SUPERCOOLED WATER
    ANGELL, CA
    [J]. ANNUAL REVIEW OF PHYSICAL CHEMISTRY, 1983, 34 : 593 - 630
  • [3] Dynamics of supercooled water in confined geometry
    Bergman, R
    Swenson, J
    [J]. NATURE, 2000, 403 (6767) : 283 - 286
  • [4] Dielectric study of supercooled 2D water in a vermiculite clay
    Bergman, R
    Swenson, J
    Börjesson, L
    Jacobsson, P
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2000, 113 (01) : 357 - 363
  • [5] Spontaneous and induced dynamic fluctuations in glass formers. I. General results and dependence on ensemble and dynamics
    Berthier, L.
    Biroli, G.
    Bouchaud, J.-P.
    Kob, W.
    Miyazaki, K.
    Reichman, D. R.
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2007, 126 (18)
  • [6] Direct experimental evidence of a growing length scale accompanying the glass transition
    Berthier, L
    Biroli, G
    Bouchaud, JP
    Cipelletti, L
    El Masri, D
    L'Hôte, D
    Ladieu, F
    Pierno, M
    [J]. SCIENCE, 2005, 310 (5755) : 1797 - 1800
  • [7] Experimental determination of the site-site radial distribution functions of supercooled ultrapure bulk water
    Botti, A
    Bruni, F
    Isopo, A
    Ricci, MA
    Soper, AK
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2002, 117 (13) : 6196 - 6199
  • [8] Experimental evidence of fragile-to-strong dynamic crossover in DNA hydration water
    Chen, S. -H.
    Liu, L.
    Chu, X.
    Zhang, Y.
    Fratini, E.
    Baglioni, P.
    Faraone, A.
    Mamontov, E.
    [J]. JOURNAL OF CHEMICAL PHYSICS, 2006, 125 (17)
  • [9] Observation of fragile-to-strong dynamic crossover in protein hydration water
    Chen, S. -H.
    Liu, L.
    Fratini, E.
    Baglioni, Piero
    Faraone, A.
    Mamontov, E.
    [J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA, 2006, 103 (24) : 9012 - 9016
  • [10] CHEN SH, 1991, NATO ADV SCI I C-MAT, V329, P289