Separable cooperative and localized translational motions of water confined by a chemically heterogeneous environment |
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Authors: | Malardier-Jugroot Cecile Head-Gordon Teresa |
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Institution: | Department of Bioengineering, University of California, Berkeley, CA 94720, USA. |
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Abstract: | We report quasi-elastic neutron scattering experiments at two resolutions that probe timescales of picoseconds to nanoseconds for the hydration dynamics of water, confined in a concentrated solution of N-acetyl-leucine-methylamide (NALMA) peptides in water over a temperature range of 248 K to 288 K. The two QENS resolutions used allow for a clean separation of two observable translational components, and ultimately two very different relaxation processes, that become evident when analyzed under a combination of the jump diffusion model and the relaxation cage model. The first translational motion is a localized beta-relaxation process of the bound surface water, and exhibits an Arrhenius temperature dependence and a large activation energy of approximately 8 kcal mol(-1). The second non-Arrhenius translational component is a dynamical signature of the alpha-relaxation of more fluid water, exhibiting a glass transition temperature of approximately 116 K when fit to the Volger Fulcher Tamman functional form. These peptide solutions provide a novel experimental system for examining confinement in order to understand the dynamical transition in bulk supercooled water by removing the unwanted interface of the confining material on water dynamics. |
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