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Dynamic heterogeneity controls diffusion and viscosity near biological interfaces.

ABSTRACT: At a nanometre scale, the behaviour of biological fluids is largely governed by interfacial physical chemistry. This may manifest as slowed or anomalous diffusion. Here we describe how measures developed for studying glassy systems allow quantitative measurement of interfacial effects on water dynamics, showing that correlated motions of particles near a surface result in a viscosity greater than anticipated from individual particle motions. This effect arises as a fundamental consequence of spatial heterogeneity on nanometre length scales and applies to any fluid near any surface. Increased interfacial viscosity also causes the classic finding that large solutes such as proteins diffuse much more slowly than predicted in bulk water. This has previously been treated via an empirical correction to the solute size: the hydrodynamic radius. Using measurements of quantities from theories of glass dynamics, we can now calculate diffusion constants from molecular details alone, eliminating the empirical correction factor.

SUBMITTER: Pronk S

PROVIDER: S-EPMC3971065 | biostudies-literature | 2014

REPOSITORIES: biostudies-literature

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Dynamic heterogeneity controls diffusion and viscosity near biological interfaces.

Pronk Sander S Lindahl Erik E Kasson Peter M PM

Nature communications 20140101

At a nanometre scale, the behaviour of biological fluids is largely governed by interfacial physical chemistry. This may manifest as slowed or anomalous diffusion. Here we describe how measures developed for studying glassy systems allow quantitative measurement of interfacial effects on water dynamics, showing that correlated motions of particles near a surface result in a viscosity greater than anticipated from individual particle motions. This effect arises as a fundamental consequence of spa ...[more]

PMID: 24398864

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Project description:The slow transport of water, organic species and oxidants in viscous aerosol can lead to aerosol existing in transient states that are not solely governed by thermodynamic principles but by the kinetics of gas-particle partitioning. The relationship between molecular diffusion constants and particle viscosity (for example, as reflected in the Stokes-Einstein equation) is frequently considered to provide an approximate guide to relate the kinetics of aerosol transformation with a material property of the aerosol. We report direct studies of both molecular diffusion and viscosity in the aerosol phase for the ternary system water/maleic acid/sucrose, considering the relationship between the hygroscopic response associated with the change in water partitioning, the volatilisation of maleic acid, the ozonolysis kinetics of maleic acid and the particle viscosity. Although water clearly acts as a plasticiser, the addition of minor fractions of other organic moieties can similarly lead to significant changes in the viscosity from that expected for the dominant component forming the organic matrix (sucrose). Here we highlight that the Stokes-Einstein relationship between the diffusion constant of water and the viscosity of the particle may be more than an order of magnitude in error, even at viscosities as low as 1 Pa s. We show that the thermodynamic relationships of hygroscopic response that underpin such kinetic determinations must be accurately known to retrieve accurate values for diffusion constants; such data are often not available. Further, we show that scaling of the diffusion constants of organic molecules of similar size to those forming the matrix with particle viscosity may be well represented by the Stokes-Einstein equation, suppressing the apparent volatility of semi-volatile components. Finally, the variation in uptake coefficients and diffusion constants for oxidants and small weakly interacting molecules may be much less dependent on viscosity than the diffusion constants of more strongly interacting molecules such as water.

Project description:BackgroundDynamic diffusion magnetic resonance imaging (ddMRI) metrics can assess transient microstructural alterations in tissue diffusivity but requires additional scan time hindering its clinical application.PurposeTo determine whether a diffusion gradient table can simultaneously acquire data to estimate dynamic and diffusion tensor imaging (DTI) metrics.Study typeProspective.SubjectsSeven healthy subjects, 39 epilepsy patients (15 female, 31 male, age ± 15).Field strength/sequenceTwo-dimensional diffusion MRI (b = 1000 s/mm2 ) at a field strength of 3 T. Sessions in healthy subjects-standard ddMRI (30 directions), standard DTI (15 and 30 directions), and nested cubes scans (15 and 30 directions). Sessions in epilepsy patients-two 30 direction (standard ddMRI, 10 nested cubes) or two 15 direction scans (standard DTI, 5 nested cubes).AssessmentFifteen direction DTI was repeated twice for within-session test-retest measurements in healthy subjects. Bland-Altman analysis computed bias and limits of agreement for DTI metrics using test-retest scans and standard 15 direction vs. 5 nested cubes scans. Intraclass correlation (ICC) analysis compared tensor metrics between 15 direction DTI scans (standard vs. 5 nested cubes) and the coefficients of variation (CoV) of trace and apparent diffusion coefficient (ADC) between 30 direction ddMRI scans (standard vs. 10 nested cubes).Statistical testsBland-Altman and ICC analysis using a P-value of 0.05 for statistical significance.ResultsCorrelations of mean diffusivity (MD), axial diffusivity (AD), and radial diffusivity (RD) were strong and significant in gray (ICC > 0.95) and white matter (ICC > 0.95) between standard vs. nested cubes DTI acquisitions. Correlation of white matter fractional anisotropy was also strong (ICC > 0.95) and significant. ICCs of the CoV of dynamic ADC measured using repeated cubes and nested cubes acquisitions were modest (ICC >0.60), but significant in gray matter.ConclusionA nested cubes diffusion gradient table produces tensor-based and dynamic diffusion measurements in a single acquisition.Level of evidence2 TECHNICAL EFFICACY: Stage 1.

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Dynamic heterogeneity controls diffusion and viscosity near biological interfaces.

Publications

Dynamic heterogeneity controls diffusion and viscosity near biological interfaces.

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