Abstract/Details

Understanding and exploiting nanoscale surface heterogeneity for particle and cell manipulation


2010 2010

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Abstract (summary)

This thesis explores the impact of surface heterogeneities on colloidal interactions and translates concepts to biointerfacial systems, for instance, microfluidic and biomedical devices. The thesis advances a model system, originally put forth by Kozlova: Tunable electrostatic surface heterogeneity is produced by adsorbing small amounts of cationic polyelectrolyte on a silica flat. The resulting positive electrostatic patches possess a density that is tuned from a saturated carpet down to average spacings on the order of a few hundred nanometers. At these length-scales, multiple adhesive elements (from tens to thousands) are present in the area of contact between a particle and a surface, a distinguishing feature of the thesis. Much of the literature addressing surface “heterogeneity” engineers surfaces with micron-scale features, almost always larger than the contact area between a particle and a second surface.

With a nanoscale heterogeneity model, this thesis reports and quantitatively explains particle interaction behavior not typical of homogeneous interfaces. This includes (1) an adhesion threshold, a minimum average surface density of cationic patches needed for particle capture, (previously observed by Kozlova); (2) a crossover, from salt-destabilized to salt-stabilized interactions between heterogeneous surfaces with net-negative charge; (3) a shift of the adhesion threshold with shear, reducing adhesion; (4) a crossover from shear-enhanced to shear-hindered particle adhesion; (5) a range of surface compositions and processing parameters that sustain particle rolling; and (6) conditions where particles arrest immediately on contact.

Through variations in ionic strength and particle size, the particle-surface contact area is systematically varied relative to the heterogeneity lengthscale. This provides a semi-quantitative explanation for the shifting of the adhesion threshold, in terms of the statistical probability of a particle being able to find a surface region sufficiently attractive for capture. Though neglecting hydrodynamics, the resulting (κ-1a)1/2 power law scaling for the density of patches at the adhesion threshold roughly captures the general shape of the data. The study also reveals that at high ionic strength, particle-surface interactions are most influenced by the patchy surface heterogeneity; however, at low ionic strengths, the system becomes most sensitive to the average system properties. Thus for heterogeneous interfaces, the extent to which heterogeneity is influential depends on other factors (particle size, ionic strength). While this comprises a crossover from heterogeneity-dominated to mean field behavior, it is worth noting that even in the mean field regime, the spacing between patches always exceeds the Debye length, making the regions of different surface charge always distinct. Comparison with the simulations of Duffadar and Davis reveals that the criterion for particle capture is a nearly constant number of cationic patches per unit area of contact between a particle and a heterogeneous collector.

The heterogeneous surface model displays a shear crossover seen with bacteria and other complex systems: At low shear, particle capture is enhanced, while at higher shears it is reduced. This behavior, sometimes rationalized in terms of the complex energy landscapes of biological bonds, is clearly explained in the heterogeneity model. For weakly adhesive systems engaging only a few adhesive elements or receptors, shear compromises the ability of a few bonds to capture particles. For more strongly adhesive systems, shear increases particle transport. The convolution of this competition leads to the non-monotonic effect of shear seen in biology.

The complex variety of particle behaviors combined with the large number of independently variable parameters, each with different scaling of interfacial forces, necessitates a state-space approach to mapping regimes interactions and motion signatures. Following the approach taken by biophysicists for describing the interactions of leukocytes with the endothelial vasculature near an injury, the state spaces in this thesis map regimes of free particle motion, immediate firm arrest, and persistent rolling against macroscopic average patch density, Debye length, particle size, and shear rate. Surprisingly, the electrostatic heterogeneity state space resembles that for selectin-mediated leukocyte motion, and reasons are put forth. This finding is important because it demonstrates how synthetic nanoscale constructs can be exploited to achieve the selective cell capture mechanism previously attributed only to specialized cell adhesion molecules.

This thesis initiates studies that extend these fundamental principles, developed for a tunable and well-characterized synthetic model to biological systems. For instance, it is demonstrated that general behaviors seen with the electrostatic model are observed when fibrinogen proteins are substituted for the electrostatic patches. This shows that the nature of the attractions is immaterial to adhesion, and that the effect of added salt primarily alters the range of the electrostatic repulsion and, correspondingly, the contact area. Also, studies with Staphylococcus aureus run parallel to those employing 1 μm silica spheres, further translating the concepts. Inaugural studies with mammalian cells, in the future work section, indicate that application of the surface heterogeneity approach to cell manipulation holds much future promise.

Indexing (details)


Subject
Physics;
Biophysics
Classification
0605: Physics
0786: Biophysics
Identifier / keyword
Pure sciences, Biological sciences, Biointerfaces, Cell manipulation, Colloids, Nanoscale, Surface heterogeneity
Title
Understanding and exploiting nanoscale surface heterogeneity for particle and cell manipulation
Author
Kalasin, Surachate
Number of pages
331
Publication year
2010
Degree date
2010
School code
0118
Source
DAI-B 71/07, Dissertation Abstracts International
Place of publication
Ann Arbor
Country of publication
United States
ISBN
9781124072661
Advisor
Santore, Maria M.
Committee member
Davis, Jeffrey M.; Dinsmore, Anthony D.; Menon, Narayanan
University/institution
University of Massachusetts Amherst
Department
Physics
University location
United States -- Massachusetts
Degree
Ph.D.
Source type
Dissertations & Theses
Language
English
Document type
Dissertation/Thesis
Dissertation/thesis number
3409603
ProQuest document ID
638634139
Copyright
Database copyright ProQuest LLC; ProQuest does not claim copyright in the individual underlying works.
Document URL
http://search.proquest.com/docview/638634139
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