Self-assembly and elasticity of hierarchical proteoglycan–hyaluronan brushes

Attili, Seetharamaiah; Richter, Ralf P.

doi:10.1039/c3sm51213d

Cited by 27 publications

(27 citation statements)

References 73 publications

(149 reference statements)

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“…Furthermore, in their reconstituted PCM assays, Knudson et al performed controls comparing the final thickness of the PCM on living and fixed cells, demonstrating the same outcome (15,17). Instead, we infer that the PCM swells as aggrecan binds to free sites on the HA, further stretching out of the polymer in an aggrecan concentration-dependent manner (33,34). Swelling might also be partly driven by the formation of a polymer brush type scenario, because overlap of the grafted HA strands might increase with exogenous aggrecan binding (35,36).…”

Section: Pcm Swells With Increasing Aggrecan Concentrationmentioning

confidence: 62%

“…Meanwhile, 200 nm diameter particles do not reach the cell surface in native or aggrecan-treated cells. Their average distance from the cell surface is 3.7 mm in both cases (N ¼ 24 (34), N ¼ 15 (19)), with low relative intensities of 12.2 5 1.8% and 17.2 5 2.6% (N ¼ 24 (33) and N ¼ 12 (18)). This blockage may represent the limit to approach the cell surface due to microvilli on the RCJ-P surface, which we estimate extend~1-3 mm (18).…”

Section: Fluorescent Aggrecan Assay Reveals Free Binding Sites In Pcmmentioning

confidence: 96%

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Cell Surface Access Is Modulated by Tethered Bottlebrush Proteoglycans

Chang

McLane

Fogg

et al. 2016

Biophysical Journal

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The hyaluronan-rich pericellular matrix (PCM) plays physical and chemical roles in biological processes ranging from brain plasticity, to adhesion-dependent phenomena such as cell migration, to the onset of cancer. This study investigates how the spatial distribution of the large negatively charged bottlebrush proteoglycan, aggrecan, impacts PCM morphology and cell surface access. The highly localized pericellular milieu limits transport of nanoparticles in a size-dependent fashion and sequesters positively charged molecules on the highly sulfated side chains of aggrecan. Both rat chondrocyte and human mesenchymal stem cell PCMs possess many unused binding sites for aggrecan, showing a 2.5x increase in PCM thickness from ∼7 to ∼18 μm when provided exogenous aggrecan. Yet, full extension of the PCM occurs well below aggrecan saturation. Hence, cells equipped with hyaluronan-rich PCM can in principle manipulate surface accessibility or sequestration of molecules by tuning the bottlebrush proteoglycan content to alter PCM porosity and the number of electrostatic binding sites.

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Section: Pcm Swells With Increasing Aggrecan Concentrationmentioning

confidence: 62%

Section: Fluorescent Aggrecan Assay Reveals Free Binding Sites In Pcmmentioning

confidence: 96%

Cell Surface Access Is Modulated by Tethered Bottlebrush Proteoglycans

Chang

McLane

Fogg

et al. 2016

Biophysical Journal

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“…They confer different conformational states to HA, 6 mediate its cross-linking and/or attachment to the cell surface, 7,8 and thereby engender self-assembly into large and typically strongly hydrated supra-molecular architectures. 9,10 Due to its large size, HA chains can interact with many binding partners simultaneously, and the dynamic remodeling of HA-rich matrices as a function of the surrounding binding partners is believed to be functionally important. 2,8 Its biocompatibility, physico-chemical properties and biological effects make HA also attractive for applications in biomaterials [11][12][13] and bionanotechnology.…”

Section: Introductionmentioning

confidence: 99%

Interaction of Hyaluronan with Cationic Nanoparticles

et al. 2015

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The polysaccharide hyaluronan (HA) is a main component of peri- and extracellular matrix, and an attractive molecule for materials design in tissue engineering and nanomedicine. Here, we study the morphology of complexes that form upon interaction of nanometer-sized amine-coated gold particles with this anionic, linear, and regular biopolymer in solution and grafted to a surface. We find that cationic nanoparticles (NPs) have profound effects on HA morphology on the molecular and supramolecular scale. Quartz crystal microbalance (QCM-D) shows that depending on their relative abundance, cationic NPs promote either strong compaction or swelling of films of surface-grafted HA polymers (HA brushes). Transmission electron and atomic force microscopy reveal that the NPs do also give rise to complexes of distinct morphologies-compact nanoscopic spheres and extended microscopic fibers-upon interaction with HA polymers in solution. In particular, stable and hydrated spherical complexes of single HA polymers with NPs can be prepared when balancing the ionizable groups on HA and NPs. The observed self-assembly phenomena could be useful for the design of drug delivery vehicles and a better understanding of the reorganization of HA-rich synthetic or biological matrices.

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“…As for polymer gels [51], the modulus of a brush scales as M ∼ 1/ξ 3 (see Supplemental Material). From previous measurements of the mechanical response of HA brushes [27,52], we determine M ref ≃ 100 Pa for a brush of ξ ref = 57 nm (see Supplemental Material and references [53,54]). We can thus compute the expected moduli of the brushes from…”

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confidence: 99%

Elastohydrodynamic Lift at a Soft Wall

et al. 2018

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We study experimentally the motion of non-deformable microbeads in a linear shear flow close to a wall bearing a thin and soft polymer layer. Combining microfluidics and 3D optical tracking, we demonstrate that the steady-state bead/surface distance increases with the flow strength. Moreover, such lift is shown to result from flow-induced deformations of the layer, in quantitative agreement with theoretical predictions from elastohydrodynamics. This study thus provides the first experimental evidence of "soft lubrication" at play at small scale, in a system relevant e.g. to the physics of blood microcirculation.

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Self-assembly and elasticity of hierarchical proteoglycan–hyaluronan brushes

Abstract: We assemble aggrecan-containing hyaluronan brushes to study how the supramolecular structure and dynamics relate to material properties in hyaluronan-rich pericellular matrices.

Cited by 27 publications

References 73 publications

Cell Surface Access Is Modulated by Tethered Bottlebrush Proteoglycans

Cell Surface Access Is Modulated by Tethered Bottlebrush Proteoglycans

Interaction of Hyaluronan with Cationic Nanoparticles

Elastohydrodynamic Lift at a Soft Wall

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