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The mechanical competence and suturing ability of collagen-based membranes are paramount in Guided Bone Regeneration (GBR) therapy, to ensure damage-free implantation, fixation and space maintenance in vivo. However, contact with the biological medium can induce swelling of collagen molecules, yielding risks of membrane sinking into the bone defect, early loss of barrier function, and irreversibly compromised clinical outcomes. To address these challenges, this study investigates the effect of the crosslinked network architecture on both mechanical and suture-holding properties of a new atelocollagen (AC) membrane. UV-cured networks were obtained via either single functionalisation of AC with 4-vinylbenzyl chloride (4VBC) or sequential functionalisation of AC with both 4VBC and methacrylic anhydride (MA). The wet-state compression modulus (Ec), Atomic Force Microscopy elastic modulus (EAFM) and swelling ratio (SR) were significantly affected by the UV-cured network architecture, leading up to a three-fold reduction in SR, and about two-fold increase in both Ec and EAFM, in the sequentially functionalised, compared to the single-functionalised, samples. Electron microscopy, dimensional analysis and compression testing revealed the direct impact of the ethanol series dehydration process on membrane microstructure, yielding densification of the freshly synthesised porous samples and a pore-free microstructure with increased Ec. Noteworthy, the single-functionalised, but not the sequentially functionalised, samples displayed higher suture retention strength in both the dry state and following 1 hour in Phosphate Buffered Saline (PBS), compared to Bio-Gide(r). These structure-property relationships confirm the key role played by the molecular architecture of covalently crosslinked collagen, aimed towards long-lasting resorbable membranes for predictable GBR., Comment: 40 pages, 9 figures, 1 Table. Accepted in Biomaterials Materials

Covalent functionalisation of collagen has been shown to be a promising strategy to adjust the mechanical properties of highly swollen collagen hydrogels. At the same time, secondary interactions between for example, amino acidic terminations or introduced functional groups also play an important role and are often challenging to predict and control. To explore this challenge, 4-vinylbenzyl chloride (4VBC) and methacrylic anhydride (MA) were reacted with type I collagen, and the swelling and rheological properties of resulting photo activated hydrogel systems investigated. 4VBC-based hydrogels showed significantly increased swelling ratio, in light of the lower degree of collagen functionalisation, with respect to methacrylated collagen networks, whilst rheological storage moduli were found to be comparable between the two systems. To explore the role of benzyl groups in the mechanical properties of the 4VBC-based collagen system, model chemical force microscopy (CFM) was carried out in aqueous environment with an aromatised probe against an aromatised gold coated glass slide. A marked increase in adhesion force (F: 0.11 +/- 0.01 nN) was measured between aromatised samples, compared to the adhesion force observed between the non-modified probe and a glass substrate (F: 2.64 +/- 1.82 nN). These results suggest the formation of additional and reversible {\pi}-{\pi} stacking interactions in aromatic 4VBC-based networks and explain the remarkable rheological properties of this system in comparison to MA based hydrogels., Comment: 6 pages, 4 figures, accepted in MRS Advances on 3 December 2015

While the fundamental limit on the resolution achieved in an atomic force microscope (AFM) is clearly related to the tip radius, the fact that the tip can creep and/or wear during an experiment is often ignored. This is mainly due to the difficulty in characterizing the tip, and in particular a lack of reliable methods that can achieve this in situ. Here, we provide an in situ method to characterize the tip radius and monitor tip creep and/or wear and biomolecular sample wear in ambient dynamic AFM. This is achieved by monitoring the dynamics of the cantilever and the critical free amplitude to observe a switch from the attractive to the repulsive regime. The method is exemplified on the mechanically heterogeneous sample of single DNA molecules bound to mica mineral surfaces. Simultaneous monitoring of apparent height and width of single DNA molecules while detecting variations in the tip radius R as small as one nanometer are demonstrated. The yield stress can be readily exceeded for sharp tips (R<10 nm) at typical operating amplitudes (A>10nm). The ability to know the AFM tip radius in situ and in real-time opens up the future for quantitative nanoscale materials properties determination at the highest possible spatial resolution., Comment: 26 pages, 6 figures

Biological hydrogels have been increasingly sought after as e.g. wound dressings or scaffolds for regenerative medicine, due to their inherent biofunctionality in biological environments. Especially in moist wound healing, the ideal material should absorb large amounts of wound exudate whilst remaining mechanically competent in-situ. Despite their large hydration, however, current biological hydrogels still leave much to be desired in terms of mechanical properties in physiological conditions. To address this challenge, a multi-scale approach is presented for the synthetic design of cyto-compatible collagen hydrogels with tunable mechanical properties (from nano- up to the macro-scale), uniquely high swelling ratios and retained (>70%) triple-helical features. Type I collagen was covalently functionalized with three different monomers, i.e. 4 vinylbenzyl chloride, glycidyl methacrylate and methacrylic anhydride, respectively. Backbone rigidity, hydrogen-bonding capability and degree of functionalization (F: 16&plusmn12 &ndash 91&plusmn7 mol.-%) of introduced moieties governed the structure-property relationships in resulting collagen networks, so that the swelling ratio (SR: 707&plusmn51 &ndash 1996&plusmn182 wt.-%), bulk compressive modulus (Ec: 30&plusmn7 &ndash 168&plusmn40 kPa) and Atomic Force Microscopy elastic modulus (EAFM: 16&plusmn2 &ndash 387&plusmn66 kPa) were readily adjusted. In light of their remarkably high swelling and mechanical properties, these tunable collagen hydrogels may be further exploited for the design of advanced dressings for chronic wound care., Comment: Accepted in "Journal of the Royal Society Interface"