Materials fabrication with nanoscale structural precision based on bottom-up-type self-assembly has become more important in various current disciplines in chemistry including materials chemistry, ...

Layer-by-layer Nanoarchitectonics: Invention, Innovation, and Evolution

The design of advanced functional materials with nanometer- and micrometer-scale control over their properties is of considerable interest for both fundamental and applied studies because of the many potential applications for these materials in the fields of biomedical materials, tissue engineering, and regenerative medicine. The layer-by-layer deposition technique introduced in the early 1990s by Decher, Moehwald, and Lvov is a versatile technique, which has attracted an increasing number of researchers in recent years due to its wide range of advantages for biomedical applications: ease of preparation under "mild" conditions compatible with physiological media, capability of incorporating bioactive molecules, extra-cellular matrix components and biopolymers in the films, tunable mechanical properties, and spatio-temporal control over film organization. The last few years have seen a significant increase in reports exploring the possibilities offered by diffusing molecules into films to control their internal structures or design "reservoirs," as well as control their mechanical properties. Such properties, associated with the chemical properties of films, are particularly important for designing biomedical devices that contain bioactive molecules. In this review, we highlight recent work on designing and controlling film properties at the nanometer and micrometer scales with a view to developing new biomaterial coatings, tissue engineered constructs that could mimic in vivo cellular microenvironments, and stem cell "niches."

Multiple Functionalities of Polyelectrolyte Multilayer Films: New Biomedical Applications

http://fanyanggroup.com/pdf/Biomaterials%202013%20Yang.pdf

The Future of Biologic Coatings for Orthopaedic Implants

This work received funding from the European Union's Seventh Framework Programme (FP7/2007-2013) under grant agreement no. REGPOT-CT2012-316331-POLARIS. The work was also funded by FEDER through the Competitive Factors Operational Program (COMPETE) and by National funds through the Portuguese Foundation for Science and Technology (FCT) in the scope of the projects PTDC/FIS/115048/2009 and PTDC/CTM-BIO/1814/2012. The authors gratefully acknowledge Dr. Luca Gasperini (3B's Research Group, University of Minho, Portugal) for his help with the figures.

Molecular Interactions Driving the Layer-by-Layer Assembly of Multilayers

Methods for depositing thin films are important in generating functional materials for diverse applications in a wide variety of fields. Over the last half-century, the layer-by-layer assembly of nanoscale films has received intense and growing interest. This has been fueled by innovation in the available materials and assembly technologies, as well as the film-characterization techniques. In this Review, we explore, discuss, and detail innovation in layer-by-layer assembly in terms of past and present developments, and we highlight how these might guide future advances. A particular focus is on conventional and early developments that have only recently regained interest in the layer-by-layer assembly field. We then review unconventional assemblies and approaches that have been gaining popularity, which include inorganic/organic hybrid materials, cells and tissues, and the use of stereocomplexation, patterning, and dip-pen lithography, to name a few. A relatively recent development is the use of layer-by...

https://minerva-access.unimelb.edu.au/bitstream/handle/11343/123195/Caruso_ChemRev_ms_rev.pdf

Innovation in Layer-by-Layer Assembly.

Beside chemical properties and topographical features, mechanical properties of gels have been recently demonstrated to play an important role in various cellular processes, including cell attachment, proliferation, and differentiation. In this work, we used multilayer films made of poly(L-lysine)/Hyaluronan (PLL/HA) of controlled stiffness to investigate the effects of mechanical properties of thin films on skeletal muscle cells (C2C12 cells) differentiation. Prior to differentiation, cells need to adhere and proliferate in growth medium. Stiff films (E(0) > 320 kPa) promoted formation of focal adhesions and organization of the cytoskeleton as well as an enhanced proliferation, whereas soft films were not favorable for cell anchoring, spreading or proliferation. Then C2C12 cells were switched to a low serum containing medium to induce cell differentiation, which was also greatly dependent on film stiffness. Although myogenin and troponin T expressions were only moderately affected by film stiffness, the morphology of the myotubes exhibited striking stiffness-dependent differences. Soft films allowed differentiation only for few days and the myotubes were very short and thick. Cell clumping followed by aggregates detachment could be observed after ~2 to 4 days. On stiffer films, significantly more elongated and thinner myotubes were observed for up to ~ 2 weeks. Myotube striation was also observed but only for the stiffer films. These results demonstrate that film stiffness modulates deeply adhesion, proliferation and differentiation, each of these processes having its own stiffness requirement.

Polyelectrolyte multilayer films of controlled stiffness modulate myoblast cells differentiation.

Efficient delivery of growth or survival factors to cells is one of the most important long-term challenges of current cell-based tissue engineering strategies. The extracellular matrix acts as a reservoir for a number of growth factors through interactions with its components. In the matrix, growth factors are protected against circulating proteases and locally concentrated. Thus, the localized and long-lasting delivery of a matrix-bound recombinant human bone morphogenetic protein 2 (rhBMP-2) from a biomaterial surface would mimic in vivo conditions and increase BMP-2 efficiency by limiting its degradation. Herein, it is shown that crosslinked poly(L-lysine)/hyaluronan (HA) layer-by-layer films can serve as a reservoir for rhBMP-2 delivery to myoblasts and induce their differentiation into osteoblasts in a dose-dependent manner. The amount of rhBMP-2 loaded in the films is controlled by varying the deposition conditions and the film thickness. Its local concentration in the film is increased up to approximately 500-fold when compared to its initial solution concentration. Its adsorption on the films, as well as its diffusion within the films, is evidenced by microfluorimetry and confocal microscopy observations. A direct interaction of rhBMP-2 with HA is demonstrated by size-exclusion chromatography, which could be at the origin of the rhBMP-2 "trapping" in the film and of its low release from the films. The bioactivity of rhBMP-2-loaded films is due neither to film degradation nor to rhBMP-2 release. The rhBMP-2-containing films are extremely resistant and could sustain three successive culture sequences while remaining bioactive, thus confirming the important and protective effect of rhBMP-2 immobilization. These films may find applications in the local delivery of immobilized growth factors for tissue-engineered constructs and for metallic biomaterial surfaces, as they can be deposited on a wide range of substrates with different shapes, sizes, and composition.

/pdf/layer-by-layer-films-as-a-biomimetic-reservoir-for-rhbmp-2-4uie6u7t5d.pdf

Layer‐By‐Layer Films as a Biomimetic Reservoir for rhBMP‐2 Delivery: Controlled Differentiation of Myoblasts to Osteoblasts

In recent years, the layer-by-layer technique has grown in various fields. One of the emerging trends of bio-applications is the use of polysaccharides as main film components, which stems from their intrinsic physical, chemical and biological properties. These allow the simple formation, by self-assembly, of new kinds of mimics of extra-cellular matrices from plant and animal tissues. These assemblies, which possess specific properties arising from their hydration and internal composition, can indeed contain additional functionalities obtained by chemical modification of the biopolymers or film post-processing. They can be molded into different forms (films, membranes, and capsules).

Thomas Crouzier

Papers

Multiple Functionalities of Polyelectrolyte Multilayer Films: New Biomedical Applications

Polyelectrolyte multilayer films of controlled stiffness modulate myoblast cells differentiation.

Layer‐By‐Layer Films as a Biomimetic Reservoir for rhBMP‐2 Delivery: Controlled Differentiation of Myoblasts to Osteoblasts

Polysaccharide-based polyelectrolyte multilayers

Ion pairing and hydration in polyelectrolyte multilayer films containing polysaccharides.