Microscale patterning of hydrogel stiffness through light-triggered uncaging of thiols
Literature Information
Katarzyna A. Mosiewicz, Laura Kolb, Matthias P. Lutolf
Mammalian cell behavior is strongly influenced by physical and chemical cues originating from the extracellular matrix (ECM). In vivo, ECM signals are displayed in a spatiotemporally complex fashion, often composed as gradients and in concentration profiles that change in time. Most in vitro models to study the role of ECM signals in regulating cell behavior are limited in capturing this microenvironmental complexity, as they are static and homogeneous. In order to achieve a dynamic control of the physical properties of a hydrogel network, we here designed a chemical scheme to control poly(ethylene glycol) (PEG) hydrogel stiffness in space, time and intensity. Specifically, we combined caging chemistry and Michael-type addition to enable the light-triggered local control of hydrogel crosslinking density. Thiol moieties of one of the reactive PEG macromers undergoing crosslinking were equipped with caging groups to prevent their susceptibility to the counter-reactive vinyl sulfone groups on the termini of the complementary PEG macromers. Thus, the crosslinking density of the hydrogel network could be tuned by uncaging with light which directly translated into differential patterns of hydrogel stiffness. Using this approach, user-defined stiffness patterns in a range of soft tissue microenvironments (i.e. between 3–8 kPa) were obtained and shown to influence the migratory behavior of primary human mesenchymal stem cells (hMSC). Stiffness gradients in the higher range (5.5–8 kPa) were able to elicit durotaxis towards the more densely crosslinked regions, whereas those in the lower range (3–5.5 kPa) showed no significant directional preference in hMSC migration. Our patterning tool should be useful for the manipulation of cell fate in various other contexts.
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Biomaterials Science

Biomaterials Science is an international high impact journal exploring the science of biomaterials and their translation towards clinical use. Its scope encompasses new concepts in biomaterials design, studies into the interaction of biomaterials with the body, and the use of materials to answer fundamental biological questions. Papers do not necessarily need to report a new biomaterial but should provide novel insight into the biological applications of the biomaterial. Articles that primarily focus on demonstrating novel materials chemistry and bring a molecular picture to bear on a given material’s suitability as a biomaterial are more suited to our companion journal, Journal of Materials Chemistry B. Biomaterials Science publishes primary research and review-type articles in the following areas: molecular design of biomaterials, including translation of emerging chemistries to biomaterials science of cells and materials at the nanoscale and microscale materials as model systems for stem cell and human biology materials for tissue engineering and regenerative medicine (Nano)materials and (nano)systems for therapeutic delivery interactions at the biointerface biologically inspired and biomimetic materials, including bio-inspired self-assembly systems and cell-inspired synthetic tools next-generation biomaterials tools and methods
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