Abstract

We report a photolithographic method for the shape control of DNA hydrogels based on photo-activated self-assembly of Y-shaped DNA nanostructures (Y-motifs). To date, various methods to control the shape of DNA hydrogels have been developed to enhance the functions of the DNA hydrogel system. However, photolithographic production of shape-controlled DNA hydrogels formed through the self-assembly of DNA nanostructures without the use of radical polymerizations has never been demonstrated, although such a method is expected to be applied for the shape-control of DNA hydrogels encapsulating sensitive biomolecules, such as proteins. In this study, we used a photo-activated linker to initiate the self-assembly of Y-motifs, where the cross-linker DNA was at first inactive but was activated after UV light irradiation, resulting in the formation of shape-controlled DNA hydrogels only at the UV-exposed area produced by photomasks. We believe that this method will be applied for the construction of biohybrid machines, such as molecular robots and artificial cells that contain intelligent biomolecular devices, such as molecular sensors and computers.

Highlights

  • DNA hydrogels[1,2,3,4,5] have attracted much attention[6–9] due to their programmable functions, biocompatibility, and their applicability, such as in drug delivery systems,[10,11] cell-free protein synthesis,[12] artificial cytoskeletons for artificial cells,[13] mechanical micromachines,[14] and locomotive micromaterials.[15]

  • We report a photolithographic method for the shape control of DNA hydrogels based on photo-activated self-assembly of Y-shaped DNA nanostructures (Y-motifs)

  • Y-motifs A and B are three-branched nanostructures composed of 16-base double-stranded stems and 9base single-stranded sticky ends, which are constructed from three single-stranded DNAs (YA-1, YA-2, and YA-3 for Y-motif A; YB-1, YB-2, and YB-3 for Y-motif B)

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Summary

Introduction

DNA hydrogels[1,2,3,4,5] have attracted much attention[6–9] due to their programmable functions, biocompatibility, and their applicability, such as in drug delivery systems,[10,11] cell-free protein synthesis,[12] artificial cytoskeletons for artificial cells,[13] mechanical micromachines,[14] and locomotive micromaterials.[15]. (i)–(iii), the gelation of the DNA hydrogels is based on specific. To enhance the functions of DNA hydrogels, various approaches have been used to control their shape. The most frequently used method for shape control is the gelation of DNA hydrogel using a designed mold.[15,18,26]. Researchers have achieved the shape control of DNA hydrogels without molds. Li et al demonstrated three-dimensional bioprinting of millimeter-sized DNA-cross-linked polypeptide hydrogels, based on the ink-jet-like discharge from the scanning nozzle.[19]. Wang et al demonstrated the surface-initiated pattern formation of DNA-motif hydrogels, based on the clamped hybridization chain reaction,[16] where DNA strands were elongated from the initiator DNAs micropatterned on a glass surface, resulting in DNA-motif hydrogels patterned in the scale of several hundred micrometers. Shape-controlled DNA-motif hydrogel formation based on patterned photo-irradiation was reported.

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