Multifunctional nanoarchitectures from DNA-based ABC monomers

The ability to attach different functional moieties to a molecular building block1,2 could lead to applications in nanoelectronics3, nanophotonics4, intelligent sensing5 and drug delivery6,7. The building unit needs to be both multivalent and anisotropic, and although many anisotropic building blocks have been created1,8,9,10,11,12, these have not been universally applicable. Recently, DNA has been used to generate various nanostructures13,14,15,16,17 or hybrid systems18,19,20,21,22,23,24,25, and as a generic building block for various applications26,27,28,29,30. Here, we report the creation of anisotropic, branched and crosslinkable building blocks (ABC monomers) from which multifunctional nanoarchitectures have been assembled. In particular, we demonstrate a target-driven polymerization process in which polymers are generated only in the presence of a specific DNA molecule, leading to highly sensitive pathogen detection. Using this monomer system, we have also designed a biocompatible nanovector that delivers both drugs and tracers simultaneously. Our approach provides a general yet versatile route towards the creation of a range of multifunctional nanoarchitectures. Supplementary information The online version of this article (doi:10.1038/nnano.2009.93) contains supplementary material, which is available to authorized users.

[1]  F. Szoka,et al.  A single dose of doxorubicin-functionalized bow-tie dendrimer cures mice bearing C-26 colon carcinomas , 2006, Proceedings of the National Academy of Sciences.

[2]  P. Alivisatos.  The use of nanocrystals in biological detection , 2004, Nature Biotechnology.

[3]  P. McEuen,et al.  Controlled assembly of dendrimer-like DNA , 2004, Nature materials.

[4]  Mehmet Toner,et al.  Multifunctional Encoded Particles for High-Throughput Biomolecule Analysis , 2007, Science.

[5]  G. Calzaferri,et al.  Orthogonally Bifunctional Fluorescent Zeolite‐L Microcrystals , 2008 .

[6]  Dan Luo,et al.  Multiplexed detection of pathogen DNA with DNA-based fluorescence nanobarcodes , 2005, Nature Biotechnology.

[7]  Hao Yan,et al.  Self-assembled combinatorial encoding nanoarrays for multiplexed biosensing. , 2007, Nano letters.

[8]  Soong Ho Um,et al.  Dendrimer-like DNA-based fluorescence nanobarcodes , 2006, Nature Protocols.

[9]  K. Leong,et al.  Multifunctional nanorods for gene delivery , 2003, Nature materials.

[10]  Robert M. Dirks,et al.  An autonomous polymerization motor powered by DNA hybridization , 2007, Nature Nanotechnology.

[11]  Russell P. Goodman,et al.  Reconfigurable, braced, three-dimensional DNA nanostructures. , 2008, Nature nanotechnology.

[12]  Wenlong Cheng,et al.  Nanopatterning self-assembled nanoparticle superlattices by moulding microdroplets. , 2008, Nature nanotechnology.

[13]  A Paul Alivisatos,et al.  Two-dimensional nanoparticle arrays show the organizational power of robust DNA motifs. , 2006, Nano letters.

[14]  Soong Ho Um,et al.  Enzyme-catalysed assembly of DNA hydrogel , 2006, Nature materials.

[15]  Hao Yan,et al.  Layer-by-layer assembly of nanowires for three-dimensional, multifunctional electronics. , 2007, Nano letters.

[16]  A. Alivisatos,et al.  Isolation of discrete nanoparticle-DNA conjugates for plasmonic applications. , 2008, Nano letters.

[17]  Joseph M Slocik,et al.  Peptide-assembled optically responsive nanoparticle complexes. , 2007, Nano letters.

[18]  S. Glotzer,et al.  Anisotropy of building blocks and their assembly into complex structures. , 2007, Nature materials.

[19]  Gion Calzaferri,et al.  Self-assembling living systems with functional nanomaterials. , 2007, Angewandte Chemie.

[20]  P. Rothemund.  Folding DNA to create nanoscale shapes and patterns , 2006, Nature.

[21]  Hao Yan,et al.  Programmable DNA self-assemblies for nanoscale organization of ligands and proteins. , 2005, Nano letters.

[22]  Christof M. Niemeyer,et al.  Rational Design of DNA Nanoarchitectures , 2006 .

[23]  M. Persson,et al.  Nano-architectures by covalent assembly of molecular building blocks. , 2007, Nature nanotechnology.

[24]  Chad A Mirkin,et al.  Asymmetric functionalization of gold nanoparticles with oligonucleotides. , 2006, Journal of the American Chemical Society.

[25]  Francis C Szoka,et al.  Designing dendrimers for biological applications , 2005, Nature Biotechnology.

[26]  C. Mao,et al.  Hierarchical self-assembly of DNA into symmetric supramolecular polyhedra , 2008, Nature.

[27]  Hao Yan,et al.  Self-assembled DNA nanostructures for distance-dependent multivalent ligand-protein binding. , 2008, Nature nanotechnology.

[28]  N. Seeman.  DNA in a material world , 2003, Nature.

[29]  Vladimir P Torchilin,et al.  Multifunctional nanocarriers. , 2006, Advanced drug delivery reviews.

[30]  A Paul Alivisatos,et al.  Discrete nanostructures of quantum dots/Au with DNA. , 2004, Journal of the American Chemical Society.