Copolymerization of Metal Nanoparticles: A Route to Colloidal Plasmonic Copolymers

Liu, Kun; Lukach, Ariella; Sugikawa, Kouta; Chung, Shinjae; Vickery, Jemma; Thérien-Aubin, Héloı̈se; Yang, Bai; Rubinstein, Michael; Kumacheva, Eugenia

doi:10.1002/anie.201309718

Cited by 80 publications

(67 citation statements)

References 49 publications

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“…[3a,e,f, 5, 6] Such ap rocess is analogous to polymerization in synthetic polymers but occurs at considerably larger length scales,s imilar to that observed in nanoparticle and Streptobacillus systems. [2,7] For example,P ochan et al prepared spherical micelles of poly(acrylic acid)-block-poly(methyl acrylate)-block-polystyrene in solution. [8] After introducing tetrahydrofuran (THF) into the solution in the presence of diamines,t he micelles underwent as phere-to-disk morphological transition, which allowed for preferential growth of the micelles in one dimension to form cylindrical nanostructures with alternating lamellae.T he success in creating such nanostructures by polymerizing pre-assemblies can be attributed to adirected stepwise self-assembly process that is facilitated by the anisotropy of the disk-like pre-assemblies and long-range electrostatic interactions between charged blocks with multivalent counterions.A lthough reports are available on the stepwise self-assembly process, [9] understanding the underlying principles still presents ac hallenge because of the complexity of these processes.Herein, we demonstrate astepwise self-assembly methodology for achieving one-dimensional growth of anisotropic pre-assemblies.O ur previous studies revealed that polypeptide-based graft copolymers bearing rigid a-helix blocks are able to self-assemble into distinct aggregates with unique structures,for example,anisotropic spindle-like micelles.…”

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confidence: 99%

“…Electron microscopy images also revealed that the length of the nanowires (associated with the number of repeat subunits) exhibited polydispersity.T oobtain insights into the structural details of the nanowires,wecalculated the number fraction f X of the nanowires with degree of polymerization (X). [7,11] This value was obtained by collecting SEM images with more than 400 micelles and then analyzing the images using Image-Pro Plus software (Supporting Information, Section 2). Here,t he degree of polymerization is defined as the number of spindles in ananowire.Asshown in Figure 1f, f X exhibited an exponential decay,and the number fraction of unreacted spindles (X = 1) was approximately 0.495.…”

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Hierarchical Nanowires Synthesized by Supramolecular Stepwise Polymerization

et al. 2016

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The self-organization of pre-assembled aggregates is an efficient stepwise strategy for fabricating nanostructures with a second level of hierarchy. Herein, we report that anisotropic spindle-like micelles, self-assembled from polypeptide graft copolymers with rigid backbones, can serve as ideal pre-assembled subunits for constructing one-dimensional materials with hierarchical structures. By adding organic solvents and dialyzing against water, reactive points can be generated at the ends of the spindle-like micelles, which subsequently drive the anisotropic micelles to grow as rods in a chain and eventually self-assemble into hierarchical nanowires in a stepwise manner. The second self-assembly step is a hierarchical process that resembles step polymerization. Hierarchical structures can be precisely synthesized by this new type of polymerization. These nanostructures can be tailored by the activity of the reactive points, which depends on the nature of the solvent and the molecular architecture.

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Hierarchical Nanowires Synthesized by Supramolecular Stepwise Polymerization

et al. 2016

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“…[1][2][3][4] To form am aterial with ad esired nanostructure,f undamental understanding has to be developed about the governing principles of the coassembly process.For example,the structure of linear chains assembled from different types of plasmonic NPs depends on the relationship between the rate of self-assembly of each individual component and the rate of coassembly. [5,6] Alternatively,o ne of the components can function as at emplate for the spatial organization of the second one. [7] Ap articularly interesting case is entropically mediated coassembly of NPs with different shapes,f or example,n anorods and nanospheres.T hese systems exhibit av ariety of structures,i ncluding macroscopic demixing of rods and spheres as well as microscopic and nanoscopic phase separation into layers of rods alternating with layers of spheres.…”

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Coassembly of Nanorods and Nanospheres in Suspensions and in Stratified Films

et al. 2015

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The entropically driven coassembly of nanorods (cellulose nanocrystals, CNCs) and nanospheres (dye-labeled spherical latex nanoparticles, NPs) was studied in aqueous suspensions and in solid films. In mixed CNC-latex suspensions, phase separation into an isotropic latex-NP-rich and a chiral nematic CNC-rich phase took place; the latter contained a significant amount of latex NPs. Drying the mixed suspension resulted in CNC-latex films with planar disordered layers of latex NPs, which alternated with chiral nematic CNC-rich regions. In addition, fluorescent latex NPs were embedded in the chiral nematic domains. The stratified morphology of the films, together with a random distribution of latex NPs in the anisotropic phase, led to the films having close-to-uniform fluorescence, birefringence, and circular dichroism properties.

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“…Compared with individual AuNPs, the surface plasmon resonance peak of one dimensional (1-D) chains had a large red-shift from 530 to 625 nm, which possibly arose from the 1-D transverse plasmon coupling between AuNPs along chains 44. It further confirms the morphological transition of assemblies in solution at different pHs 45.…”

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pH-programmable self-assembly of plasmonic nanoparticles: hydrophobic interaction versus electrostatic repulsion

Kanyó

Kuo

et al. 2015

Nanoscale

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We report a general strategy to conceptualize a new design for the pH-programmable self-assembly of plasmonic gold nanoparticles (AuNPs) tethered by random copolymers of poly(styrene-co-acrylic acid) (P(St-co-AA)). It is based on using pH as an external stimulus to reversibly change the surface charge of polymer tethers and to control the delicate balance of interparticle attractive and repulsive interactions. By incorporating -COOH moieties locally within PSt hydrophobic segments, the change in the ionization degree of -COOH moieties can dramatically disrupt the hydrophobic attraction within a close distance. pH acts as a key parameter to control the deprotonation of -COOH moieties and "programs" the assembled nanostructures of plasmonic nanoparticles in a stepwise manner. At a higher solution pH where -COOH groups of polymer tethers became highly deprotonated, electrostatic repulsion dominated the self-assembly and favored the formation of end-to-end, anisotropic assemblies, e.g. 1-D single-line chains. At a lower pH, the less deprotonated -COOH groups led to the decrease of electrostatic repulsion and the side-to-side aggregates, e.g. clusters and multi-line chains of AuNPs, became favorable. The pH-programmable self-assembly allowed us to engineer a "manual" program for a sequential self-assembly by changing the pH of the solution. We demonstrated that the two-step pH-programmable assembly could generate more sophisticated "multi-block" chains using two differently sized AuNPs. Our strategy offers a general means for the programmable design of plasmonic nanoparticles into the specific pre-ordained nanostructures that are potentially useful for the precise control over their plasmon coupling.

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Copolymerization of Metal Nanoparticles: A Route to Colloidal Plasmonic Copolymers

Cited by 80 publications

References 49 publications

Hierarchical Nanowires Synthesized by Supramolecular Stepwise Polymerization

Hierarchical Nanowires Synthesized by Supramolecular Stepwise Polymerization

Coassembly of Nanorods and Nanospheres in Suspensions and in Stratified Films

pH-programmable self-assembly of plasmonic nanoparticles: hydrophobic interaction versus electrostatic repulsion

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