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Locating Reactive Groups on Nanomaterials with Gold Nanoclusters: Toward a Surface Reactive Site Map

2017-05-23, Thomas, Steffi S., Coleman, Matthew, Carroll, Emma, Polo, Ester, Meder, Fabian, Dawson, Kenneth A.

Nanoparticles (NPs) are often functionalized with reactive groups like amines or thiols for the subsequent conjugation of further molecules, e.g., stabilizing polymers, drugs and proteins or targeting cells or specific diseases, etc. In addition to the quantitative estimation of the reactive conjugation sites, their nanoscale and molecular positioning and local arrangement on single nanoparticles becomes more and more important for tailored engineering and design of functional nanomaterials. Here, we use maleimide or sulfo-succinimidyl ester modified 1.4 nm gold nanoclusters (AuNCs) to specifically label reactive thiol and amine groups with sub –2 nm precision on metal oxide and polymeric nanostructures. We confirm the binding of AuNCs by measuring and modelling sedimentation properties using analytical centrifugation, image their surface distribution and surface distances by transmission electron microscopy (TEM), and compare the results to ensemble measurements of numbers of reactive surface groups obtained by common photometric assays. We map thiol and amine groups introduced on silica NPs (SiNPs), titania stars (Ti), silica inverse opals (SiOps), and polystyrene NPs (PS NPs). We show that the method is suitable to map local, clustered inhomogeneities of the reactive sites on single SiNPs introduced by masking certain areas during surface functionalization. Mapping precise positions of reactive surface groups is essential for the design and the tailored ligation of multifunctional nanomaterials.

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Ordered Surface Structuring of Spherical Colloids with Binary Nanoparticle Superlattices

2018-03-26, Meder, Fabian, Thomas, Steffi S., Bollhorst, Tobias, Dawson, Kenneth A.

Surface-patterning colloidal matter in the sub-10 nm regime generates exceptional functionality in biology and photonic and electronic materials. Techniques of artificially generating functional patterns in the small nanoscale advanced in a fascinating manner in the last several years. However, they remain often restricted to planar and noncolloidal substrates. Patterning colloidal matter in solution via bottom-up assembly of smaller subunits on larger core particles is highly challenging because it is necessary to force the subunits onto randomly moving objects. Consequently, the non-equilibrium conditions present during nanoparticle self-assembly are difficult to control to eventually achieve the desired material structures. Here, we describe the formation of surface patterns with intrinsic periodic repeats of 8.9 ± 0.9 nm and less on hard, amorphous colloidal core particles by assembling binary nanoparticle superlattices on the curved particle surface. The colloidal environment is preserved during the entire bottom-up crystallization of variable building blocks (here, monodispersed 5 nm Au and 2.4 nm Pd nanoparticles (NPs) and 230 nm SiO core particles) into AB -like, binary, and isotropic superlattice domains on the amorphous cores. The three-dimensional, bottom-up assembly technique is a new tool for patterning colloidal matter in the sub-10 nm surface regime for gaining access to multicomponent metamaterials for bionanoscience, photonics, and electronics. 2 13