Ordering in Polymer Micelle-Directed Assemblies of Colloidal Nanocrystals

Ong, Gary K.; Williams, Teresa E.; Singh, Ajay; Schaible, Eric; Helms, Brett A.; Milliron, Delia J.

doi:10.1021/acs.nanolett.5b03765

Cited by 21 publications

(13 citation statements)

References 42 publications

(59 reference statements)

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“…2a) for the ITO-PEG flowing dispersion of lowest [PEG] emerging at a lower q than that indicative of NC-NC correlation (see SI, Fig. S6 for full q range S(q)), thus characteristic of intermediate range order (IRO) in colloidal assemblies (48,60,61) . Considering the IRO behavior of this ITO-PEG mixture ([PEG]=8.00 mM), we establish that competing short-range attractions and long-range repulsions frustrate large scale aggregation and lead to the formation of discrete ITO NC clusters (~270 Å length scale) dispersed in ACN.…”

Section: Insets)mentioning

confidence: 99%

Gelation of plasmonic metal oxide nanocrystals by polymer-induced depletion attractions

Cabezas

Ong

Jadrich

et al. 2018

Proc. Natl. Acad. Sci. U.S.A.

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Gelation of colloidal nanocrystals emerged as a strategy to preserve inherent nanoscale properties in multiscale architectures. However, available gelation methods to directly form self-supported nanocrystal networks struggle to reliably control nanoscale optical phenomena such as photoluminescence and localized surface plasmon resonance (LSPR) across nanocrystal systems due to processing variabilities. Here, we report on an alternative gelation method based on physical internanocrystal interactions: short-range depletion attractions balanced by long-range electrostatic repulsions. The latter are established by removing the native organic ligands that passivate tin-doped indium oxide (ITO) nanocrystals while the former are introduced by mixing with small PEG chains. As we incorporate increasing concentrations of PEG, we observe a reentrant phase behavior featuring two favorable gelation windows; the first arises from bridging effects while the second is attributed to depletion attractions according to phase behavior predicted by our unified theoretical model. Our assembled nanocrystals remain discrete within the gel network, based on X-ray scattering and high-resolution transmission electron microscopy. The infrared optical response of the gels is reflective of both the nanocrystal building blocks and the network architecture, being characteristic of ITO nanocrystals' LSPR with coupling interactions between neighboring nanocrystals.

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Section: Insets)mentioning

confidence: 99%

Gelation of plasmonic metal oxide nanocrystals by polymer-induced depletion attractions

Cabezas

Ong

Jadrich

et al. 2018

Proc. Natl. Acad. Sci. U.S.A.

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“…Efforts have led to wide ranging applications for porous nanomaterials arising from their novel electronic, catalytic, optical, and biological properties . There has been significant progress using the self‐assembly of block copolymers to realize well‐defined nanomaterials with a range of morphologies, compositions, and dimensions . Despite the widespread production and use of nanomaterials, there remains a need for “materials by design” approaches that support predictable and tailored architectures.…”

Section: Introductionmentioning

confidence: 99%

Full Gamut Wall Tunability from Persistent Micelle Templates via Ex Situ Hydrolysis

Lantz

Clamp

Bergh

et al. 2019

Small

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The predictive self‐assembly of tunable nanostructures is of great utility for broad nanomaterial investigations and applications. The use of equilibrium‐based approaches however prevents independent feature size control. Kinetic‐controlled methods such as persistent micelle templates (PMTs) overcome this limitation and maintain constant pore size by imposing a large thermodynamic barrier to chain exchange. Thus, the wall thickness is independently adjusted via addition of material precursors to PMTs. Prior PMT demonstrations added water‐reactive material precursors directly to aqueous micelle solutions. That approach depletes the thermodynamic barrier to chain exchange and thus limits the amount of material added under PMT‐control. Here, an ex situ hydrolysis method is developed for TiO2 that mitigates this depletion of water and nearly decouples materials chemistry from micelle control. This enables the widest reported PMT range (M:T = 1.6–4.0), spanning the gamut from sparse walls to nearly isolated pores with ≈2 Å precision adjustment. This high‐resolution nanomaterial series exhibits monotonic trends where PMT confinement within increasing wall‐thickness leads to larger crystallites and an increasing extent of lithiation, reaching Li0.66TiO2. The increasing extent of lithiation with increasing anatase crystallite dimensions is attributed to the size‐dependent strain mismatch of anatase and bronze polymorph mixtures.

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“…[22][23][24] The short range attraction is caused by van der Walls forces or solvent effects, 25 while the long range repulsion can be generated by many factors. For instance, it can be caused by electrostatic repulsion in charged colloids and molecules, 26,27 or by soft shells ad in the case of spherical colloids obtained by PEG aggregates [28][29][30] or even by a polymeric brush, as metallic NP [31][32][33][34][35] decorated with polymers and star polymers. 36 From experimental 28,29 and computational 31,32 works, is well known that the SALR NP and colloids effective interaction can be depicted by core-softened potentials.…”

Section: Introductionmentioning

confidence: 99%

Hard core-soft shell particles near repulsive interfaces: interplay between adsorption, aggregation and diffusion

Marques,

Bordin

2021

Preprint

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The behavior of colloidal particles with a hard core and a soft shell has attracted the attention for researchers in the physical-chemistry interface not only due the large number of applications, but due the unique properties of these systems in bulk and at interfaces. The adsorption at the boundary of two phases can provide information related to a fluid to clusters transition and with a minima in the contact layer diffusion -and is explained by the competition between the scales in the core-softened interaction. Due the long range repulsion, the particles stay at the distance correspondent to this length scale at low densities, and overcome the repulsive barrier as the packing increases, However, increasing the temperature, the gain in kinetic energy allows the colloids to overcome the long range repulsion barrier even at low densities. As consequence, there is no competition and no maxima was observed in the adsorption.

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Ordering in Polymer Micelle-Directed Assemblies of Colloidal Nanocrystals

Cited by 21 publications

References 42 publications

Gelation of plasmonic metal oxide nanocrystals by polymer-induced depletion attractions

Gelation of plasmonic metal oxide nanocrystals by polymer-induced depletion attractions

Full Gamut Wall Tunability from Persistent Micelle Templates via Ex Situ Hydrolysis

Hard core-soft shell particles near repulsive interfaces: interplay between adsorption, aggregation and diffusion

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