3D Volumetric Structural Hierarchy Induced by Colloidal Polymerization of a Quantum-Dot Ionic Liquid Monomer Conjugate

Welch, Paul M.; Dreier, Timothy A.; Magurudeniya, Harsha D.; Frith, Matthew G.; Ilavsky, Jan; Seifert, Sönke; Rahman, Aunik K.; Rahman, Anis; Singh, Amita Joshi; Ringstrand, Bryan S.; Hanson, Christina J.; Hollingsworth, Jennifer A.; Firestone, Millicent A.

doi:10.1021/acs.macromol.0c00011

Title: 3D Volumetric Structural Hierarchy Induced by Colloidal Polymerization of a Quantum-Dot Ionic Liquid Monomer Conjugate

Journal Article · Wed Apr 15 00:00:00 EDT 2020 · Macromolecules

DOI:https://doi.org/10.1021/acs.macromol.0c00011· OSTI ID:1630700

^[1]; Dreier, Timothy A. ^[1]; Magurudeniya, Harsha D. ^[1];

^[2]; Ilavsky, Jan ^[2]; Seifert, Sönke ^[2]; Rahman, Aunik K. ^[3];

^[4]; Singh, Amita Joshi ^[1];

^[1]; Hanson, Christina J. ^[1];

^[1];

^[1]

Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Applied Research & Photonics, Inc., Harrisburg, PA (United States)
Applied Research & Photonics, Inc., Harrisburg, Pennsylvania 17111, United States

Hierarchically structured emissive quantum dot (CdS/CdSe) poly(ionic liquid) composites are synthesized through colloidal polymerization within a lyotropic liquid crystal, yielding a solvent-responsive nanoparticle (NP) composite possessing four ordered structural motifs. The composite is prepared by coassembling an amphiphilic ionic liquid (IL) monomer, 3-decyl-1-vinylimidazolium chloride, [C₁₀VIm⁺][Cl^-], and IL monomer, 3-(10-mercaptodecyl)-1-vinylimidazolium bromide surface-functionalized quantum dots, QD-[SC₁₀VIm⁺][Br^-], in 30 wt % water. Photo (UV)-initiated free radical polymerization serves to form a colloidal copolymer that collimates pairs of QDs within the core of large cylinders (average diameter = 21 nm and length = 422 nm), as evidenced by ultrasmall-angle X-ray scattering (USAXS). As revealed by continuous wave terahertz multispectral reconstructive 3-D imaging, the subsurface structure along the cylinder axis undergoes dynamic rearrangement between 2D hexagonal and cubic packing. The polymerized ionic liquid sheath surrounding the QDs is composed of concentric hexagonally perforated lamellae (HPL) with an interlamellar repeat distance of 3 nm, as determined by small-angle X-ray scattering (SAXS). The encapsulated QDs retain crystallinity (TEM and WAXS) and emission characteristics (photoluminescence spectroscopy, lambda(EM) = 638 nm). Phenomenological time-dependent Ginzburg-Landau calculations verify the mesoscale cylinders arise from the topological constraints imposed by the in-plane perforations of the polymerized ionic liquid as it wraps around the hard (unmalleable) spherical QDs.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1630700

Journal Information:: Macromolecules, Vol. 53, Issue 8; ISSN 0024-9297

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 2 works

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Title: 3D Volumetric Structural Hierarchy Induced by Colloidal Polymerization of a Quantum-Dot Ionic Liquid Monomer Conjugate

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