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

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.

View Accepted Manuscript (DOE)

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

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1630700

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

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

Solvent-Mediated Plasmon Tuning in a Gold-Nanoparticle-Poly(Ionic Liquid) Composite Batra, D.; Seifert, S.; Varela, L. M. Advanced Functional Materials, Vol. 17, Issue 8 https://doi.org/10.1002/adfm.200600797	journal	April 2007
Higher-Order Organization by Mesoscale Self-Assembly and Transformation of Hybrid Nanostructures Cölfen, Helmut; Mann, Stephen Angewandte Chemie International Edition, Vol. 42, Issue 21 https://doi.org/10.1002/anie.200200562	journal	May 2003
Exceptionally Mild Reactive Stripping of Native Ligands from Nanocrystal Surfaces by Using Meerwein’s Salt Rosen, Evelyn L.; Buonsanti, Raffaella; Llordes, Anna Angewandte Chemie International Edition, Vol. 51, Issue 3, p. 684-689 https://doi.org/10.1002/anie.201105996	journal	December 2011
Self-Assembly Directed Organization of Nanodiamond During Ionic Liquid Crystalline Polymer Formation Ringstrand, Bryan S.; Seifert, Sönke; Podlesak, David W. Macromolecular Rapid Communications, Vol. 37, Issue 14 https://doi.org/10.1002/marc.201600070	journal	May 2016
Synthesis and application of a metal ion coordinating ionic liquid monomer: Towards size and dispersity control of nanoparticles formed within a structured polyelectrolyte Dreier, Timothy A.; Ringstrand, Bryan S.; Seifert, Sönke European Polymer Journal, Vol. 107 https://doi.org/10.1016/j.eurpolymj.2018.08.017	journal	October 2018
Effects of thiol ligands on the growth and stability of CdS nanoclusters Nasraoui, Sabah; Attia, Ghada; Haj Mohamed, Naim Bel Journal of Molecular Structure, Vol. 1198 https://doi.org/10.1016/j.molstruc.2019.07.079	journal	December 2019
Comparative photoluminescence properties of type-I and type-II CdTe/CdS core/shell quantum dots Thuy, Ung Thi Dieu; Tu, Le Anh; Loan, Nguyen Thu Optical Materials, Vol. 53 https://doi.org/10.1016/j.optmat.2016.01.022	journal	March 2016
Optical properties of core/multishell CdSe/Zn(S,Se) nanocrystals Bleuse, Joël; Carayon, Sophie; Reiss, Peter Physica E: Low-dimensional Systems and Nanostructures, Vol. 21, Issue 2-4 https://doi.org/10.1016/j.physe.2003.11.044	journal	March 2004
Colloidal polymers from inorganic nanoparticle monomers Hill, Lawrence J.; Pinna, Nicola; Char, Kookheon Progress in Polymer Science, Vol. 40 https://doi.org/10.1016/j.progpolymsci.2014.08.003	journal	January 2015
Advances in transition-metal catalyzed thioetherification reactions of aromatic compounds Ghaderi, Arash Tetrahedron, Vol. 72, Issue 32 https://doi.org/10.1016/j.tet.2016.06.067	journal	August 2016
A one-pot, efficient, and odorless synthesis of symmetrical disulfides using organic halides and thiourea in the presence of manganese dioxide and wet polyethylene glycol (PEG-200) Firouzabadi, Habib; Iranpoor, Nasser; Abbasi, Mohammad Tetrahedron Letters, Vol. 51, Issue 3 https://doi.org/10.1016/j.tetlet.2009.11.060	journal	January 2010
Distance-Dependence of Interparticle Energy Transfer in the Near-Infrared within Electrostatic Assemblies of PbS Quantum Dots Kodaimati, Mohamad S.; Wang, Chen; Chapman, Craig ACS Nano, Vol. 11, Issue 5 https://doi.org/10.1021/acsnano.7b01778	journal	April 2017
Electrochemical Activity of Glucose Oxidase on a Poly(ionic liquid)–Au Nanoparticle Composite Lee, Sungwon; Ringstrand, Bryan S.; Stone, David A. ACS Applied Materials & Interfaces, Vol. 4, Issue 5 https://doi.org/10.1021/am300629n	journal	May 2012
Formation of a Biomimetic, Liquid-Crystalline Hydrogel by Self-Assembly and Polymerization of an Ionic Liquid Batra, Dolly; Firestone, Millicent A. Chemistry of Materials, Vol. 19, Issue 18 https://doi.org/10.1021/cm062992z	journal	September 2007
Degradation Products from Consumer Nanocomposites: A Case Study on Quantum Dot Lighting Liu, Jingyu; Katahara, John; Li, Guanglai Environmental Science & Technology, Vol. 46, Issue 6 https://doi.org/10.1021/es204430f	journal	March 2012
Time-Dependent Photoluminescence Blue Shift of the Quantum Dots in Living Cells: Effect of Oxidation by Singlet Oxygen Zhang, Yu; He, Jia; Wang, Pei-Nan Journal of the American Chemical Society, Vol. 128, Issue 41 https://doi.org/10.1021/ja061225y	journal	October 2006
New Insights into the Complexities of Shell Growth and the Strong Influence of Particle Volume in Nonblinking “Giant” Core/Shell Nanocrystal Quantum Dots Ghosh, Yagnaseni; Mangum, Benjamin D.; Casson, Joanna L. Journal of the American Chemical Society, Vol. 134, Issue 23 https://doi.org/10.1021/ja212032q	journal	May 2012
Flexible Polymer-Assisted Mesoscale Self-Assembly of Colloidal CsPbBr ₃ Perovskite Nanocrystals into Higher Order Superstructures with Strong Inter-Nanocrystal Electronic Coupling Yang, Yang; Lee, Jacob T.; Liyanage, Thakshila Journal of the American Chemical Society, Vol. 141, Issue 4 https://doi.org/10.1021/jacs.8b10083	journal	December 2018
Solvent Tunable Optical Properties of a Polymerized Vinyl- and Thienyl-Substituted Ionic Liquid ^† Becht, Gregory A.; Lee, Sungwon; Seifert, Sönke The Journal of Physical Chemistry B, Vol. 114, Issue 45 https://doi.org/10.1021/jp102904e	journal	November 2010
Re-examination of the Size-Dependent Absorption Properties of CdSe Quantum Dots Jasieniak, Jacek; Smith, Lisa; van Embden, Joel The Journal of Physical Chemistry C, Vol. 113, Issue 45 https://doi.org/10.1021/jp906827m	journal	October 2009
Attenuated Total Reflection Infrared Studies of Oleate and Trioctylphosphine Oxide Ligand Adsorption and Exchange Reactions on CdS Quantum Dot Films Young, Aidan G.; Al-Salim, Najeh; Green, David P. Langmuir, Vol. 24, Issue 8 https://doi.org/10.1021/la703655v	journal	March 2008
Formation of a Liquid-Crystalline Interpenetrating Poly(ionic liquid) Network Hydrogel Becht, Gregory A.; Sofos, Marina; Seifert, Sönke Macromolecules, Vol. 44, Issue 6 https://doi.org/10.1021/ma102146r	journal	March 2011
Guided hierarchical co-assembly of soft patchy nanoparticles Gröschel, André H.; Walther, Andreas; Löbling, Tina I. Nature, Vol. 503, Issue 7475 https://doi.org/10.1038/nature12610	journal	November 2013
Lifetime blinking in nonblinking nanocrystal quantum dots Galland, Christophe; Ghosh, Yagnaseni; Steinbrück, Andrea Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1916	journal	January 2012
Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking Chen, Ou; Zhao, Jing; Chauhan, Vikash P. Nature Materials, Vol. 12, Issue 5 https://doi.org/10.1038/nmat3539	journal	February 2013
Plasmonic polymer nanocomposites Pastoriza-Santos, Isabel; Kinnear, Calum; Pérez-Juste, Jorge Nature Reviews Materials, Vol. 3, Issue 10 https://doi.org/10.1038/s41578-018-0050-7	journal	September 2018
Nanomaterial-based devices for point-of-care diagnostic applications Quesada-González, Daniel; Merkoçi, Arben Chemical Society Reviews, Vol. 47, Issue 13 https://doi.org/10.1039/C7CS00837F	journal	January 2018
Recent advances in colloidal nanocomposite design via heterogeneous polymerization techniques Thickett, Stuart C.; Teo, Guo Hui Polymer Chemistry, Vol. 10, Issue 23 https://doi.org/10.1039/C9PY00097F	journal	January 2019
Multi-stimuli responsive tetra-PPO ₆₀ -PEO ₂₀ ethylene diamine block copolymer enables pH, temperature, and solvent regulation of Au nanoparticle composite plasmonic response Diouf, Sokhna I. Y.; Williams, Darrick J.; Seifert, Sönke Polymer Chemistry, Vol. 10, Issue 47 https://doi.org/10.1039/C9PY01098J	journal	January 2019
Conductivity of ionic liquid-derived polymers with internal gold nanoparticle conduits Lee, Sungwon; Cummins, Matthew D.; Willing, Gerold A. Journal of Materials Chemistry, Vol. 19, Issue 43 https://doi.org/10.1039/b910059h	journal	January 2009
Alternating layer addition approach to CdSe/CdS core/shell quantum dots with near-unity quantum yield and high on-time fractions Greytak, Andrew B.; Allen, Peter M.; Liu, Wenhao Chemical Science, Vol. 3, Issue 6 https://doi.org/10.1039/c2sc00561a	journal	January 2012
Review on Polymer, Hydrogel and Microgel Metal Nanocomposites: A Facile Nanotechnological Approach Thomas, Varsha; Namdeo, Mini; Murali Mohan, Y. Journal of Macromolecular Science, Part A, Vol. 45, Issue 1 https://doi.org/10.1080/10601320701683470	journal	November 2007
Analysis of Classical Statistical Mechanics by Means of Collective Coordinates Percus, Jerome K.; Yevick, George J. Physical Review, Vol. 110, Issue 1 https://doi.org/10.1103/PhysRev.110.1	journal	April 1958
Kinetic Pathways of Order-Disorder and Order-Order Transitions in Weakly Segregated Microstructured Systems Qi, Shuyan; Wang, Zhen-Gang Physical Review Letters, Vol. 76, Issue 10 https://doi.org/10.1103/PhysRevLett.76.1679	journal	March 1996
Irena : tool suite for modeling and analysis of small-angle scattering Ilavsky, Jan; Jemian, Peter R. Journal of Applied Crystallography, Vol. 42, Issue 2 https://doi.org/10.1107/S0021889809002222	journal	February 2009
Small-Angle Scattering from Polymeric Mass Fractals of Arbitrary Mass-Fractal Dimension Beaucage, G. Journal of Applied Crystallography, Vol. 29, Issue 2 https://doi.org/10.1107/S0021889895011605	journal	April 1996
Nanoscale Metrology of Line Patterns on Semiconductor by Continuous Wave Terahertz Multispectral Reconstructive 3-D Imaging Overcoming the Abbe Diffraction Limit Rahman, Anis; Rahman, Aunik K. IEEE Transactions on Semiconductor Manufacturing, Vol. 32, Issue 1 https://doi.org/10.1109/TSM.2018.2865167	journal	February 2019
Polymer ligand–induced autonomous sorting and reversible phase separation in binary particle blends Schmitt, Michael; Zhang, Jianan; Lee, Jaejun Science Advances, Vol. 2, Issue 12 https://doi.org/10.1126/sciadv.1601484	journal	December 2016
Photothermally and magnetically controlled reconfiguration of polymer composites for soft robotics Liu, Jessica A. -C.; Gillen, Jonathan H.; Mishra, Sumeet R. Science Advances, Vol. 5, Issue 8 https://doi.org/10.1126/sciadv.aaw2897	journal	August 2019
Electronic Excitation Energy Transfer in an Array of CdS Quantum Dots on a Quasi-Two-Dimensional Surface Bondar, N. V.; Brodyn, M. S.; Matveevskaya, N. A. Semiconductors, Vol. 53, Issue 2 https://doi.org/10.1134/S1063782619020040	journal	February 2019
Small-Angle X-Ray Scattering on Biological Macromolecules and Nanocomposites in Solution Blanchet, Clement E.; Svergun, Dmitri I. Annual Review of Physical Chemistry, Vol. 64, Issue 1 https://doi.org/10.1146/annurev-physchem-040412-110132	journal	April 2013
When excitons and plasmons meet: Emerging function through synthesis and assembly Hollingsworth, Jennifer A.; Htoon, Han; Piryatinski, Andrei MRS Bulletin, Vol. 40, Issue 9 https://doi.org/10.1557/mrs.2015.200	journal	September 2015
Greater than the sum: Synergy and emergent properties in nanoparticle–polymer composites Firestone, Millicent A.; Hayden, Steven C.; Huber, Dale L. MRS Bulletin, Vol. 40, Issue 9 https://doi.org/10.1557/mrs.2015.202	journal	September 2015
Synthesis of Spherical CdS Quantum Dots Using Cadmium Diethyldithiocarbamate as Single Source Precursor in Olive Oil Medium Devendran, P.; Alagesan, T.; Ravindran, T. R. Current Nanoscience, Vol. 10, Issue 2 https://doi.org/10.2174/15734137113096660117	journal	March 2014
Impact of Crystal Structure and Particles Shape on the Photoluminescence Intensity of CdSe/CdS Core/Shell Nanocrystals Ludescher, Lukas; Dirin, Dmity N.; Kovalenko, Maksym V. Frontiers in Chemistry, Vol. 6 https://doi.org/10.3389/fchem.2018.00672	journal	January 2019
Metal Matrix Composites Reinforced by Nano-Particles—A Review Casati, Riccardo; Vedani, Maurizio Metals, Vol. 4, Issue 1 https://doi.org/10.3390/met4010065	journal	March 2014
Polarization of Colloidal CdSe Quantum Dots Liem, Nguyen Quang; Phuong, Le Quang; Thuy, Ung Thi Dieu Journal of the Korean Physical Society, Vol. 53, Issue 3 https://doi.org/10.3938/jkps.53.1570	journal	September 2008

Similar Records

Multiscale additive manufacturing of polymers using 3D photo-printable self-assembling ionic liquid monomers

Journal Article · Sun Apr 07 20:00:00 EDT 2019 · Molecular Systems Design & Engineering · OSTI ID:1511633

Synthesis and application of a metal ion coordinating ionic liquid monomer: Towards size and dispersity control of nanoparticles formed within a structured polyelectrolyte

Journal Article · Mon Aug 06 20:00:00 EDT 2018 · European Polymer Journal · OSTI ID:1473822

Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Composites
Monomers
Quantum dots
Scattering
Solvents

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

Citation Formats

References (47)

Similar Records

Related Subjects